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Mohammed, Sulafa Abdalmageed Saadaldeen, Wan Zaireen Nisa Yahya, and Mohamad Azmi Bustam. "Computational studies of ionic liquids as co-catalyst for CO2 electrochemical reduction to produce syngas using COSMO-RS." E3S Web of Conferences 287 (2021): 02016. http://dx.doi.org/10.1051/e3sconf/202128702016.
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Transforming carbon dioxide (CO2) into value-added products through electrochemical reduction reaction (CO2ERR) is a promising technique due to its potential advantages using renewable energy. The main challenge is to find a stable catalytic system that could minimize the reaction overpotential with high faradaic efficiency and high current density. Ionic liquids (ILs) as electrolyte in CO2ERR have attracted attention due to the advantages of their unique properties in enhancing catalytic efficiency. For better performance, a systematic understanding of the role of ILs as electrocatalyst is needed. Therefore, this paper aims to correlate the performance of ILs as co-catalyst in (CO2ERR) with the lowest unoccupied molecular orbital (LUMO) energy level and the interaction energy as predicted by quantum chemical calculation using Conductor like Screening Model for Real Solvents (COSMO-RS) and Turbomole. The results show strong linearity (R2=0.98) between hydrogen bond energy (HB) and LUMO values. It is demonstrated that as HB increases, the LUMO value decreases, and the catalytic activity for CO2ERR also increases. This result allows further understanding on the correlation between the molecular structure and the catalytic activity for CO2ERR. It can serve as a priori prediction to aid in the design of new effective catalysts.
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Yan, Yi, Xuerui Wang, Ke Li, Xiaopeng Kang, Weizheng Kong, and Hongcai Dai. "Tri-Level Integrated Optimization Design Method of a CCHP Microgrid with Composite Energy Storage." Sustainability 14, no. 9 (April 28, 2022): 5322. http://dx.doi.org/10.3390/su14095322.
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Combined cooling, heating, and power (CCHP) microgrids are important means of solving the energy crisis and environmental problems. Multidimensional composite energy storage systems (CESSs) are vital to promoting the absorption of distributed renewable energy using CCHP microgrids and improving the level of energy cascade utilization. In this context, this paper proposes a multi-energy coupling structure that includes a multidimensional CESS with a compressed air energy storage (CAES) connected to a CCHP microgrid. Dividing design and operation causes some problems, such as low operating efficiency and difficult energy matching of CESSs. To solve the existing problems, an integrated design method is proposed that considers the capacity configuration of the equipment and the optimal operation of the system on a multi-timescale. The optimization result of the capacity configuration level is used as the constraint of the operational control level, and the equipment output plan of the operational control level is used as the optimized operation strategy and parameters of the system. The C-NSGA-II algorithm is adopted at the capacity configuration level and day-ahead scheduling level. Rolling optimization is solved using the PSO algorithm. The final result that satisfied the output design was obtained after several iterations. The average daily cost and CO2 emission reduction rate (CO2ERR) of capacity configuration levels are $2241 and 45.02%. The best CO2ERRs of day-ahead scheduling optimization levels are 39.9% and 45.9% in summer and winter, where the operating cost saving rate (OCSR) are 30.5% and 38.3% separately. Examples show that the integrated design method presented in this paper has significant advantages in enhancing energy-grade matching and improving the economy and environmental protection of the system.
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Hamonnet, Johan, Michael Bennington, Sally Brooker, Vladimir Golovko, and Aaron Timothy Marshall. "Pyrolysed Co-N4 Macrocycles on Carbon Supports for the Efficient Electroreduction of CO2." ECS Meeting Abstracts MA2022-01, no. 14 (July 7, 2022): 959. http://dx.doi.org/10.1149/ma2022-0114959mtgabs.
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Converting CO2 into materials such as chemicals or synfuels is an attractive way to mitigate greenhouse gas emissions while producing value-added products1-4. Even though the intrinsic chemical stability of CO2 significantly limits its reactivity, the use of electrocatalysts allows its efficient reduction in a mild environment and at relatively low overpotentials5,6. Cobalt phthalocyanine (CoPC), cobalt tetra-phenyl porphyrin (CoTPP) and Vitamin B12 (VB12) are well-defined Co-N4 macrocycles whose incorporation into heterogeneous catalyst setups have led to materials with outstanding CO2 electroreduction reaction (CO2ERR) properties, most notably in the selective formation of CO at high current densities7-11. These Co-N4 macrocycles have also been used to manufacture catalysts efficient for the oxygen reduction reaction (ORR). Notably, the pyrolysis of the macrocyclic precursor supported by carbon materials allowed the fabrication of heterogeneous ORR catalysts with high loadings of catalytically active components, controlled local environments and enhanced stabilities12,13. While these properties could lead to these materials also being efficient catalysts for CO2ERR, to the best of our knowledge, such pyrolyzed catalysts have not been investigated for the CO2 reduction reaction. In this work, we report materials based on CoPC, CoTPP and VB12, supported by carbon black and pyrolyzed under argon, as efficient catalysts for the CO2ERR. The catalytic precursors were dispersed on carbon powders with ball-milling before being annealed at different temperatures chosen from the positions of the significant steps and plateaus observed by thermogravimetric analysis of the pure precursors. The structures of the resulting materials were analyzed by powder X-ray diffraction and X-ray absorption spectroscopy. The electrochemical behaviour of these materials for the CO2ERR were characterized in CO2-saturated potassium bicarbonate (KHCO3) electrolyte using a custom-made flow cell at a range of potentials, and the products of the reaction were analyzed with gas chromatography, 1H NMR spectroscopy and high-performance liquid chromatography. The high reactivity of the catalysts for the reduction of CO2 into CO was maintained for all materials treated at temperatures as high as 700 °C, even though the structures of their active sites were drastically different from that of the precursor molecules. The pyrolyzed materials also exhibited a change in correlation between the CO current densities and the KHCO3 concentration of the electrolyte, indicating that the reaction mechanism had changed compared to that of the pristine materials. 1 Peter, S. C. Reduction of CO2 to Chemicals and Fuels: A Solution to Global Warming and Energy Crisis. ACS Energy Letters 3, 1557-1561, doi:10.1021/acsenergylett.8b00878 (2018). 2 Lee, Z. H., Sethupathi, S., Lee, K. T., Bhatia, S. & Mohamed, A. R. An overview on global warming in Southeast Asia: CO2 emission status, efforts done, and barriers. Renewable and Sustainable Energy Reviews 28, 71-81, doi:10.1016/j.rser.2013.07.055 (2013). 3 Saeidi, S., Amin, N. A. S. & Rahimpour, M. R. Hydrogenation of CO2 to value-added products - A review and potential future developments. Journal of CO2 Utilization 5, 66-81, doi:10.1016/j.jcou.2013.12.005 (2014). 4 Zhao, G., Huang, X., Wang, X. X. & Wang, X. X. Progress in catalyst exploration for heterogeneous CO2 reduction and utilization: A critical review. Journal of Materials Chemistry A 5, 21625-21649, doi:10.1039/c7ta07290b (2017). 5 Finn, C., Schnittger, S., Yellowlees, L. J. & Love, J. B. Molecular approaches to the electrochemical reduction of carbon dioxide. Chemical Communications 48, 1392-1399, doi:10.1039/c1cc15393e (2012). 6 Torbensen, K., Boudy, B., Joulié, D., von Wolff, N. & Robert, M. Emergence of CO2 electrolyzers including supported molecular catalysts. Current Opinion in Electrochemistry 24, 49-55, doi:10.1016/j.coelec.2020.07.001 (2020). 7 Wang, M. et al. CO2 electrochemical catalytic reduction with a highly active cobalt phthalocyanine. Nature Communications 10, doi:10.1038/s41467-019-11542-w (2019). 8 Ni, W. et al. Dual single-cobalt atom-based carbon electrocatalysts for efficient CO2-to-syngas conversion with industrial current densities. Applied Catalysis B: Environmental 291, doi:10.1016/j.apcatb.2021.120092 (2021). 9 Jia, C. et al. Vitamin B12 on Graphene for Highly Efficient CO2 Electroreduction. ACS Appl Mater Interfaces 12, 41288-41293, doi:10.1021/acsami.0c10125 (2020). 10 Hu, B. et al. How does the ligands structure surrounding metal-N4 of Co-based macrocyclic compounds affect electrochemical reduction of CO2 performance? Electrochimica Acta 331, 135283, doi:10.1016/j.electacta.2019.135283 (2020). 11 Hu, X. M., Ronne, M. H., Pedersen, S. U., Skrydstrup, T. & Daasbjerg, K. Enhanced Catalytic Activity of Cobalt Porphyrin in CO2 Electroreduction upon Immobilization on Carbon Materials. Angew Chem Int Ed Engl 56, 6468-6472, doi:10.1002/anie.201701104 (2017). 12 Wan, G. et al. Tuning the Performance of Single-Atom Electrocatalysts: Support-Induced Structural Reconstruction. Chemistry of Materials 30, 7494-7502, doi:10.1021/acs.chemmater.8b02315 (2018). 13 Wan, G. et al. Anion-Regulated Selective Generation of Cobalt Sites in Carbon: Toward Superior Bifunctional Electrocatalysis. Adv Mater 29, doi:10.1002/adma.201703436 (2017).
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Gozalpour, F., S. R. Ren, and B. Tohidi. "CO2Eor and Storage in Oil Reservoir." Oil & Gas Science and Technology 60, no. 3 (May 2005): 537–46. http://dx.doi.org/10.2516/ogst:2005036.
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Zhao, Shuangyang, Aihua Liu, Yonghe Li, Yanyan Wen, Xiaoqian Gao, and Qiaoli Chen. "Boosting the Electrocatalytic CO2 Reduction Reaction by Nanostructured Metal Materials via Defects Engineering." Nanomaterials 12, no. 14 (July 13, 2022): 2389. http://dx.doi.org/10.3390/nano12142389.
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Electrocatalytic CO2 reduction reaction (CO2RR) is one of the most effective methods to convert CO2 into useful fuels. Introducing defects into metal nanostructures can effectively improve the catalytic activity and selectivity towards CO2RR. This review provides the recent progress on the use of metal nanomaterials with defects towards electrochemical CO2RR and defects engineering methods. Accompanying these ideas, we introduce the structure of defects characterized by electron microscopy techniques as the characterization and analysis of defects are relatively difficult. Subsequently, we present the intrinsic mechanism of how the defects affect CO2RR performance. Finally, to promote a wide and deep study in this field, the perspectives and challenges concerning defects engineering in metal nanomaterials towards CO2RR are put forward.
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Alfath, Muhammad, and Chan Woo Lee. "Recent Advances in the Catalyst Design and Mass Transport Control for the Electrochemical Reduction of Carbon Dioxide to Formate." Catalysts 10, no. 8 (August 2, 2020): 859. http://dx.doi.org/10.3390/catal10080859.
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Closing the carbon cycle by the electrochemical reduction of CO2 to formic acid and other high-value chemicals is a promising strategy to mitigate rapid climate change. The main barriers to commercializing a CO2 reduction reaction (CO2RR) system for formate production are the chemical inertness, low aqueous solubility, and slow mass transport characteristics of CO2, along with the low selectivity and high overpotential observed in formate production via CO2 reduction. To address those problems, we first explain the possible reaction mechanisms of CO2RRs to formate, and then we present and discuss several strategies to overcome the barriers to commercialization. The electronic structure of the catalyst can be tuned to favor a specific intermediate by adjusting the catalyst composition and tailoring the facets, edges, and corners of the catalyst to better expose the active sites, which has primarily led to increased catalytic activity and selectivity. Controlling the local pH, employing a high-pressure reactor, and using systems with three-phase boundaries can tune the mass transport properties of reactants at the catalyst surface. The reported electrocatalytic performances are summarized afterward to provide insight into which strategies have critical effects on the production of formate.
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Guo, Gengzhan, Tianyang Wang, and Yuzhe Wang. "Utilizing Metal-Organic Frameworks to Achieve High-Efficiency CO2 Electroreduction." Journal of Physics: Conference Series 2254, no. 1 (April 1, 2022): 012025. http://dx.doi.org/10.1088/1742-6596/2254/1/012025.
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Abstract Electrochemical CO2 reduction reaction (CO2RR) is the key part of clean energy generation and utilization, which has great potential to help the world to reach the carbon-neutral energy cycle in the future. In line with the development of metal-organic frameworks (MOFs) with the large specific area and considerable porosity in the past two decades, some of the MOF-based electrocatalysts have shown superior ability to accelerate CO2RR. However, regarding such a significant CO2RR process, some critical disadvantages, including inferior robustness, low yield and selectivity, and idealistic working environment, are still required to be concentrated on. Herein, a comprehensive outline of the reaction mechanism of CO2 conversion and rational synthesis of the state-of-the-art pristine MOFs is given. Further, recent progress of pristine MOF-based electrocatalysts in CO2RR is systematically summarized. Lastly, the major limitations and future opportunities in MOF electrocatalysis for CO2RR are presented.
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Mohammed, Sulafa Abdalmageed Saadaldeen, Wan Zaireen Nisa Yahya, Mohamad Azmi Bustam, and Md Golam Kibria. "Elucidation of the Roles of Ionic Liquid in CO2 Electrochemical Reduction to Value-Added Chemicals and Fuels." Molecules 26, no. 22 (November 18, 2021): 6962. http://dx.doi.org/10.3390/molecules26226962.
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The electrochemical reduction of carbon dioxide (CO2ER) is amongst one the most promising technologies to reduce greenhouse gas emissions since carbon dioxide (CO2) can be converted to value-added products. Moreover, the possibility of using a renewable source of energy makes this process environmentally compelling. CO2ER in ionic liquids (ILs) has recently attracted attention due to its unique properties in reducing overpotential and raising faradaic efficiency. The current literature on CO2ER mainly reports on the effect of structures, physical and chemical interactions, acidity, and the electrode–electrolyte interface region on the reaction mechanism. However, in this work, new insights are presented for the CO2ER reaction mechanism that are based on the molecular interactions of the ILs and their physicochemical properties. This new insight will open possibilities for the utilization of new types of ionic liquids. Additionally, the roles of anions, cations, and the electrodes in the CO2ER reactions are also reviewed.
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Lu, Qingqing, Kamel Eid, and Wenpeng Li. "Heteroatom-Doped Porous Carbon-Based Nanostructures for Electrochemical CO2 Reduction." Nanomaterials 12, no. 14 (July 12, 2022): 2379. http://dx.doi.org/10.3390/nano12142379.
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The continual rise of the CO2 concentration in the Earth’s atmosphere is the foremost reason for environmental concerns such as global warming, ocean acidification, rising sea levels, and the extinction of various species. The electrochemical CO2 reduction (CO2RR) is a promising green and efficient approach for converting CO2 to high-value-added products such as alcohols, acids, and chemicals. Developing efficient and low-cost electrocatalysts is the main barrier to scaling up CO2RR for large-scale applications. Heteroatom-doped porous carbon-based (HA-PCs) catalysts are deemed as green, efficient, low-cost, and durable electrocatalysts for the CO2RR due to their great physiochemical and catalytic merits (i.e., great surface area, electrical conductivity, rich electrical density, active sites, inferior H2 evolution activity, tailorable structures, and chemical–physical–thermal stability). They are also easily synthesized in a high yield from inexpensive and earth-abundant resources that meet sustainability and large-scale requirements. This review emphasizes the rational synthesis of HA-PCs for the CO2RR rooting from the engineering methods of HA-PCs to the effect of mono, binary, and ternary dopants (i.e., N, S, F, or B) on the CO2RR activity and durability. The effect of CO2 on the environment and human health, in addition to the recent advances in CO2RR fundamental pathways and mechanisms, are also discussed. Finally, the evolving challenges and future perspectives on the development of heteroatom-doped porous carbon-based nanocatalysts for the CO2RR are underlined.
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Zhang, Yaping, Jixiang Xu, Lei Wang, and Banglin Chen. "Multiple roles of metal–organic framework-based catalysts in photocatalytic CO2 reduction." Chemical Physics Reviews 3, no. 4 (December 2022): 041306. http://dx.doi.org/10.1063/5.0099758.
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Photocatalytic CO2 reduction is one of the ideal means to realize the carbon cycle. Metal–organic frameworks (MOFs) have received great attention as catalysts for photocatalytic CO2RR in recent years. The adjustable metal nodes and organic ligands in MOFs make them multifunctional catalysts. Therefore, they can participate in photocatalytic CO2RR in different roles. MOFs can be used as primary photocatalysts or be coupled with other active species to form composite materials. They can also act as co-catalysts to cooperate with photosensitizers. Moreover, MOFs can be used as precursors or templates for the preparation of derived nanomaterials. These derivatives are also promising candidates in photocatalytic CO2RR. This review aims to outline multiple roles of MOFs and their derivatives in photocatalytic CO2RR. Meanwhile, the corresponding modification strategies are summarized. At the end of the manuscript, the present problems of MOFs applied in photocatalytic CO2RR are summarized and the future development and challenges are also proposed.
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Wang, Zhonghao, Rui Shi, Siyu Lu, Kan Zhang, and Tierui Zhang. "Atom manufacturing of photocatalyst towards solar CO2 reduction." Reports on Progress in Physics 85, no. 2 (February 1, 2022): 026501. http://dx.doi.org/10.1088/1361-6633/ac4d88.
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Abstract Photocatalytic CO2 reduction reaction (CO2RR) is believed to be a promising remedy to simultaneously lessen CO2 emission and obtain high value-added products, but suffers from the thwarted activity of photocatalyst and poor selectivity of product. Over the past decade, aided by the significant advances in nanotechnology, the atom manufacturing of photocatalyst, including vacancies, dopants, single-atom catalysts, strains, have emerged as efficient approaches to precisely mediate the reaction intermediates and processes, which push forward in the rapid development of highly efficient and selective photocatalytic CO2RR. In this review, we summarize the recent developments in highly efficient and/or selective photocatalysts toward CO2RR with the special focus on various atom manufacturing. The mechanisms of these atom manufacturing from active sites creation, light absorbability, and electronic structure modulation are comprehensively and scientifically discussed. In addition, we attempt to establish the structure–activity relationship between active sites and photocatalytic CO2RR capability by integrating theoretical simulations and experimental results, which will be helpful for insights into mechanism pathways of CO2RR over defective photocatalysts. Finally, the remaining challenges and prospects in this field to improve the photocatalytic CO2RR performances are proposed, which can shed some light on designing more potential photocatalysts through atomic regulations toward CO2 conversion.
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Luévano-Hipólito, Edith, Oscar L. Quintero-Lizárraga, and Leticia M. Torres-Martínez. "A Critical Review of the Use of Bismuth Halide Perovskites for CO2 Photoreduction: Stability Challenges and Strategies Implemented." Catalysts 12, no. 11 (November 11, 2022): 1410. http://dx.doi.org/10.3390/catal12111410.
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Inspired by natural photosynthesis, the photocatalytic CO2 reduction reaction (CO2RR) stands as a viable strategy for the production of solar fuels to mitigate the high dependence on highly polluting fossil fuels, as well as to decrease the CO2 concentration in the atmosphere. The design of photocatalytic materials is crucial to ensure high efficiency of the CO2RR process. So far, perovskite materials have shown high efficiency and selectivity in CO2RR to generate different solar fuels. Particularly, bismuth halide perovskites have gained much attention due to their higher absorption coefficients, their more efficient charge transfer (compared to oxide perovskites), and their required thermodynamic potential for CO2RR. Moreover, these materials represent a promising alternative to the highly polluting lead halide perovskites. However, despite all the remarkable advantages of bismuth halide perovskites, their use has been limited, owing to instability concerns. As a consequence, recent reports have offered solutions to obtain structures highly stable against oxygen, water, and light, promoting the formation of solar fuels with promising efficiency for CO2RR. Thus, this review analyzes the current state of the art in this field, particularly studies about stability strategies from intrinsic and extrinsic standpoints. Lastly, we discuss the challenges and opportunities in designing stable bismuth halide perovskites, which open new opportunities for scaling up the CO2RR.
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Li, Sanxiu, Yufei Kang, Chenyang Mo, Yage Peng, Haijun Ma, and Juan Peng. "Nitrogen-Doped Bismuth Nanosheet as an Efficient Electrocatalyst to CO2 Reduction for Production of Formate." International Journal of Molecular Sciences 23, no. 22 (November 21, 2022): 14485. http://dx.doi.org/10.3390/ijms232214485.
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Electrochemical CO2 reduction (CO2RR) to produce high value-added chemicals or fuels is a promising technology to address the greenhouse effect and energy challenges. Formate is a desirable product of CO2RR with great economic value. Here, nitrogen-doped bismuth nanosheets (N-BiNSs) were prepared by a facile one-step method. The N-BiNSs were used as efficient electrocatalysts for CO2RR with selective formate production. The N-BiNSs exhibited a high formate Faradic efficiency (FEformate) of 95.25% at −0.95 V (vs. RHE) with a stable current density of 33.63 mA cm−2 in 0.5 M KHCO3. Moreover, the N-BiNSs for CO2RR yielded a large current density (300 mA cm−2) for formate production in a flow-cell measurement, achieving the commercial requirement. The FEformate of 90% can maintain stability for 14 h of electrolysis. Nitrogen doping could induce charge transfer from the N atom to the Bi atom, thus modulating the electronic structure of N-Bi nanosheets. DFT results demonstrated the N-BiNSs reduced the adsorption energy of the *OCHO intermediate and promoted the mass transfer of charges, thereby improving the CO2RR with high FEformate. This study provides a valuable strategy to enhance the catalytic performance of bismuth-based catalysts for CO2RR by using a nitrogen-doping strategy.
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Huang, Yu. "(Invited) Engineered Cu Surface for Efficient CO2RR." ECS Meeting Abstracts MA2020-01, no. 39 (May 1, 2020): 1745. http://dx.doi.org/10.1149/ma2020-01391745mtgabs.
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Iwase, Kazuyuki, Takayuki Kojima, Naoto Todoroki, and Itaru Honma. "Activity switching of Sn and In species in Heusler alloys for electrochemical CO2 reduction." Chemical Communications 58, no. 31 (2022): 4865–68. http://dx.doi.org/10.1039/d2cc00754a.
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Oh, Hyung-Suk, and Chulwan Lim. "Ag Dendrites on W/C as Enhanced Active and Stable Electrocatalysts for Scalable Solar-Driven CO2rr." ECS Meeting Abstracts MA2022-02, no. 48 (October 9, 2022): 1866. http://dx.doi.org/10.1149/ma2022-02481866mtgabs.
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The electrochemical conversion of solar energy into competent chemicals is the most efficient technique to ensure clean and sustainable energy source for society in the future. In fact, solar cells can electrochemically produce electricity without pollution by converting CO2 into a variety of chemicals. The carbon dioxide reduction reaction (CO2RR) is an environmentally friendly approach to produce useful hydrocarbons such as carbon monoxide (CO), methane, ethylene, formates, etc and alcohols and remove exhausted CO2, which is a greenhouse gas. Conventionally, studies on the CO2RR have been conducted by using liquid-phase H-cells and a CO2-saturated electrolyte. However, it resulted in a low current density because the low solubility of CO2 in the liquid electrolyte occurs mass transfer limitation. To improve of the current density related to the CO2RR, two types of gas-fed CO2RR electrolyzers containing gas diffusion layer (GDL) electrodes have been proposed. The first type of CO2RR devices use a liquid electrolyte, the electrolyte increases CO2RR performance through controlling the cathode conditions, such as pH and anion concentration. The second type of CO2RR devices is zero-gap electrolyzers that use an anion exchange membrane (AEM) and humidified CO2 gas. AEM transmits carbonate and hydroxide ion, inducing favorable environmental for CO2RR. These zero-gap CO2 electrolyzers are attracting attention as the most promising system owing to several advantages such as extremely low ohmic resistance, scalable and stackable configuration, and commercial applicability, as affirmed by using a system consisting of a fuel cell and water electrolyzer. Among the products of the CO2RR, CO is particularly attractive as aspect of its economic benefits and large demand. Ag-based materials exhibit the most electrochemical performance for producing CO. and high selectivity. To enhance the catalytic activity of Ag-based catalysts, various approaches have been studied to change the surface electronic structure of Ag such as alloy formation, anion-based modification, shape control, near-surface structure and engineering. However, catalyst designs that do not consider the gas phase reactions cannot enough utilize their catalytic activity although recent progress has made in the development of Ag-based catalysts for the CO2RR. Therefore, considerable efforts must be preoccupied with the development of highly active, stable, and gas-transferable structured catalysts for gas-fed CO2RR electrolyzers with incoporating a GDL. Additionally, aming for the realization of clean technology for producing CO, we demonstrate the practicalbility of sunlight-driven CO2RR on a large scale using commercial silicon-based solar cells and zero-gap electrolyzers. Silicon-based solar cells are still the preferred commercially applicapable options for producing large amounts of electrical power from solar energy because of their scalability. In this study, we report a 3D silver dendrite on W/C (as denoted WC@AgD) catalyst with abundant nanograin boundaries that show enhanced CO2RR performance and stability. WC@AgD exhibited marked catalytic activity with a maximum CO partial current density of 400 mA cm-2 and durability for 100 h at 150 mA cm-2. We also fabricated an solar-to-CO (STC) conversion device combined with a silicon-based solar cell of 120 cm2 area and a zero-gap CO2 electrolyzer with an area of 10 cm2. The stand-alone photovoltaic-electrochemical system achieved a solar-to-CO efficiency (ηSTC) of 12.1 % at 1A under AM 1.5 G illumination and realistic outdoor conditions. The device design and electrode configuration extended viable route for implementing large-scale installations for solar-driven production of chemicals. Figure 1
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Wang, Fangyuan, Yu Liu, Zhiling Song, Zhichao Miao, and Jinping Zhao. "Ni-N-Doped Carbon-Modified Reduced Graphene Oxide Catalysts for Electrochemical CO2 Reduction Reaction." Catalysts 11, no. 5 (April 28, 2021): 561. http://dx.doi.org/10.3390/catal11050561.
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Electrochemical CO2 reduction reaction (CO2RR) is eliciting considerable attention in relation to the carbon cycle and carbon neutrality. As for the practical application of CO2RR, the electrocatalyst is a crucial factor, but, even so, designing and synthesizing an excellent catalyst remains a significant challenge. In this paper, the coordination compound of Ni ions and dimethylglyoxime (DMG) was employed as a precursor to modify reduced graphene oxide (rGO) for CO2RR. The textural properties and chemical bonds of as-obtained rGO, N–C–rGO, Ni–rGO, Ni–N–C, and Ni–N–C–rGO materials were investigated in detail, and the role of Ni, N–C, and rGO in the CO2RR were researched and confirmed. Among all the catalysts, the Ni–N–C–rGO showed the optimal catalytic activity and selectivity with a high current density of 10 mA cm−2 and FE(CO)% of 85% at −0.87 V vs. RHE. In addition, there was no obvious decrease in activity for 10 h. Therefore, the Ni–N–C–rGO is a promising catalyst for CO2RR to CO.
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Sui, Peng-Fei, Chenyu Xu, Mengnan Zhu, Subiao Liu, and Jing-Li Luo. "Maximizing the Formate Formation of CO2 Electroreduction Via Boosting Charge Transfer Ability." ECS Meeting Abstracts MA2022-01, no. 55 (July 7, 2022): 2301. http://dx.doi.org/10.1149/ma2022-01552301mtgabs.
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The electrochemical reduction reaction of CO2 (CO2RR) is an attractive strategy for achieving carbon-neutral sustainability while the highly active and selective reaction for formate formation remains challenging. In addition, the thermodynamic inertness of CO2 usually leads to a high energy barrier for CO2RR, resulting in a preference for the competitive hydrogen evolution reaction. It is known that CO2RR is a proton-coupled electron transfer (PCET) process and the complicated multi-electron transfer steps occur on the catalyst surface. Therefore, improving the charge transfer ability is considered as an effective approach to maximizing the electrocatalytic activity and selectivity for CO2RR. Interface engineering has been proven as an effective method to prompt charge transfer by constructing interfaces within the catalysts that is widely used in many electrochemical reactions. The introduced interfaces would benefit the electronic interaction at the interface and assist the electron redistribution, thus optimizing the electronic structure and boosting the interfacial charge transfer. Herein, we report the heterostructure of Bi2S3-Bi2O3 nanosheets (BS-BO NSs) with substantial interfaces for the efficient CO2-to-formate conversion. The rapid-interfacial charge transfer induced by the abundant interfaces not only optimizes electronic structure, but also accelerates the kinetics of CO2RR and improves the electrocatalytic activity and selectivity. Compared with the separate Bi2O3 and Bi2S3 electrocatalysts, BS-BO NSs shows desirable selectivity to formate with a maximum Faradaic efficiency of 93.8 % at a moderate potential. The CO2RR performance is further boosted by using a flow cell system. The high selectivity with large current density makes BS-BO NSs a promising candidate for the practical application of CO2RR in the formate formation.
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He, Yanghua, John Christian Weiss, and Piotr Zelenay. "Me-N-C Electrocatalysts for Electrochemical CO2 Reduction to High-Value Products." ECS Meeting Abstracts MA2022-02, no. 54 (October 9, 2022): 2016. http://dx.doi.org/10.1149/ma2022-02542016mtgabs.
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The development of sustainable carbon-neutral energy technologies to mitigate greenhouse gas emissions has become imperative and urgent. Of special interest and importance in this context is the use of electricity from intermittent renewable energy sources (wind, solar) for electrochemical conversion of carbon dioxide (CO2) to easily storable and transportable value-added products: fuels and feedstock chemicals. Nanoparticles of non-precious metals, e.g., Cu, Sn, Co, show high activity for electrochemical CO2 reduction reaction (CO2RR) but suffer from poor selectivity, resulting in a mixture of products that require tedious and costly separation. Recently, transition metal- and nitrogen-doped carbon (Me-N-C) materials have been emerged as promising CO2RR catalysts thanks to their well-defined structures and good activity. However, their selectivity, while respectable for the generation of carbon monoxide (CO), is low for high energy-content products. A limited understanding of reaction pathways and degradation mechanism of Me-N-C catalysts for CO2RR has additionally stemmed a rational design of these materials. In this presentation, we summarize our study of the activity, selectivity, and stability of Me-N-C (Me = Fe, Co, Ni, or Cu, etc.) catalysts for the CO2RR, focusing on the role of the local coordination environment at metal centers and metal-carbon substrate interactions. We also report the obtained bimetallic M1M2-N-C catalysts, designed to enable the formation of multi-carbon products through CO2RR and utilizing high surface-area three-dimensional carbon matrix as support for metal sites with improved CO2RR activity. The main objective of this work is to use Me-N-C catalysts to produce high energy-density chemicals, enhance mechanistic understanding, and bring CO2RR closer to practical applications.
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Hou, Xianghua, Junyang Ding, Wenxian Liu, Shusheng Zhang, Jun Luo, and Xijun Liu. "Asymmetric Coordination Environment Engineering of Atomic Catalysts for CO2 Reduction." Nanomaterials 13, no. 2 (January 11, 2023): 309. http://dx.doi.org/10.3390/nano13020309.
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Single-atom catalysts (SACs) have emerged as well-known catalysts in renewable energy storage and conversion systems. Several supports have been developed for stabilizing single-atom catalytic sites, e.g., organic-, metal-, and carbonaceous matrices. Noticeably, the metal species and their local atomic coordination environments have a strong influence on the electrocatalytic capabilities of metal atom active centers. In particular, asymmetric atom electrocatalysts exhibit unique properties and an unexpected carbon dioxide reduction reaction (CO2RR) performance different from those of traditional metal-N4 sites. This review summarizes the recent development of asymmetric atom sites for the CO2RR with emphasis on the coordination structure regulation strategies and their effects on CO2RR performance. Ultimately, several scientific possibilities are proffered with the aim of further expanding and deepening the advancement of asymmetric atom electrocatalysts for the CO2RR.
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Hung, Sung-Fu. "Electrochemical flow systems enable renewable energy industrial chain of CO2 reduction." Pure and Applied Chemistry 92, no. 12 (December 16, 2020): 1937–51. http://dx.doi.org/10.1515/pac-2020-0705.
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AbstractThe development of a comprehensive renewable energy industrial chain becomes urgent since renewable energy will soon dominate the power generation. Among the industries, carbon dioxide reduction reaction (CO2RR), which uses energy to convert carbon dioxide into high-value products and reduce CO2 in the atmosphere, is regarded as a promising and potential industrial application. The conventional H-type reactor shows limited catalytic activity toward CO2RR, leading to the incompatible combination with the massive renewable energy. The flow systems – flow-cell reactor and the membrane electrode assemblies – show the promising selectivity and activities of CO2RR products, meeting the criteria for industrial mass production. In this Perspective, I start by comparing the market price and annual global production of major CO2RR products with the necessary costs using technoeconomic analysis for industrial utilization. Subsequently, I systematically summarize the catalytic performances of the same copper catalyst in these reactors for CO2RR and discuss the possibility of industrialization. Owing to the distinctive catalytic behaviors in flow systems, I finally present prospects to investigate the catalytic mechanisms by developing various in-situ techniques in these flow systems to speed up the renewable energy industry.
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He, Jingfu, Chenghui Wu, Yanming Li, and Changli Li. "Design of pre-catalysts for heterogeneous CO2 electrochemical reduction." Journal of Materials Chemistry A 9, no. 35 (2021): 19508–33. http://dx.doi.org/10.1039/d1ta03624f.
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This work reviews the recent advances of pre-catalysts for CO2 reduction reaction (CO2RR) research. The important factors that may be responsible for the improvement of the CO2RR performance are categorized and a perspective is also presented.
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Ling, Yangfang, Qinglang Ma, Yifu Yu, and Bin Zhang. "Optimization Strategies for Selective CO2 Electroreduction to Fuels." Transactions of Tianjin University 27, no. 3 (March 8, 2021): 180–200. http://dx.doi.org/10.1007/s12209-021-00283-x.
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AbstractCapturing CO2 from the atmosphere and converting it into fuels are an efficient strategy to stop the deteriorating greenhouse effect and alleviate the energy crisis. Among various CO2 conversion approaches, electrocatalytic CO2 reduction reaction (CO2RR) has received extensive attention because of its mild operating conditions. However, the high onset potential, low selectivity toward multi-carbon products and poor cruising ability of CO2RR impede its development. To regulate product distribution, previous studies performed electrocatalyst modification using several universal methods, including composition manipulation, morphology control, surface modification, and defect engineering. Recent studies have revealed that the cathode and electrolytes influence the selectivity of CO2RR via pH changes and ionic effects, or by directly participating in the reduction pathway as cocatalysts. This review summarizes the state-of-the-art optimization strategies to efficiently enhance CO2RR selectivity from two main aspects, namely the cathode electrocatalyst and the electrolyte.
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Galindo Paliza, Luis Miguel, Paulina Guadalupe Reyes Martínez, and Karina Caballero Güendulain. "Escenarios de mitigación para México a 2050: algunos hechos estilizados." Sobre México Temas de Economía 1, no. 6 (November 7, 2022): 156–208. http://dx.doi.org/10.48102/rsm.v1i6.118.
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El principal objetivo de este artículo es analizar algunos hechos estilizados de la trayectoria de las emisiones de gases de efecto invernadero, y con base en ello construir algunos escenarios prospectivos para México que ilustran la urgencia, la magnitud, los riesgos, las posibilidades y las limitaciones del esfuerzo de mitigación requerido para alcanzar la meta de una economía carbono neutral entre 2050-2070. La construcción de estos escenarios se basa en los modelos IPAT y STIRPAT. Los principales resultados indican que las emisiones de energía (CO2eet) están estrechamente asociadas a la evolución del producto interno bruto (PIBt), del PIBT per cápita, de la población y del consumo de energía, y que el actual proceso de desacoplamiento en la trayectoria de las emisiones de CO2eet provenientes de sus principales variables determinantes es insuficiente para cumplir la meta de una economía carbono neutral para 2050-2070. A fin de alcanzar la meta de una economía carbono neutral entre 2050-2070 es necesario realizar transformaciones estructurales con urgencia y de una gran magnitud, que se reflejen en intensos procesos de reducción de las razones de consumo de energía a PIBt y de emisiones de CO2et a consumo de energía. La actual trayectoria de la economía mexicana donde se posponen los procesos de mitigación conduce a una trayectoria de encadenamiento que reduce la credibilidad del cumplimiento de las metas de descarbonización profunda y está aumentando los riesgos de una transición climática justa.
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Lee, Jungkuk, Hengzhou Liu, Yifu Chen, and Wenzhen Li. "Selective Electrochemical CO2 Reduction to Formate over Bismuth Nanosheets Derived By in-Situ Morphology Transformation of Bismuth Oxides." ECS Meeting Abstracts MA2022-01, no. 39 (July 7, 2022): 1780. http://dx.doi.org/10.1149/ma2022-01391780mtgabs.
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The electrochemical CO2 reduction reaction (CO2RR) has attracted enormous attention as a promising technology not only to mitigate CO2 accumulation, but also to convert CO2 into valuable chemicals and fuels.Formate/formic acid is a value-added product from CO2RR that is an important intermediate for chemical industries such as medicines, rubbers, leather and deicing materials. Moreover, it can be used as a source for hydrogen storage, transportation, as well as a fuel for direct formic acid fuel cells. Bismuth nanosheets (BiNSs) have been recognized as a promising catalyst for electrochemical CO2 reduction (CO2RR) to formate, but its preparation typically involves an elaborate synthesis of Bi-precursors under elevated temperature and pressure. Here, we have demonstrated a simple, low-cost preparation method for BiNSs by in-situ morphology transformation of Bi2O3 particles by simple electrochemical processing. SEM analysis showed that such transformation is exceedingly facile on the precipitated Bi2O3 particles compared to BiNPs and Oxi-BiNPs, revealing the crucial roles of oxygen and the initial morphology of Bi precursor in the exfoliation of BiNSs. The OD-BiNS exhibited superior CO2RR performance compared to the BiNPs and Oxi-BiNPs. 93% of FE was achieved with the current density of 62 mA cm−2 at −0.95 VRHE in the H-type cell. The enhanced CO2RR performance of OD-BiNSs can be attributed to its higher intrinsic activity and increased ECSA. 94% of FE with a high current density of 200 mA cm−2 was achieved in the flow cell, suggesting OD-BiNSs as a promising catalyst for practical applications of CO2RR. Our recent research on flow electrolytic cells for CO2 reduction will also be presented.
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Shahrestani, Shohreh, Mohammadali Beheshti, and Saeid Kakooei. "Investigation of Electrochemical Parameters on Cost-Effective Zn/Ni-Based Electrocatalysts for Electrochemical CO2 Reduction Reaction to SYNGAS(H2+CO)." Journal of The Electrochemical Society 169, no. 4 (April 1, 2022): 044519. http://dx.doi.org/10.1149/1945-7111/ac645a.
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Electrochemical CO2 reduction reaction (CO2RR) has been studied in 0.1 M of KCl (pH of 6.96), NaHCO3 (pH of 8.3) and K2CO3 (pH of 11.36) cathodic solutions with various counter electrodes including graphite rod, SS316 rod and Pt mesh at different potential ranges on the Znx–Ni1-x bimetallic electrocatalysts. Among the Znx–Ni1-x electrocatalysts, the Zn–Ni electrode with a composition of 65 wt% Zn and 35 wt% Ni and cluster-like microstructure has the best performance for CO2RR by according to minimum coke formation and optimum CO and H2 faradaic efficiencies (CO FE% = 55% and H2 FE% = 45%). The cyclic voltammetry (CV) measurements and gas chromatography (GC) analysis for the CO2RR showed that KCl solution as the cathodic electrolyte with pH of 7 has the best performance and appropriate faradaic efficiency for H2(40%) and CO(30%) products in low potential value (−0.6 v) in this study. The best potential range for the CO2RR on the Zn-Ni bimetallic electrocatalyst in KCl solution with the scan rate (SR) 0.05 V. s−1 is between −0.3 V to −1 V vs Ag/AgCl. The use of stainless-steel electrode (SS316) as a counter electrode for electrochemical CO2RR is cost-effective and performs better than graphite electrode, but at high applied potential it oxidizes and dissolves in the electrolyte and then ions transfer to the Nafion membrane and poisons it.
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Geng, Dongsheng, and Gang Dong. "Facet-Dependent Selectivity of Cuprous Oxide/Silver Tandem Catalysts for Promoting C2H4 Production from Electrochemical CO2 Reduction." ECS Meeting Abstracts MA2022-01, no. 38 (July 7, 2022): 1700. http://dx.doi.org/10.1149/ma2022-01381700mtgabs.
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The over-exploitation of fossil fuels and the consequent increase of atmospheric CO2 concentration have aroused people's attention to energy and environmental issues.(1) In terms of reducing CO2 content, the electrocatalytic CO2 reduction reaction (CO2RR) can effectively solidify CO2 and convert it into high value-added chemicals. There are many CO2RR reduction products, including CO, HCOOH, C2H5OH, CH4,C2H4, etc.(2) However, in the CO2RR process, the hydrogen evolution reaction (HER) in the water phase has a lower reduction potential, making the CO2RR products less selective, which has become the most important problem restricting its practical application. Therefore, improving the selectivity and activity of CO2RR products has important research significance and practical application value. In this work, a series of Cu2O/Ag nanocrystals (NCs) with different crystal faces were prepared by hydrothermal method. Specifically, cubic Cu2O (c-Cu2O) enclosed with {100} facets, rhombic dodecahedral Cu2O (d-Cu2O) enclosed with {110} facets, and octahedral Cu2O (o-Cu2O) enclosed with {111} facets, are mixed with Ag nanospheres to form c-Cu2O/Ag, d-Cu2O/Ag, and o-Cu2O/Ag bimetallic tandem catalysts. The catalysts can improve the high activity and selectivity of CO2RR to produce C2H4 product by adjusting different crystal faces. We can find from Figure 1 that o-Cu2O/Ag tandem catalyst exhibits an impressive Faradaic efficiency (66.8%) and partial current density (17.8 mA cm-2) for C2H4 product at -1.2 VRHE. This result provides a new strategy for improving the selectivity of CO2RR to produce C2+ products by adjusting the crystal facet engineering. Figure 1. (a) SEM images of o-Cu2O/Ag, (b) LSV curves of three Cu2O/Ag catalysts in Ar and CO2-saturated 0.5 M KHCO3 solutions, (c) Partial current density of C2H4 formation on the three Cu2O/Ag catalysts at -1.2 V, (d) Faradaic efficiencies of C2H4 on the three Cu2O/Ag NCs. Reference [1] P. De Luna, C. Hahn, D. Higgins, S. A. Jaffer, T. F. Jaramillo and E. H. Sargent, Science, 364 (2019). [2]Y. Zheng, A. Vasileff, X. Zhou, Y. Jiao, M. Jaroniec and S. Z. Qiao, J Am Chem Soc, 141, 7646 (2019). Figure 1
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Zhu, Mengnan, Bowen Zhang, Karthik Shankar, Steven Bergens, and Jingli Luo. "Switchable CO2 Electroreduction Induced By the Bismuth Moiety with Tunable Local Structures on Graphene." ECS Meeting Abstracts MA2022-01, no. 49 (July 7, 2022): 2090. http://dx.doi.org/10.1149/ma2022-01492090mtgabs.
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Controlling the chemical environment of the atomically dispersed central atoms doped in the graphene lattice is critical to achieve desirable catalytic performances in carbon dioxide reduction reaction (CO2RR), however, how the local structures of non-transition metal-based single atom (SAs) affect the catalytic performances of CO2RR remains less understood. This study reports the immobilization of bismuth single atom catalysts (SACs) on pristine and nitrogenated graphene nanosheets with switchable catalytic selectivity in the carbon dioxide reduction reaction (CO2RR). Based on systematic physical characterizations and electrochemical analysis, it has been demonstrated that the Bi atom coordinated with four adjacent nitrogen atoms (Bi-N-C) selectively produces carbon monoxide (CO) with high selectivity at low overpotential, whereas Bi SACs bounded with carbon atoms (Bi-C) almost exclusively generate formate (FA). Theoretical investigations reveal that the Bi-N-C catalyst displays the lowest activation barrier for the first hydrogenation step of CO2 to produce *COOH, while Bi-C shows the most preferable pathway towards the formation of *OCHO, which is considered as the important intermediate species to generate FA. The controllable product distributions are dictated by the different local structures of Bi centers in Bi-N-C and Bi-C, and such differences could induce distinct electronic properties of Bi centers and subsequently switch the CO2RR products from CO to FA. This work has substantiated the importance of the fine-regulation of the coordination environment of one of the representative p-blocking SAs to steer the selectivity of CO2RR.
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Hsieh, Jui Ching, David T. W. Lin, Wei Mon Yan, and Long Der Shin. "The Design of Heat Pipe Heat Exchanger for CO2 EGS." Applied Mechanics and Materials 479-480 (December 2013): 284–88. http://dx.doi.org/10.4028/www.scientific.net/amm.479-480.284.
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The findings of new energy and energy harvester are the important issues for the lacking of fossil energy. For the purpose of the effective usage of supercritical CO2flowed from the product well of CO2EGS (Enhanced Geothermal System), an innovative heat pipe heat exchanger (Hx) is designed and practiced in this study. This study presents an innovative Hx of heat pipe for extracting the heat from CO2or warm gas. By using the heat pipe for cooling gas is the fundamental idea of this Hx. The experimental apparatus of Hx consists a heating blower to blow out hot gas, a circulating cool water device, and a set of heat pipes. The efficiency of Hx is approved as the increasing air velocity and the more fins gradually. This innovative heat pipe exchanger is proofed through our experiment. This heat pipe Hx is suitable for the application of enhanced geothermal system (EGS) and more energy harvesting application.
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Sun, Jiameng, Bin Yu, Xuejiao Yan, Jianfeng Wang, Fuquan Tan, Wanfeng Yang, Guanhua Cheng, and Zhonghua Zhang. "High Throughput Preparation of Ag-Zn Alloy Thin Films for the Electrocatalytic Reduction of CO2 to CO." Materials 15, no. 19 (October 4, 2022): 6892. http://dx.doi.org/10.3390/ma15196892.
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Ag-Zn alloys are identified as highly active and selective electrocatalysts for CO2 reduction reaction (CO2RR), while how the phase composition of the alloy affects the catalytic performances has not been systematically studied yet. In this study, we fabricated a series of Ag-Zn alloy catalysts by magnetron co-sputtering and further explored their activity and selectivity towards CO2 electroreduction in an aqueous KHCO3 electrolyte. The different Ag-Zn alloys involve one or more phases of Ag, AgZn, Ag5Zn8, AgZn3, and Zn. For all the catalysts, CO is the main product, likely due to the weak CO binding energy on the catalyst surface. The Ag5Zn8 and AgZn3 catalysts show a higher CO selectivity than that of pure Zn due to the synergistic effect of Ag and Zn, while the pure Ag catalyst exhibits the highest CO selectivity. Zn alloying improves the catalytic activity and reaction kinetics of CO2RR, and the AgZn3 catalyst shows the highest apparent electrocatalytic activity. This work found that the activity and selectivity of CO2RR are highly dependent on the element concentrations and phase compositions, which is inspiring to explore Ag-Zn alloy catalysts with promising CO2RR properties.
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Pinthong, Piriya, Phongsathon Klongklaew, Piyasan Praserthdam, and Joongjai Panpranot. "Effect of the Nanostructured Zn/Cu Electrocatalyst Morphology on the Electrochemical Reduction of CO2 to Value-Added Chemicals." Nanomaterials 11, no. 7 (June 25, 2021): 1671. http://dx.doi.org/10.3390/nano11071671.
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Zn/Cu electrocatalysts were synthesized by the electrodeposition method with various bath compositions and deposition times. X-ray diffraction results confirmed the presence of (101) and (002) lattice structures for all the deposited Zn nanoparticles. However, a bulky (hexagonal) structure with particle size in the range of 1–10 μm was obtained from a high-Zn-concentration bath, whereas a fern-like dendritic structure was produced using a low Zn concentration. A larger particle size of Zn dendrites could also be obtained when Cu2+ ions were added to the high-Zn-concentration bath. The catalysts were tested in the electrochemical reduction of CO2 (CO2RR) using an H-cell type reactor under ambient conditions. Despite the different sizes/shapes, the CO2RR products obtained on the nanostructured Zn catalysts depended largely on their morphologies. All the dendritic structures led to high CO production rates, while the bulky Zn structure produced formate as the major product, with limited amounts of gaseous CO and H2. The highest CO/H2 production rate ratio of 4.7 and a stable CO production rate of 3.55 μmol/min were obtained over the dendritic structure of the Zn/Cu–Na200 catalyst at −1.6 V vs. Ag/AgCl during 4 h CO2RR. The dissolution and re-deposition of Zn nanoparticles occurred but did not affect the activity and selectivity in the CO2RR of the electrodeposited Zn catalysts. The present results show the possibilities to enhance the activity and to control the selectivity of CO2RR products on nanostructured Zn catalysts.
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Ren, Shaoxuan, Dorian Joulié, Danielle Salvatore, Kristian Torbensen, Min Wang, Marc Robert, and Curtis P. Berlinguette. "Molecular electrocatalysts can mediate fast, selective CO2 reduction in a flow cell." Science 365, no. 6451 (July 25, 2019): 367–69. http://dx.doi.org/10.1126/science.aax4608.
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Practical electrochemical carbon dioxide (CO2) conversion requires a catalyst capable of mediating the efficient formation of a single product with high selectivity at high current densities. Solid-state electrocatalysts achieve the CO2 reduction reaction (CO2RR) at current densities ≥ 150 milliamperes per square centimeter (mA/cm2), but maintaining high selectivities at high current densities and efficiencies remains a challenge. Molecular CO2RR catalysts can be designed to achieve high selectivities and low overpotentials but only at current densities irrelevant to commercial operation. We show here that cobalt phthalocyanine, a widely available molecular catalyst, can mediate CO2 to CO formation in a zero-gap membrane flow reactor with selectivities > 95% at 150 mA/cm2. The revelation that molecular catalysts can work efficiently under these operating conditions illuminates a distinct approach for optimizing CO2RR catalysts and electrolyzers.
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Lin, Roger, Jiaxun Guo, Xiaojia Li, Poojan Patel, and Ali Seifitokaldani. "Electrochemical Reactors for CO2 Conversion." Catalysts 10, no. 5 (April 26, 2020): 473. http://dx.doi.org/10.3390/catal10050473.
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Increasing risks from global warming impose an urgent need to develop technologically and economically feasible means to reduce CO2 content in the atmosphere. Carbon capture and utilization technologies and carbon markets have been established for this purpose. Electrocatalytic CO2 reduction reaction (CO2RR) presents a promising solution, fulfilling carbon-neutral goals and sustainable materials production. This review aims to elaborate on various components in CO2RR reactors and relevant industrial processing. First, major performance metrics are discussed, with requirements obtained from a techno-economic analysis. Detailed discussions then emphasize on (i) technical benefits and challenges regarding different reactor types, (ii) critical features in flow cell systems that enhance CO2 diffusion compared to conventional H-cells, (iii) electrolyte and its effect on liquid phase electrolyzers, (iv) catalysts for feasible products (carbon monoxide, formic acid and multi-carbons) and (v) strategies on flow channel and anode design as next steps. Finally, specific perspectives on CO2 feeds for the reactor and downstream purification techniques are annotated as part of the CO2RR industrial processing. Overall, we focus on the component and system aspects for the design of a CO2RR reactor, while pointing out challenges and opportunities to realize the ultimate goal of viable carbon capture and utilization technology.
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Sassone, Daniele, Juqin Zeng, Marco Fontana, Adriano Sacco, M. Amin Farkhondehfal, Monica Periolatto, Candido F. Pirri, and Sergio Bocchini. "Polymer-metal complexes as emerging catalysts for electrochemical reduction of carbon dioxide." Journal of Applied Electrochemistry 51, no. 9 (June 21, 2021): 1301–11. http://dx.doi.org/10.1007/s10800-021-01585-7.
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AbstractA class of metal-doped polyanilines (PANIs) was synthesized and investigated as electrocatalysts for the carbon dioxide reduction reaction (CO2RR). These materials show good affinity for the electrode substrate and allow to obtain stable binder-free electrodes, avoiding the utilization of expensive ionomer and additives. The emeraldine-base polyaniline (EB-PANI), in absence of metal dopant, shows negligible electrocatalytic activity and selectivity toward the CO2RR. Such behavior significantly improves once EB-PANI is doped with an appropriate cationic metal (Mn, Cu or Sn). In particular, the Sn-PANI outperforms other metal-doped samples, showing a good turnover frequency of 72.2 h−1 for the CO2RR at − 0.99 V vs the reversible hydrogen electrode and thus satisfactory activity of metal single atoms. Moreover, the Sn-PANI also displays impressive stability with a 100% retention of the CO2RR selectivity and an enhanced current density of 4.0 mA cm−2 in a 10-h test. PANI, a relatively low-cost substrate, demonstrates to be easily complexed with different metal cations and thus shows high tailorability. Complexing metal with conductive polymer represents an emerging strategy to realize active and stable metal single-atom catalysts, allowing efficient utilization of metals, especially the raw and precious ones. Graphic abstract
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Gao, Jinghan, Lin Cheng, Kai Li, Ying Wang, and Zhijian Wu. "Electrochemical CO2 Reduction On Two-Dimensional Metal 1,3,5-triamino-2,4,6-Benzenetriol Frameworks: A Density Functional Study." Journal of The Electrochemical Society 169, no. 2 (February 1, 2022): 024513. http://dx.doi.org/10.1149/1945-7111/ac51f7.
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Electrocatalytic CO2 reduction reaction (CO2RR) is a very prospective strategy to reduce CO2 to valuable fuels and chemical products, thereby alleviating the growing energy crisis and greenhouse effect. In this study, CO2RR mechanisms on M3(TABTO)2 (M = Sc-Cu, Y-Mo and Ru-Rh, TABTO = 1,3,5-triamino-2,4,6-benzenetriol) are investigated by means of density functional method. The results show that the studied catalysts are stable thermodynamically. Co3(TABTO)2 exhibits the best catalytic performance for the formation of CH3OH with the same overpotential of 0.41 V both in the gas phase and in solution. For Fe3(TABTO)2, however, the product is HCOOH with the overpotential of 0.29 V in the gas phase and 0.70 V in solution. For Ru3(TABTO)2 to produce CH4, solvent effect reduces the overpotential significantly from 0.97 V in the gas phase to 0.54 V in solution, making it to be a promising CO2RR catalyst. Moreover, the improvement of CO2RR catalyst activity can be achieved by the axial oxygen modification in M3(TABTO)2 (M = Sc, Y and V). A good relationship between d band center and overpotential is observed, which might provide us with a new direction to design the promising catalyst.
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Kaplan, Ekrem, Selin Gümrükçü, Metin Gençten, Yücel Şahin, and Esin Hamuryudan. "Thiophene Functionalized Porphyrin for Electrochemical Carbon Dioxide Reduction." Journal of The Electrochemical Society 168, no. 12 (December 1, 2021): 126512. http://dx.doi.org/10.1149/1945-7111/ac3e7b.
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The production of catalysts that display strong efficiencies in aqueous media for the electrochemical carbon dioxide reduction reaction (CO2RR) is essential both for a healthy world and for realistic application of energy waste to generate value-added fuels. In this study, thiophene functionalized metal-free (poly-H2Por) and cobalt porphyrin-based (poly-CoPor) organometallic catalysts were easily attached on the pencil graphite electrode surface via electrochemical polymerization method and these, porphyrin coated, pencil graphite electrodes (PGE) were used as electrocatalysts for electrochemical CO2 reduction for the first time in the literature. To reveal the electrochemical activity of CO2RR, the electropolymerized catalysts were investigated with linear sweep voltammetry in 0.1 M KHCO3 solution. The results showed that, the electrode which is modified with poly-CoPor decreased the overpotential of CO2RR, according to bare pencil graphite electrode, from −1.35 V to −0.63 V.
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Sharifi Golru, Samaneh, and Elizabeth J. Biddinger. "Influence of the Nature of Ionic Additives in Aqueous Electrolyte on CO2 Electroreduction over Cu Catalysts." ECS Meeting Abstracts MA2022-01, no. 56 (July 7, 2022): 2340. http://dx.doi.org/10.1149/ma2022-01562340mtgabs.
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CO2 electroreduction (CO2ER) has attracted considerable attention due to its promising results in producing valuable chemicals and fuels and mitigating global warming. Among different electrolytes, water-based solutions are the most common electrolytes for CO2ER due to their low cost, abundance, and eco-friendliness. However, the product selectivity and activity in aqueous electrolytes are poor due to their low CO2 solubility and the presence of the competing hydrogen evolution reaction (HER). Using ionic additives such as inorganic salts and ionic liquids can enhance CO2ER by controlling the water and CO2 concentration at the interface. Ionic additives can also impact the intermediate stability on the surface. In this study, the effect of additive anion and cation on CO2ER has been studied. A series of salts (10 mM) with different anions and cations were added to 0.1 M potassium bicarbonate (KHCO3). Bis(trifluoromethylsulfonyl)imide [NTF2]- or dicyanamide [DCA]- as anion were chosen due to their significantly different hydrophobicity and CO2 absorption capacity. Sodium (Na+), potassium (K+), 1-ethyl-3-methylimidazolium [EMIM]+, and 1-butyl-3-methylimidazolium [BMIM]+ were used as cation. Results showed that the effect of anion is more significant on CO2ER compared to cations. Adding DCA-based salts, regardless of the cation type significantly enhanced HER and suppressed CO2ER. According to the cyclic voltammetry in N2-saturated electrolytes with DCA anions, a current density ~44 mA/cm2 (regardless of the cation type) was observed at -1.12 V vs. RHE. By saturating the DCA electrolytes with CO2, the total current density decreased. Regarding the product selectivity, [DCA]-based salts also had a high faradaic efficiency (FE) for hydrogen and a very low FE for hydrocarbons even at high overpotentials. This can be justified by high hydrophilicity and strong adsorption of DCA-salts on the surface. The strong adsorption of DCA-salts was also confirmed by X-ray photoelectron spectroscopy (XPS) and In-situ electrochemical quartz crystal microbalance (EQCM). Strongly adsorbed DCA ions on the surface can promote hydrogen evolution reaction, destabilize the intermediates and suppress CO2ER. On the other hand, NTF2-based salts showed a lower HER activity compared to DCA-salts. Among different cations with NTF2 anion, Na[NTF2] showed a higher HER compared to [EMIM][NTF2] and [BMIM][NTF2]. According to the cyclic voltammetry in N2-saturated electrolytes with NTF2 anions, NaNTF2 showed a current density of ~14 mA/cm2 at -1.12 V vs. By saturating the NTF2 electrolytes with CO2, the total current density increased, in opposite to DCA-salts. This can show that NTF2 salts are able to enhance CO2ER. This can be due to their high hydrophobicity and CO2 absorption capacity. The best performance was observed for [BMIM][NTF2]. [BMIM][NTF2] showed a high faradaic efficiency (38.7%) for formate at -0.92 V vs. RHE. Electrochemical impedance spectroscopy (EIS) showed that the charge transfer resistance is more impacted by the anion nature. DCA salts showed a lower charge transfer resistance compared to NTF2 salts probably due to the enhanced HER which is kinetically faster than CO2ER. Moreover, an inductive loop was observed in EIS for both [EMIM][NTF2] and [BMIM][NTF2] additives (not for Na[NTF2]) which can be indicative of the interaction of CO2 with imidazolium cations at the interface which can facilitate formate formation.
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He, Yanghua, and Piotr Zelenay. "(Invited) Effect of Nanostructure and Surface Chemistry on Activity and Selectivity of Cu-Based Electrocatalysts for Carbon Dioxide Reduction." ECS Meeting Abstracts MA2022-01, no. 49 (July 7, 2022): 2096. http://dx.doi.org/10.1149/ma2022-01492096mtgabs.
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Electrochemical conversion of carbon dioxide (CO2) to value-added chemicals using electricity from renewable sources represents a promising path to carbon-neutral fuel cycle and enhanced economic benefits.1 To date, copper (Cu) has been the leading metal electrocatalyst for the electroreduction of CO2 to high-value chemicals: fuels and chemical feedstocks. Although there has been a significant progress in CO2 reduction reaction (CO2RR), the overall CO2RR performance of Cu-based electrocatalysts is still limited by poor selectivity, resulting in a variety of products, such as hydrogen, carbon monoxide, formic acid, methane, and ethylene.2 Enhancing the CO2RR rate relative to the competing hydrogen evolution reaction (HER) and achieving high selectivity for multi-carbon products thus represent the major scientific challenges. In this presentation, we will summarize our study of innovative Cu-based catalysts aimed at producing high energy-density chemicals, enhancing the understanding of reaction mechanism, and bringing CO2RR closer to practical application. The study has focused on the relationship between the composition and structure of Cu-based electrocatalysts, especially the nanostructure and oxidation states (Cu0, Cu+, and Cu2+), on CO2RR activity. By using a novel approach in the catalyst synthesis we have been able to obtain Cu-based materials with controlled nanostructure, e.g., pore-size distribution, higher surface area, and correlate the catalyst morphology with the selectivity for multi-carbon products. We have associated the formation of CO2RR products with the presence of different active sites on the catalyst surface, a necessary step towards achieving desirable selectivity. We will also recap the results of a study on the effect of adding a secondary transition metal, e.g., Zn, Ni, and Ag, on electrocatalytic properties of Cu-based catalysts. The rationale behind this approach has been to tune electrocatalytic activity and selectivity via changing the binding strength of the key intermediates, such as *OCHO, *CO, *COOH, *CHO, and *COH. References G. Kibria, J. P. Edwards, C. M. Gabardo, C.-T. Dinh, A. Seifitokaldani, D. Sinton, and E. H. Sargent, Adv. Mater. 2019, 31, 1807166. S. Nitopi, E. Bertheussen, S. B. Scott, X. Liu, A. K. Engstfeld, S. Horch, B. Seger, I. E. L. Stephens, K. Chan, C. Hahn, J. K. Nørskov, T. F. Jaramillo, and I. Chorkendorff, Chem. Rev. 2019, 119, 7610−7672.
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Wakayama, Hiroaki, and Yoshiaki Fukushima. "Supercritical CO2for Making Nanoscale Materials." Industrial & Engineering Chemistry Research 45, no. 10 (May 2006): 3328–31. http://dx.doi.org/10.1021/ie050658r.
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Kauffman, Douglas R., and Dominic R. Alfonso. "(Invited) Ligand-Directed CO2 Conversion at Bimetallic Au/Cu Nanocatalysts." ECS Meeting Abstracts MA2018-01, no. 31 (April 13, 2018): 1835. http://dx.doi.org/10.1149/ma2018-01/31/1835.
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The electrochemical CO2 reduction reaction (CO2RR) is a promising approach for converting waste CO2 emissions into value-added chemicals and fuels. Product selectivity will be a key requirement because down-stream chemical separation steps will introduce cost barriers and reduce the efficiency of large-scale systems. Gold electrocatalysts selectively convert CO2 into CO, which can be further processed into a wide range of other commodity chemicals, industrial precursors, and fuel additives. Copper is another popular material because it is less expensive and can directly produce hydrocarbons, but it typically demonstrates a wider product distribution than gold. Bimetallic gold-copper electrocatalysts have emerged as promising candidates for selective CO2 conversion with lower precious metal loadings, but most Au/Cu systems reported to date demonstrate lower product selectivity than pure gold. Here, we’ve combined experiment and theory to describe the CO2RR performance of monodisperse (~1.5 nm), thiol-capped, gold-copper nanoparticles (Au/Cu NPs) containing between 0-64% copper. NPs containing 49% Cu demonstrated the best performance with 94±5% CO Faradaic efficiency between -0.5V to -1.0V vs. RHE and turnover frequencies reaching 60 molecules site-1 s-1. This activity represents a 4-8 fold improvement in catalytic activity and improved product selectivity compared with identically sized, thiol capped Au NPs. X-ray absorption spectroscopy and extended x-ray absorption fine structure (EXAFS) analysis characterized the Au/Cu NP electronic structure and identified unique copper-thiol structures at the NP surface. Complementary density functional theory modeling with realistic, thiol-capped Au/Cu NP structures identified key relationships between NP composition and electrocatalytic performance. Our results show that unique copper-thiol surface structures on the Au/Cu NPs influenced CO2RR performance by stabilizing bound *CO reaction intermediates and preventing H2 evolution. Experiment and theory both indicated less-selective CO2RR at ligand-free NPs, and ligand-free Au/Cu NPs produced H2 with approximately 95% selectivity. Our combination of experiment and theory demonstrate that ligand-directed surface structuring can influence NP chemistry, improve CO2RR product selectivity, and produce highly active electrocatalysts with reduced precious metal loadings.
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Kondrat’ev, D. A., I. V. Tolstobrov, A. N. Bushuev, O. V. El’kin, O. S. Bervitskaya, and O. V. Chernova. "Powder Co2Er Intermetallic Compound Synthesis Conditions in a Halide Melt." Russian Metallurgy (Metally) 2018, no. 2 (February 2018): 174–77. http://dx.doi.org/10.1134/s0036029518020076.
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Song, Yujiang. "Pyrolysis of Self-Assembled Metalloporphyrins Toward ORR and/or CO2RR." ECS Meeting Abstracts MA2020-01, no. 12 (May 1, 2020): 934. http://dx.doi.org/10.1149/ma2020-0112934mtgabs.
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Kao, Yi-Lin, Stephen Paul, Iris Herrmann-Geppert, Ulrike Ingrid Kramm, and Peter Bogdanoff. "(Invited) Electroreduction of CO2 (CO2RR) on Pyrolysed Transition Metal Porphyrins." ECS Meeting Abstracts MA2020-01, no. 51 (May 1, 2020): 2795. http://dx.doi.org/10.1149/ma2020-01512795mtgabs.
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Liu, Shiyuan, Botao Hu, Junkai Zhao, Wenjun Jiang, Deqiang Feng, Ce Zhang, and Wei Yao. "Enhanced Electrocatalytic CO2 Reduction of Bismuth Nanosheets with Introducing Surface Bismuth Subcarbonate." Coatings 12, no. 2 (February 11, 2022): 233. http://dx.doi.org/10.3390/coatings12020233.
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The electrocatalytic CO2 reduction reaction (CO2RR) into hydrocarbon products is one of the most promising approaches for CO2 utilization in modern society. However, the application of CO2RR requires optimizing state-of-the-art catalysts as well as elucidating the catalytic interface formation mechanism. In this study, a flower-like nano-structured Bi catalyst is prepared by a facile pulse current electrodeposition method wherein the morphologies could be accurately controlled. Interestingly, nano-structured Bi is inclined to generate Bi2O2CO3 in the air and form a stable Bi2O2CO3@Bi interface, which could enhance the CO2 adsorption and conversion. In-situ Raman spectroscopy analysis also proves the existence of Bi2O2CO3 on the electrode surface. In a practical CO2 reduction test by a flow-cell reactor, the Bi2O2CO3@Bi electrode delivers a high faradaic efficiency of the CO2 to formate/formic acid (~90%) at −1.07 V vs. reversible hydrogen electrode (RHE) with no obvious decay during more than a 10 h continuous test. The introducing surface Bi2O2CO3 in nano-structured Bi supports a promising strategy as well as facile access to prepare improved CO2RR electrocatalysts.
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Chen, Qisi, Panagiotis Tsiakaras, and Peikang Shen. "Electrochemical Reduction of Carbon Dioxide: Recent Advances on Au-Based Nanocatalysts." Catalysts 12, no. 11 (November 2, 2022): 1348. http://dx.doi.org/10.3390/catal12111348.
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The electrocatalytic reduction of CO2 to other high value-added chemicals under ambient conditions is a promising and ecofriendly strategy to achieve sustainable carbon recycling. However, the CO2 reduction reaction (CO2RR) is still confronted with a large number of challenges, such as high reaction overpotential and low product selectivity. Therefore, the rapid development of appropriate electrocatalysts is the key to promoting CO2 electroreduction. Over the past few decades, Au-based nanocatalysts have been demonstrated to be promising for the selective CO2RR to CO owing to their low reaction overpotential, good product selectivity, high Faraday efficiency and inhibition of the hydrogen evolution reaction. In this respect, this review first introduces the fundamentals of the electrochemical reduction of CO2 and then focuses on recent accomplishments with respect to Au-based nanocatalysts for CO2RR. The manipulation of various factors, e.g., the nanoporous structure, nanoparticle size, composition, morphology, support and ligand, allows for the identification of several clues for excellent Au-based nanocatalysts. We hope that this review will offer readers some important insights on Au-based catalyst design and provide new ideas for developing robust electrocatalysts.
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Karthik, S. V., A. Rajanikanth, Y. K. Takahashi, T. Ohkubo, and K. Hono. "Microstructure and spin polarization of quaternary Co2Cr1−xVxAl, Co2V1−xFexAl and Co2Cr1−xFexAl Heusler alloys." Acta Materialia 55, no. 11 (June 2007): 3867–74. http://dx.doi.org/10.1016/j.actamat.2007.03.003.
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Zou, Yingbing, Tingting Zhan, Ying Yang, Zhiwen Fan, Yunbin Li, Yongfan Zhang, Xiuling Ma, Qianhuo Chen, Shengchang Xiang, and Zhangjing Zhang. "Single-phase proton- and electron-conducting Ag-organic coordination polymers for efficient CO2 electroreduction." Journal of Materials Chemistry A 10, no. 6 (2022): 3216–25. http://dx.doi.org/10.1039/d1ta09548j.
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Niu, Di, Cong Wei, Zheng Lu, Yanyan Fang, Bo Liu, Da Sun, Xiaobin Hao, Hongge Pan, and Gongming Wang. "Cu2O-Ag Tandem Catalysts for Selective Electrochemical Reduction of CO2 to C2 Products." Molecules 26, no. 8 (April 9, 2021): 2175. http://dx.doi.org/10.3390/molecules26082175.
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The electrochemical carbon dioxide reduction reaction (CO2RR) to C2 chemicals has received great attention. Here, we report the cuprous oxide (Cu2O) nanocubes cooperated with silver (Ag) nanoparticles via the replacement reaction for a synergetic CO2RR. The Cu2O-Ag tandem catalyst exhibits an impressive Faradaic efficiency (FE) of 72.85% for C2 products with a partial current density of 243.32 mA·cm−2. The electrochemical experiments and density functional theory (DFT) calculations reveal that the introduction of Ag improves the intermediate CO concentration on the catalyst surface and meanwhile reduces the C-C coupling reaction barrier energy, which is favorable for the synthesis of C2 products.
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Ait Ahsaine, Hassan, Mohamed Zbair, Amal BaQais, and Madjid Arab. "CO2 Electroreduction over Metallic Oxide, Carbon-Based, and Molecular Catalysts: A Mini-Review of the Current Advances." Catalysts 12, no. 5 (April 19, 2022): 450. http://dx.doi.org/10.3390/catal12050450.
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Electrochemical CO2 reduction reaction (CO2RR) is one of the most challenging targets of current energy research. Multi-electron reduction with proton-coupled reactions is more thermodynamically favorable, leading to diverse product distribution. This requires the design of stable electroactive materials having selective product generation and low overpotentials. In this review, we have explored different CO2RR electrocatalysts in the gas phase and H-cell configurations. Five groups of electrocatalysts ranging from metals and metal oxide, single atom, carbon-based, porphyrins, covalent, metal–organic frameworks, and phthalocyanines-based electrocatalysts have been reviewed. Finally, conclusions and prospects have been elaborated.
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Ummireddi, Ashok Kumar, Shilendra Kumar Sharma, and Raj Ganesh S. Pala. "Ammonium ionic liquid cation promotes electrochemical CO2 reduction to ethylene over formate while inhibiting the hydrogen evolution on a copper electrode." Catalysis Science & Technology 12, no. 2 (2022): 519–29. http://dx.doi.org/10.1039/d1cy01584b.
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