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1
Dagorne, Samuel. „Recent Developments on N-Heterocyclic Carbene Supported Zinc Complexes: Synthesis and Use in Catalysis“. Synthesis 50, Nr. 18 (28.06.2018): 3662–70. http://dx.doi.org/10.1055/s-0037-1610088.
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The present contribution reviews the synthesis, reactivity, and use in catalysis of NHC–Zn complexes reported since 2013. NHC-stabilized Zn(II) species typically display enhanced stability relative to common organozinc species (such as Zn dialkyls), a feature of interest for the mediation of various chemical processes and the stabilization of reactive Zn-based species. Their use in catalysis is essentially dominated by reduction reactions of various unsaturated small molecules (including CO2), thus primarily involving Zn–H and Zn–alkyl derivatives as catalysts. Simple NHC adducts of Zn(II) dihalides also appear as effective catalysts for the reduction amination of CO2 and borylation of alkyl/aryl halides. Stable and well-defined Zn alkoxides have also been prepared and behave as effective catalysts in the polymerization of cyclic esters/carbonates for the production of well-defined biodegradable materials. Overall, the attractive features of NHC-based Zn(II) species include ready access, a reasonable stability/reactivity balance, and steric/electronic tunability (through the NHC source), which should promote their further development.1 Introduction2 NHC-Supported Zinc Alkyl/Aryl Species2.1 Synthesis2.2 Reactivity and Use in Catalysis3 NHC-Supported Zinc Hydride Species3.1 Synthesis3.2 Reactivity and Use in Catalysis4 NHC-Supported Zinc Amido/Alkoxide Species4.1 Synthesis4.2 Use in Catalysis5 NHC-Supported Zinc Dihalide Species5.1 Synthesis5.2 Use in Catalysis6 Other NHC-Stabilized Zn Species7 Conclusion
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Tian, Jindan, Ru Han, Qiangsheng Guo, Zhe Zhao und Na Sha. „Direct Conversion of CO2 into Hydrocarbon Solar Fuels by a Synergistic Photothermal Catalysis“. Catalysts 12, Nr. 6 (02.06.2022): 612. http://dx.doi.org/10.3390/catal12060612.
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Photothermal coupling catalysis technology has been widely studied in recent years and may be a promising method for CO2 reduction. Photothermal coupling catalysis can improve chemical reaction rates and realize the controllability of reaction pathways and products, even in a relatively moderate reaction condition. It has inestimable value in the current energy and global environmental crisis. This review describes the application of photothermal catalysis in CO2 reduction from different aspects. Firstly, the definition and advantages of photothermal catalysis are briefly described. Then, different photothermal catalytic reductions of CO2 products and catalysts are introduced. Finally, several strategies to improve the activity of photothermal catalytic reduction of CO2 are described and we present our views on the future development and challenges of photothermal coupling. Ultimately, the purpose of this review is to bring more researchers’ attention to this promising technology and promote this technology in solar fuels and chemicals production, to realize the value of the technology and provide a better path for its development.
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Srivastava, Sumit, Manvender S. Dagur, Afsar Ali und Rajeev Gupta. „Trinuclear {Co2+–M3+–Co2+} complexes catalyze reduction of nitro compounds“. Dalton Transactions 44, Nr. 40 (2015): 17453–61. http://dx.doi.org/10.1039/c5dt03442f.
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Trinuclear {Co2+–Co3+–Co2+} and {Co2+–Fe3+–Co2+} complexes function as reusable heterogeneous catalysts for the selective reduction of assorted nitro compounds to their corresponding amines. The mechanistic investigations suggest the involvement of a Co(ii)–Co(i) cycle in the catalysis.
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Lisovski, Oleg, Sergei Piskunov, Dmitry Bocharov, Yuri Zhukovskii, Janis Kleperis, Ainars Knoks und Peteris Lesnicenoks. „CO2 and CH2 Adsorption on Copper-Decorated Graphene: Predictions from First Principle Calculations“. Crystals 12, Nr. 2 (28.01.2022): 194. http://dx.doi.org/10.3390/cryst12020194.
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Single-layer graphene decorated with monodisperse copper nanoparticles can support the size and mass-dependent catalysis of the selective electrochemical reduction of CO2 to ethylene (C2H4). In this study, various active adsorption sites of nanostructured Cu-decorated graphene have been calculated by using density functional theory to provide insight into its catalytic activity toward carbon dioxide electroreduction. Based on the results of our calculations, an enhanced adsorption of the CO2 molecule and CH2 counterpart placed atop of Cu-decorated graphene compared to adsorption at pristine Cu metal surfaces was predicted. This approach explains experimental observations for carbon-based catalysts that were found to be promising for the two-electron reduction reaction of CO2 to CO and, further, to ethylene. Active adsorption sites that lead to a better catalytic activity of Cu-decorated graphene, with respect to general copper catalysts, were identified. The atomic configuration of the most selective CO2 toward the reduction reaction nanostructured catalyst is suggested.
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Petersen, Haley A., Tessa H. T. Myren und Oana R. Luca. „Redox-Active Manganese Pincers for Electrocatalytic CO2 Reduction“. Inorganics 8, Nr. 11 (11.11.2020): 62. http://dx.doi.org/10.3390/inorganics8110062.
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The decrease of total amount of atmospheric CO2 is an important societal challenge in which CO2 reduction has an important role to play. Electrocatalytic CO2 reduction with homogeneous catalysts is based on highly tunable catalyst design and exploits an abundant C1 source to make valuable products such as fuels and fuel precursors. These methods can also take advantage of renewable electricity as a green reductant. Mn-based catalysts offer these benefits while incorporating a relatively cheap and abundant first-row transition metal. Historically, interest in this field started with Mn(bpy-R)(CO)3X, whose performance matched that of its Re counterparts while achieving substantially lower overpotentials. This review examines an emerging class of homogeneous Mn-based electrocatalysts for CO2 reduction, Mn complexes with meridional tridentate coordination also known as Mn pincers, most of which contain redox-active ligands that enable multi-electron catalysis. Although there are relatively few examples in the literature thus far, these catalysts bring forth new catalytic mechanisms not observed for the well-established Mn(bpy-R)(CO)3X catalysts, and show promising reactivity for future studies.
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Hahn, Christopher. „(Invited) Steering Electrocatalytic CO2 Reduction Reactivity Using Microenvironments“. ECS Meeting Abstracts MA2022-02, Nr. 49 (09.10.2022): 1879. http://dx.doi.org/10.1149/ma2022-02491879mtgabs.
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A key challenge in electrocatalysis is co-designing the catalyst and its microenvironment to work in concert to efficiently steer complex reaction networks. First, I will describe the development of a tandem catalysis strategy on Au/Cu electrocatalysts to control the potential energy landscape of the CO2 and CO reduction at length scales beyond the active site and achieve synergistic catalytic activity for alcohols superior to that of either Cu or Au. Next, I will provide examples of CO2 reduction on catalysts supported on gas diffusion electrodes to discuss how the intrinsic catalysis and mass transport are interconnected through microenvironments, leading to emergent catalytic properties under industrially relevant reaction rates. Finally, I will conclude by providing our perspective on key remaining challenges to the scale-up of CO2 electrolyzers within the context of electrifying the chemicals manufacturing sector.
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Cao, Yanwei, Qiongyao Chen, Chaoren Shen und Lin He. „Polyoxometalate-Based Catalysts for CO2 Conversion“. Molecules 24, Nr. 11 (30.05.2019): 2069. http://dx.doi.org/10.3390/molecules24112069.
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Polyoxometalates (POMs) are a diverse class of anionic metal-oxo clusters with intriguing chemical and physical properties. Owing to unrivaled versatility and structural variation, POMs have been extensively utilized for catalysis for a plethora of reactions. In this focused review, the applications of POMs as promising catalysts or co-catalysts for CO2 conversion, including CO2 photo/electro reduction and CO2 as a carbonyl source for the carbonylation process are summarized. A brief perspective on the potentiality in this field is proposed.
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Zhou, Yiying, Junxi Cai, Yuming Sun, Shuhan Jia, Zhonghuan Liu, Xu Tang, Bo Hu, Yue Zhang, Yan Yan und Zhi Zhu. „Research on Cu-Site Modification of g-C3N4/CeO2-like Z-Scheme Heterojunction for Enhancing CO2 Reduction and Mechanism Insight“. Catalysts 14, Nr. 8 (20.08.2024): 546. http://dx.doi.org/10.3390/catal14080546.
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In this work, the successful synthesis of a Cu@g-C3N4/CeO2-like Z-scheme heterojunction through hydrothermal and photo-deposition methods represents high CO2 reduction activity with remarkable CO selectivity, as evidenced by the impressive CO yield of 33.8 μmol/g for Cu@g-C3N4/CeO2, which is over 10 times higher than that of g-C3N4 and CeO2 individually. The characterization and control experimental results indicate that the formation of heterojunctions and the introduction of Cu sites promote charge separation and the transfer of hot electrons, as well as the photothermal effect, which are the essential reasons for the improved CO2 reduction activity. Remarkably, Cu@g-C3N4/CeO2 still exhibits about 92% performance even after multiple cycles. In situ FTIR was utilized to confirm the production of COOH* at 1472 cm−1 and to elucidate the mechanism behind the high selectivity for CO production. The study’s investigation into the wide-ranging applicability of the Cu@g-C3N4/CeO2-like Z-scheme heterojunction catalysts is noteworthy, and the exploration of potential reaction mechanisms for CO2 reduction adds valuable insights to the field of catalysis.
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Xue, Sensen, Xingyou Liang, Qing Zhang, Xuefeng Ren, Liguo Gao, Tingli Ma und Anmin Liu. „Density Functional Theory Study of CuAg Bimetal Electrocatalyst for CO2RR to Produce CH3OH“. Catalysts 14, Nr. 1 (20.12.2023): 7. http://dx.doi.org/10.3390/catal14010007.
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Converting superfluous CO2 into value-added chemicals is regarded as a practical approach for alleviating the global warming problem. Powered by renewable electricity, CO2 reduction reactions (CO2RR) have attracted intense interest owing to their favorable efficiency. Metal catalysts exhibit high catalytic efficiency for CO2 reduction. However, the reaction mechanisms have yet to be investigated. In this study, CO2RR to CH3OH catalyzed by CuAg bimetal is theoretically investigated. The configurations and stability of the catalysts and the reaction pathway are studied. The results unveil the mechanisms of the catalysis process and prove the feasibility of CuAg clusters as efficient CO2RR catalysts, serving as guidance for further experimental exploration. This study provides guidance and a reference for future work in the design of mixed-metal catalysts with high CO2RR performance.
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Hall, Anthony Shoji, Youngmin Yoon, Anna Wuttig und Yogesh Surendranath. „Mesostructure-Induced Selectivity in CO2 Reduction Catalysis“. Journal of the American Chemical Society 137, Nr. 47 (18.11.2015): 14834–37. http://dx.doi.org/10.1021/jacs.5b08259.
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Geri, Jacob B., Joanna L. Ciatti und Nathaniel K. Szymczak. „Charge effects regulate reversible CO2 reduction catalysis“. Chemical Communications 54, Nr. 56 (2018): 7790–93. http://dx.doi.org/10.1039/c8cc04370a.
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Modular but geometrically constrained ligands were used to investigate the impact of key ligand design parameters (charge and bite angle) on CO2 hydrogenation and formic acid dehydrogenation activity.
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Jia, Mingwen, Qun Fan, Shizhen Liu, Jieshan Qiu und Zhenyu Sun. „Single-atom catalysis for electrochemical CO2 reduction“. Current Opinion in Green and Sustainable Chemistry 16 (April 2019): 1–6. http://dx.doi.org/10.1016/j.cogsc.2018.11.002.
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Grills, David C., Mehmed Z. Ertem, Meaghan McKinnon, Ken T. Ngo und Jonathan Rochford. „Mechanistic aspects of CO2 reduction catalysis with manganese-based molecular catalysts“. Coordination Chemistry Reviews 374 (November 2018): 173–217. http://dx.doi.org/10.1016/j.ccr.2018.05.022.
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Xie, Wen-Jun, Olga M. Mulina, Alexander O. Terent’ev und Liang-Nian He. „Metal–Organic Frameworks for Electrocatalytic CO2 Reduction into Formic Acid“. Catalysts 13, Nr. 7 (15.07.2023): 1109. http://dx.doi.org/10.3390/catal13071109.
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Metal–organic frameworks (MOFs) are used in catalysis due to their high specific surface area and porous structure. The dispersed active sites and limited reaction space that render MOFs have the potential for highly selective electrocatalytic CO2 reduction reaction (ECO2RR). Meanwhile, formic acid (HCOOH) is attracting attention as a liquid product with high economic benefits. This review summarizes the MOFs and their derivatives applied for ECO2RR into HCOOH products. The preparation methods of MOFs as electrocatalysts and their unique advantages are discussed. A series of MOFs and MOF derivatives obtained by electrochemical reduction or carbonization processes are highlighted, including metal nanomaterials, carbon-based nanocomposites, single-atom catalysts, and bimetallic nanocomposites. Depending on the MOF building units (metal ions and organic linkers) and the reaction conditions of derivatization, MOF-based catalysts exhibit rich diversity and controllable modulation of catalytic performance. Finally, the challenges encountered at this stage and the future research directions of MOF-based catalysts are proposed.
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Cobb, Samuel J., Azim M. Dharani, Ana Rita Oliveira, Inês A. C. Pereira und Erwin Reisner. „Using Enzymes to Understand and Control the Local Environment of Catalysis“. ECS Meeting Abstracts MA2023-02, Nr. 52 (22.12.2023): 2530. http://dx.doi.org/10.1149/ma2023-02522530mtgabs.
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Local environments within porous electrodes are an inherent, but often neglected component of catalysis as the local conversion of reactants to products means catalysis occurs in a very different environment to bulk solution. By understanding and modifying these local environments using a combination of experimental and computational techniques, we show how to improve the performance of electrocatalytic reactions to address the climate crisis by efficiently converting renewable energy to chemical fuels. The selectivity and activity of enzymes means they are ideal model catalysts that can guide the design of synthetic systems. However, they must be in an environment that is close to their optimal to operate efficiently, with small changes in properties such as pH drastically affecting their activity. By optimising their local environment, the rates of fuel formation can be drastically (>18×) increased.[1] We also demonstrate the crucial role of CO2 hydration kinetics on the local pH and CO2 concentration using the enzyme Carbonic Anhydrase co-immobilised with Formate Dehydrogenase.[2] Carbonic Anhydrase catalyses CO2 hydration, causing CO2 to act as a better buffer to mitigate changes in the local pH environment allowing the system to operate closer to its optimal and how this contrasts with heterogeneous CO2 reduction. (fig. 1a) We extend this approach to low CO2 concentrations, taking inspiration from the natural carboxysome to develop a system where Formate Dehydrogenase and Carbonic Anhydrase are co-immobilised in a nanoconfined structure to improve low CO2 concentration utilisation. (fig. 1b).[3] The electrolysis of dilute CO2 streams suffers from low concentrations of dissolved substrate and its rapid depletion at the electrolyte-electrocatalyst interface. These limitations require first energy-intensive CO2 capture and concentration, before electrolyzers can achieve acceptable performances. For direct electrocatalytic CO2 reduction from low-concentration sources, we introduce a strategy that mimics the carboxysome in cyanobacteria by utilizing microcompartments with nanoconfined enzymes in a porous electrode. Carbonic Anhydrase accelerates CO2 hydration kinetics and minimizes substrate depletion by making all dissolved carbon available for utilization, while a highly efficient formate dehydrogenase reduces CO2 cleanly to formate; down to even atmospheric concentrations of CO2. This bio-inspired concept demonstrates that the carboxysome provides a viable blueprint for the reduction of low-concentration CO2 streams to chemicals by using all forms of dissolved carbon. References [1] E. E. Moore, S. J. Cobb et al., Proc. Natl. Acad. Sci. USA 2022,119, e2114097119 [2] S. J. Cobb et al., Nat. Chem. 2022, 14, 417 – 424 [3] S. J. Cobb et al., Angew. Chem. Int. Ed.,2023 Just Accepted, DOI: 10.1002/anie.202218782 Figure 1
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Marquart, Wijnand, Shaine Raseale, Gonzalo Prieto, Anna Zimina, Bidyut Bikash Sarma, Jan-Dierk Grunwaldt, Michael Claeys und Nico Fischer. „CO2 Reduction over Mo2C-Based Catalysts“. ACS Catalysis 11, Nr. 3 (20.01.2021): 1624–39. http://dx.doi.org/10.1021/acscatal.0c05019.
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Yuan, Zhimin, Xianhui Sun, Haiquan Wang, Xingling Zhao und Zaiyong Jiang. „Applications of Ni-Based Catalysts in Photothermal CO2 Hydrogenation Reaction“. Molecules 29, Nr. 16 (16.08.2024): 3882. http://dx.doi.org/10.3390/molecules29163882.
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Heterogeneous CO2 hydrogenation catalytic reactions, as the strategies for CO2 emission reduction and green carbon resource recycling, play important roles in alleviating global warming and energy shortages. Among these strategies, photothermal CO2 hydrogenation technology has become one of the hot catalytic technologies by virtue of the synergistic advantages of thermal catalysis and photocatalysis. And it has attracted more and more researchers’ attentions. Various kinds of effective photothermal catalysts have been gradually discovered, and nickel-based catalysts have been widely studied for their advantages of low cost, high catalytic activity, abundant reserves and thermal stability. In this review, the applications of nickel-based catalysts in photothermal CO2 hydrogenation are summarized. Finally, through a good understanding of the above applications, future modification strategies and design directions of nickel-based catalysts for improving their photothermal CO2 hydrogenation activities are proposed.
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St. John, Allison, Esraa Ahmad, Tianqi Jin und Gonghu Li. „(Invited) Single Atom Catalysts in Functionalized Carbon Nitride for Efficient Solar CO2 Reduction“. ECS Meeting Abstracts MA2023-01, Nr. 37 (28.08.2023): 2160. http://dx.doi.org/10.1149/ma2023-01372160mtgabs.
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Single atom catalysts (SACs) have demonstrated unique properties in a variety of chemical transformations. Using graphitic carbon nitride (C3N4) as a photoactive support, we have prepared different cobalt SACs for use in solar CO2 reduction. Functionalization of C3N4 was carried out to produce well-defined N4 binding sites for cobalt ions. Spectroscopic techniques and computational tools were employed to confirm the structures of the SACs. In these photosynthetic assemblies, C3N4 absorbs visible light and, in the presence of electron donor, transfers electrons to the cobalt sites for CO2-reduction catalysis.
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Xuemei Yang and Xiaohua Wang, Xuemei Yang and Xiaohua Wang. „Reduction Reactions of CO2 on Rutile TiO2 (110) Nanosheet via Coordination Activation“. Journal of the chemical society of pakistan 44, Nr. 6 (2022): 576. http://dx.doi.org/10.52568/001180/jcsp/44.06.2022.
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Based on the previous coordination catalysis theory, the active site on the surface of transition metal oxides can activate the CO2 molecule. Ultrathin two-dimensional (2D) rutile TiO2 nanosheet with (110) crystal face as the main exposed surface has many active sites of Ti3+ and O vacancy, which have some synergistic effects to greatly reduce the dissociation energy of CO2. Following previous assumptions, four possible reduction processes of CO2 on rutile TiO2 (110) surface were systematically assessed by density functional theory (DFT) simulations. The reduction reactions of CO2 along I faces difficultly in proceeding due to the relatively weak interaction between CO2 and the active surface. Additionally, along III, the adsorption configuration of CO2 in the pristine state has huge distinctions with the model that suggests that the defined route is unlikely to occur on the rutile TiO2 (110) surface. However, through carefully comparing the energy differences as well as transition state searching, the reduction reaction along II has a high probability of finishing and finally generating HCOOH on the surface owing to the minimal energy differences and low activation barrier. Furthermore, the reduction reaction of CO2 to CH4 guided along IV is predicted to more easily take place with the assistance of O vacancy on the active surface. The synergistic action among Ti3+ site, O vacancy, and H+ can aid in fixing molecular CO2 by breaking the strong bond of C=O in CO2 and generating different fuels via coordination activation. This work will not only provide strong theoretical support to previous assumptions but can also lighten the routes to explore more active catalysis towards the reduction of CO2.
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Hahn, Christopher, und Thomas F. Jaramillo. „Electrocatalysis for CO2 Reduction: Controlling Selectivity to Oxygenates and Multicarbon Products“. ECS Meeting Abstracts MA2018-01, Nr. 31 (13.04.2018): 1832. http://dx.doi.org/10.1149/ma2018-01/31/1832.
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Many technical challenges remain for the implementation of CO2 electrolysis as a practical means for CO2 utilization. Here, we outline strategies for improving the performance of catalysts for the electroreduction of CO2 to oxygenated and multicarbon reduction products. To this end, we will first discuss how engineering the surface structure of Cu electrocatalysts led to the discovery of active site structure-selectivity relationships. Using a combination of electrocatalysis experiments and in situ surface probe microscopy, we demonstrate that undercoordinated sites are selective motifs for oxygenates and C-C coupling. By comparing these results with state-of-the-art Cu electrocatalysts from the literature, we show that different morphologies have similar intrinsic activities for CO2 reduction. Afterwards, we will discuss a tandem catalysis approach for improving upon these normalized CO2 reduction activities, which is enabled by utilizing bimetallic electrodes consisting of Au nanoparticles on polycrystalline Cu (Au/Cu). At low overpotentials, the Au/Cu electrocatalyst has a synergistic catalytic activity superior to that of either Cu or Au, indicating that tandem catalysis mechanisms can be utilized to increase the energy efficiency for alcohol production. By comparing Au/Cu to Cu, we highlight common potential-driven trends in the selectivity to oxygenated and multicarbon products, providing insights on how to develop new electrocatalysts that can guide selectivity to valuable chemicals and fuels.
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Buonsanti, Raffaella. „Developing the Chemistry of Colloidal Cu Nanocrystals to Advance the CO2 Electrochemical Reduction“. CHIMIA International Journal for Chemistry 75, Nr. 7 (25.08.2021): 598–604. http://dx.doi.org/10.2533/chimia.2021.598.
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The ability to tailor make materials with atomic scale precision is crucial for understanding the sensitivities of their performance parameters and for achieving the design specification corresponding to optimal device operation. Herein, this topic is discussed in the context of catalysis. The electrochemical CO2 reduction reaction (CO2 RR) holds the promise to close the carbon cycle by storing renewable energies in chemical feedstocks, yet it suffers from the lack of efficient and selective catalysts. This article highlights how colloidal chemistry can contribute to tackle this compelling issue by designing shape-controlled nanocatalysts. In particular, two case studies relative to copper nanocrystals are discussed.
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He, Liang-Nian, Xiao-Fang Liu, Xiao-Ya Li und Chang Qiao. „Transition-Metal-Free Catalysis for the Reductive Functionalization of CO2 with Amines“. Synlett 29, Nr. 05 (31.01.2018): 548–55. http://dx.doi.org/10.1055/s-0036-1591533.
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Reductive functionalization of CO2 with amines and a reductant, which combines both reduction of CO2 and C–N bond formation in one pot to produce versatile chemicals and energy-storage materials such as formamides, aminals, and methylamines that are usually derived from petroleum feedstock, would be appealing and promising. Herein, we give a brief review on recent developments in the titled CO2 chemistry by employing transition-metal-free catalysis, which can be catalogued as below according to the diversified energy content of the products, that is formamides, aminals, and methylamines being consistent with 2-, 4-, and 6-electron reduction of CO2, respectively. Notably, hierarchical reduction of CO2 with amines to afford at least two products, for example, formamides and methylamines, could be realized with the same catalyst through tuning the hydrosilane type, reaction temperature, or CO2 pressure. Finally, the opportunities and challenges of the reductive functionalization of CO2 with amines are also highlighted.1 Introduction2 2-Electron Reduction of CO2 to Formamide3 6-Electron Reduction of CO2 to Methylamine4 4-Electron Reduction of CO2 to Aminal5 Hierarchical Reduction of CO2 with Amines6 Conclusion
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Al-Omari, Abdulhadi, Zain Yamani und Ha Nguyen. „Electrocatalytic CO2 Reduction: From Homogeneous Catalysts to Heterogeneous-Based Reticular Chemistry“. Molecules 23, Nr. 11 (01.11.2018): 2835. http://dx.doi.org/10.3390/molecules23112835.
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CO2, emitted mainly from fossil fuel combustion, is one of the major greenhouse gases. CO2 could be converted into more valuable chemical feedstocks including CO, HCOOH, HCHO, CH3OH, or CH4. To reduce CO2, catalysts were designed and their unique characteristics were utilized based on types of reaction processes, including catalytic hydrogenation, complex metal hydrides, photocatalysis, biological reduction, and electrochemical reduction. Indeed, the electroreduction method has received much consideration lately due to the simple operation, as well as environmentally friendly procedures that need to be optimized by both of the catalysts and the electrochemical process. In the past few decades, we have witnessed an explosion in development in materials science—especially in regards to the porous crystalline materials based on the strong covalent bond of the organic linkers containing light elements (Covalent organic frameworks, COFs), as well as the hybrid materials that possess organic backbones and inorganic metal-oxo clusters (Metal-organic frameworks, MOFs). Owing to the large surface area and high active site density that belong to these tailorable structures, MOFs and COFs can be applied to many practical applications, such as gas storage and separation, drug release, sensing, and catalysis. Beyond those applications, which have been abundantly studied since the 1990s, CO2 reduction catalyzed by reticular and extended structures of MOFs or COFs has been more recently turned to the next step of state-of-the-art application. In this perspective, we highlight the achievement of homogeneous catalysts used for CO2 electrochemical conversion and contrast it with the advances in new porous catalyst-based reticular chemistry. We then discuss the role of new catalytic systems designed in light of reticular chemistry in the heterogeneous-catalyzed reduction of CO2.
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Selva Ochoa, Angela Gabriela, Faezeh Habibzadeh und Elod Lajos Gyenge. „Metal-Organic Framework-Based Electrodes for Efficient CO2 Electroreduction to Formate at High Current Densities (up to 1 A cm−2)“. ECS Meeting Abstracts MA2024-01, Nr. 56 (09.08.2024): 2977. http://dx.doi.org/10.1149/ma2024-01562977mtgabs.
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Achieving efficient CO2 electroreduction for production of valuable chemicals requires affordable, stable, and non-toxic catalysts. One of the most studied and promising products of CO2 reduction is formic acid/formate. The latter species is receiving increased attention as an energy vector [1] or energy storage media (e.g., in CO2 redox flow batteries [2]). At present, the practical application of CO2 reduction to formate still faces challenges due to the lack of electrocatalysts capable of operating at high current densities (> 200 mA cm−2) with low degradation over long-duration operation [3]. Traditional metallic catalysts like Bi, Sn, In or Pb when scaled in flow cells typically suffer from low faradaic efficiencies (< 70%) at current densities ≥ 200 mA cm-2, coupled with inadequate durability [4]. Metal-organic frameworks (MOFs) present promising and thus far largely unexplored attributes as electrocatalysts for CO2 reduction, including high atom utilization during catalysis due to their porous crystal structure and tunable pore size distribution [5,6]. However, they also face challenges related to high overpotentials and complex synthesis methods [7]. This study elucidates the efficacy of a Bi metal-organic framework (Bi-MOF) synthesized through a rapid and facile method. The Bi-MOF obtained by our proprietary novel method [8], exhibits exceptional catalytic performance. Notably, it demonstrates outstanding faradaic efficiencies towards formate (FEHCOO - = 95–100%) at current densities up to 1 A cm−2 in a gas diffusion electrode, at low catalyst loading (0.5 mg cm−2). Moreover, Bi-MOF displays extended stability, operating continuously for over 20 hours at an industrially relevant current density (200 mA cm−2) and without electrolyte (1.5 M KOH) replenishment. In a flow reactor with 10 cm2 electrode geometric area, a 100% FEHCOO - was obtained during 2-hour electrolysis at 100 mA cm−2 across a broad pH range (8–14). The electrochemical testing of the Bi-MOF was supplemented by surface and structural characterizations to correlate the activity with structural features. This analysis unveiled the role of the organic framework and the reason why Bi-MOF surpasses other Bi-based catalysts, including commercial Bi2O2CO3, Bi2O3, and metallic Bi, in selectivity (FE), cell potential, and durability. These findings hold promise for further scale-up of CO2 reduction to formate using the cost-effective and easily prepared Bi-MOF catalyst. [1] Bienen, F., Kopljar, D., Löwe, A., Aßmann, P., Stoll, M., Rößner, P., Wagner, N., Friedrich, A., & Klemm, E. (2019). Utilizing Formate as an Energy Carrier by Coupling CO2 Electrolysis with Fuel Cell Devices. Chemie Ingenieur Technik, 91(6), 872-882. [2] Hosseini-Benhangi, P., Gyenge, C., & Gyenge, E. (2021). The carbon dioxide redox flow battery: Bifunctional CO2 reduction/formate oxidation electrocatalysis on binary and ternary catalysts. Journal of Power Sources, 495, 229752. [3] Masel, R. I., Liu, Z., Yang, H., Kaczur, J. J., Carrillo, D., Ren, S., Salvatore, D., & Berlinguette, C. P. (2021). An industrial perspective on catalysts for low-temperature CO2 electrolysis. Nature Nanotechnology, 16(2), 118-128. [4] Zou, J., Liang, G., Lee, C., & Wallace, G. G. (2023). Progress and perspectives for electrochemical CO2 reduction to formate. Materials Today Energy, 38, 101433. [5] Mazari, S. A., Hossain, N., Basirun, W. J., Mubarak, N. M., Abro, R., Sabzoi, N., & Shah, A. (2021). An overview of catalytic conversion of CO2 into fuels and chemicals using metal organic frameworks. Process Safety and Environmental Protection, 149, 67-92. [6] Xie, W., Mulina, O. M., O., A., & He, L. (2023). Metal–Organic Frameworks for Electrocatalytic CO2 Reduction into Formic Acid. Catalysts, 13(7), 1109. [7] Köppen, M., Dhakshinamoorthy, A., Inge, A.K., Cheung, O., Ångström, J., Mayer, P. and Stock, N. (2018), Synthesis, Transformation, Catalysis, and Gas Sorption Investigations on the Bismuth Metal–Organic Framework CAU-17. Eur. J. Inorg. Chem., 2018: 3496-3503. [8] Selva-Ochoa, A.G., Habibzadeh F., Gyenge E.L. (2023). Manuscript in preparation. Department of Chemical & Biological Engineering, UBC.
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Roldan Cuenya, Beatriz. „(Invited) Dynamics in the Electrocatalytic Reduction of CO2 “. ECS Meeting Abstracts MA2023-01, Nr. 37 (28.08.2023): 2163. http://dx.doi.org/10.1149/ma2023-01372163mtgabs.
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Climate change concerns have spurred a growing interest in developing environmentally friendly technologies for energy generation, such as green H2 from water splitting. Moreover, the electrochemical reduction of CO2 (CO2RR) into value-added chemicals and fuels offers an additional possibility to store renewable energy into chemical bonds. It is therefore of particular interest to develop efficient, selective and durable electrocatalysts that can operate under mild reaction conditions. The latter however requires fundamental understanding of their structure and surface composition under reaction conditions. It should be kept in mind that even morphologically and chemically well-defined pre-catalysts will be susceptible to drastic modifications under operando conditions, especially when the reaction conditions themselves change periodically. This talk will illustrate how of a multi-technique in-situ/operando experimental approach is able provide in depth mechanistic insights into CO2RR1,2. A synergistic combination of LC-TEM, EC-AFM, NAP-XPS, XAS, XRD, GC/MS, and Raman Spectroscopy, coupled with machine learning-based data analysis, has been employed to investigate the time-dependent chemical and structural changes in mono and bimetallic CO2 electrocatalysts under reaction conditions. Some of the aspects that will be discussed here include: (i) the design of size- and shape-controlled catalytically active nanoparticle (NP) pre-catalysts (Cu2O cubes, ZnO@Cu2O cubic NPs), (ii) the understanding of the active state formation (e.g for well-defined Cu(100), Cu(111) surfaces) and the correlation between the dynamically evolving structure and composition of the electrocatalysts under operando reaction conditions and their activity and selectivity. Our studies are expected to open up new routes for the reutilization of CO2 through its direct conversion into industrially valuable chemicals and fuels such as ethylene and ethanol. References [1] J. Timoshenko, A. Bergmann, B. Roldan Cuenya et al., Nature Catalysis (2022), 5, 259–267. [2] M. Rüscher, A. Herzog, J. Timoshenko, H. Jeon, W. Frandsen, S. Kühl, B. Roldan Cuenya Catalysis Science & Technology (2022)12, 3028–3043. Climate change concerns have spurred a growing interest in developing environmentally friendly technologies for energy generation, such as green H2 from water splitting. Moreover, the electrochemical reduction of CO2 (CO2RR) into value-added chemicals and fuels offers an additional possibility to store renewable energy into chemical bonds. It is therefore of particular interest to develop efficient, selective and durable electrocatalysts that can operate under mild reaction conditions. The latter however requires fundamental understanding of their structure and surface composition under reaction conditions. It should be kept in mind that even morphologically and chemically well-defined pre-catalysts will be susceptible to drastic modifications under operando conditions, especially when the reaction conditions themselves change periodically. This talk will illustrate how of a multi-technique in-situ/operando experimental approach is able provide in depth mechanistic insights into CO2RR1,2. A synergistic combination of LC-TEM, EC-AFM, NAP-XPS, XAS, XRD, GC/MS, and Raman Spectroscopy, coupled with machine learning-based data analysis, has been employed to investigate the time-dependent chemical and structural changes in mono and bimetallic CO2 electrocatalysts under reaction conditions. Some of the aspects that will be discussed here include: (i) the design of size- and shape-controlled catalytically active nanoparticle (NP) pre-catalysts (Cu2O cubes, ZnO@Cu2O cubic NPs), (ii) the understanding of the active state formation (e.g for well-defined Cu(100), Cu(111) surfaces) and the correlation between the dynamically evolving structure and composition of the electrocatalysts under operando reaction conditions and their activity and selectivity. Our studies are expected to open up new routes for the reutilization of CO2 through its direct conversion into industrially valuable chemicals and fuels such as ethylene and ethanol. References [1] J. Timoshenko, A. Bergmann, B. Roldan Cuenya et al., Nature Catalysis (2022), 5, 259–267. [2] M. Rüscher, A. Herzog, J. Timoshenko, H. Jeon, W. Frandsen, S. Kühl, B. Roldan Cuenya Catalysis Science & Technology (2022)12, 3028–3043.
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Cobb, Samuel J., Vivek M. Badiani, Azim M. Dharani, Andreas Wagner, Sónia Zacarias, Ana Rita Oliveira, Inês A. C. Pereira und Erwin Reisner. „Fast CO2 hydration kinetics impair heterogeneous but improve enzymatic CO2 reduction catalysis“. Nature Chemistry 14, Nr. 4 (28.02.2022): 417–24. http://dx.doi.org/10.1038/s41557-021-00880-2.
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Khajonvittayakul, Chalempol, Vut Tongnan, Suksun Amornraksa, Navadol Laosiripojana, Matthew Hartley und Unalome Wetwatana Hartley. „CO2 Hydrogenation to Synthetic Natural Gas over Ni, Fe and Co–Based CeO2–Cr2O3“. Catalysts 11, Nr. 10 (26.09.2021): 1159. http://dx.doi.org/10.3390/catal11101159.
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CO2 methanation was studied over monometallic catalyst, i.e., Ni, Fe and Co; on CeO2-Cr2O3 support. The catalysts were prepared using one-pot hydrolysis of mixed metal nitrates and ammonium carbonate. Physicochemical properties of the pre- and post-exposure catalysts were characterized by X-Ray Powder Diffraction (XRD), Hydrogen Temperature Programmed Reduction (H2-TPR), and Field Emission Scanning Electron Microscope (FE-SEM). The screening of three dopants over CeO2-Cr2O3 for CO2 methanation was conducted in a milli-packed bed reactor. Ni-based catalyst was proven to be the most effective catalyst among all. Thus, a group of NiO/CeO2-Cr2O3 catalysts with Ni loading was investigated further. 40 % NiO/CeO2-Cr2O3 exhibited the highest CO2 conversion of 97.67% and CH4 selectivity of 100% at 290 °C. The catalytic stability of NiO/CeO2-Cr2O3 was tested towards the CO2 methanation reaction over 50 h of time-on-stream experiment, showing a good stability in term of catalytic activity.
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Kwak, Ja Hun, Libor Kovarik und János Szanyi. „Heterogeneous Catalysis on Atomically Dispersed Supported Metals: CO2 Reduction on Multifunctional Pd Catalysts“. ACS Catalysis 3, Nr. 9 (16.08.2013): 2094–100. http://dx.doi.org/10.1021/cs4001392.
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Fernández-Alvarez, Francisco J., Abdullah M. Aitani und Luis A. Oro. „Homogeneous catalytic reduction of CO2 with hydrosilanes“. Catal. Sci. Technol. 4, Nr. 3 (2014): 611–24. http://dx.doi.org/10.1039/c3cy00948c.
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Guo, Mengquan, Xiangxiang Li, Yuxin Huang, Linfa Li, Jixiao Li, Yiren Lu, Yanhong Xu und Lihong Zhang. „CO2-Induced Fibrous Zn Catalyst Promotes Electrochemical Reduction of CO2 to CO“. Catalysts 11, Nr. 4 (08.04.2021): 477. http://dx.doi.org/10.3390/catal11040477.
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The electrochemical reduction of CO2 is a promising strategy to achieve efficient conversion and utilization. In this paper, a series of Zn catalysts were prepared by electrodeposition in different atmospheric conditions (N2, CO2, H2, CO). A fibrous Zn catalyst (Zn-CO2) exhibits high electrochemical activity and stability. The Zn-CO2 catalyst shows 73.0% faradaic efficiency of CO at −1.2 V vs. RHE and the selectivity of CO almost did not change over 6 h in −1.2 V vs. RHE. The excellent selectivity and stability is attributed to the novel fibrous morphology, which increases the electrochemical active surface area. X-ray diffraction (XRD) results show that Zn-CO2 catalyst has a higher proportion of Zn (101) crystal planes, which is considered to be conducive to the production of CO. The search further demonstrates the importance of morphology control for the preparation of highly active and stable catalysts.
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Li, Xiangxiang, Shuling Chang, Yanting Wang und Lihong Zhang. „Silver-Carbonaceous Microsphere Precursor-Derived Nano-Coral Ag Catalyst for Electrochemical Carbon Dioxide Reduction“. Catalysts 12, Nr. 5 (23.04.2022): 479. http://dx.doi.org/10.3390/catal12050479.
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The selective and effective conversion of CO2 into available chemicals by electrochemical methods was applied as a promising way to mitigate the environment and energy crisis. Metal silver is regarded as an efficient electrocatalyst that can selectively convert CO2 into CO at room temperature. In this paper, a series of coral-like porous Ag (CD-Ag) catalysts were fabricated by calcining silver-carbonaceous microsphere (Ag/CM) precursors with different Ag content and the formation mechanism of CD-Ag catalysts was proposed involving the Ag precursor reduction and CM oxidation. In the selective electrocatalytic reduction of CO2 to CO, the catalyst 15 CD-Ag showed a stable current density at −6.3 mA/cm2 with a Faraday efficiency (FE) of ca. 90% for CO production over 5 h in −0.95 V vs. RHE. The excellent performance of the 15 CD-Ag catalysts is ascribed to the special surface chemical state and the particular nano-coral porous structure with uniformly distributed Ag particles and pore structure, which can enhance the electrochemical active surface areas (ECSA) and provide more active sites and porosity compared with other CD-Ag catalysts and even Ag foil.
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Rahmati, Farnood, Negar Sabouhanian, Jacek Lipkowski und Aicheng Chen. „Synthesis of 3D Porous Cu Nanostructures on Ag Thin Film Using Dynamic Hydrogen Bubble Template for Electrochemical Conversion of CO2 to Ethanol“. Nanomaterials 13, Nr. 4 (20.02.2023): 778. http://dx.doi.org/10.3390/nano13040778.
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Cu-based nanomaterials have been widely considered to be promising electrocatalysts for the direct conversion of CO2 to high-value hydrocarbons. However, poor selectivity and slow kinetics have hindered the use of Cu-based catalysts for large-scale industrial applications. In this work, we report on a tunable Cu-based synthesis strategy using a dynamic hydrogen bubble template (DHBT) coupled with a sputtered Ag thin film for the electrochemical reduction of CO2 to ethanol. Remarkably, the introduction of Ag into the base of the three-dimensional (3D) Cu nanostructure induced changes in the CO2 reduction reaction (CO2RR) pathway, which resulted in the generation of ethanol with high Faradaic Efficiency (FE). This observation was further investigated through Tafel and electrochemical impedance spectroscopic analyses. The rational design of the electrocatalyst was shown to promote the spillover of formed CO intermediates from the Ag sites to the 3D porous Cu nanostructure for further reduction to C2 products. Finally, challenges toward the development of multi-metallic electrocatalysts for the direct catalysis of CO2 to hydrocarbons were elucidated, and future perspectives were highlighted.
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Reisner, Erwin. „(Keynote) Reversible CO2 Reduction Electrocatalysis in Solar-Powered Chemistry“. ECS Meeting Abstracts MA2023-02, Nr. 52 (22.12.2023): 2517. http://dx.doi.org/10.1149/ma2023-02522517mtgabs.
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Semi-artificial photosynthesis interfaces biological catalysts with synthetic materials such as electrodes or light absorbers to overcome limitations in natural and artificial photosynthesis. The benefit of using biocatalysts in electrocatalytic CO2 reduction is their electrochemical reversibility that enables their operation at very low overpotentials with high selectivity. This presentation will summarise my research group’s progress in integrating the CO2 reducing enzyme formate dehydrogenase into bespoke hierarchical 3D electrode scaffolds and the exploitation in solar-powered catalysis. I will present the electrochemical features and characterisation of the biocatalyst-material interface and provide my team's understanding of the electrochemical properties of the immobilised formate dehydrogenase. This insight allows the wiring of the biocatalyst into electrocatalytic schemes, photoelectrochemical devices and photocatalytic systems for unique CO2 utilisation reactions. The fundamental insights gained by integrating isolated formate dehydrogenase in electrodes will be presented and the case be made that this enzyme allows opening a solar-to-chemical conversion space that is currently not accessible with purly synthetic or biological catalysts (see uploaded Image as example). Recent publications: (1) Lam et al., Angew. Chem. Int. Ed., 2023, in print. (2) Bhattacharjee et al., Nat. Synth., 2023, 2, 182-92. (3) Badiani et al., J. Am. Chem. Soc., 2022, 144, 14207-16. (4) Cobb et al., Nat. Chem., 2022, 14, 417-24. (5) Edwardes Moore et al., Proc. Natl. Acad. Sci. USA, 2022, 119, e2114097199. (6) Anton Garcia et al., Nat. Synth. 2022, 1, 77-86. Reviews: (1) Fang et al., Chem. Soc. Rev., 2020, 49, 4926–52. (2) Zhang & Reisner, Nature Rev. Chem., 2020, 4, 6–21. (3) Kornienko et al., Acc. Chem. Res., 2019, 52, 1439–44. (4) Kornienko et al., Nature Nanotech., 2018, 13, 890–99
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Li, Qianwen, Mei Li, Shengbo Zhang, Xiao Liu, Xinli Zhu, Qingfeng Ge und Hua Wang. „Tuning Sn-Cu Catalysis for Electrochemical Reduction of CO2 on Partially Reduced Oxides SnOx-CuOx-Modified Cu Electrodes“. Catalysts 9, Nr. 5 (22.05.2019): 476. http://dx.doi.org/10.3390/catal9050476.
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Copper-based bimetallic catalysts have been recently showing promising performance for the selective electrochemical reduction of CO2. In this work, we successfully fabricated the partially reduced oxides SnOx, CuOxmodified Cu foam electrode (A-Cu/SnO2) through an electrodeposition-annealing-electroreduction approach. Notably, in comparison with the control electrode (Cu/SnO2) without undergoing annealing step, A-Cu/SnO2 exhibits a significant enhancement in terms of CO2 reduction activity and CO selectivity. By investigating the effect of the amount of the electrodeposited SnO2, it is found that A-Cu/SnO2 electrodes present the characteristic Sn-Cu synergistic catalysis with a feature of dominant CO formation (CO faradaic efficiency, 70~75%), the least HCOOH formation (HCOOH faradaic efficiency, <5%) and the remarkable inhibition of hydrogen evolution reaction. In contrast, Cu/SnO2 electrodes exhibit a SnO2 coverage-dependent catalysis—a shift from CO selectivity to HCOOH selectivity with the increasing deposited SnO2 on Cu foam. The different catalytic performance between Cu/SnO2 and A-Cu/SnO2 might be attributed to the different content of Cu atoms in SnO2 layer, which may affect the density of Cu-Sn interface on the surface. Our work provides a facile annealing-electroreduction strategy to modify the surface composition for understanding the metal effect towards CO2 reduction activity and selectivity for bimetallic Cu-based electrocatalysts.
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Cai, Fan, Dunfeng Gao, Hu Zhou, Guoxiong Wang, Ting He, Huimin Gong, Shu Miao, Fan Yang, Jianguo Wang und Xinhe Bao. „Electrochemical promotion of catalysis over Pd nanoparticles for CO2 reduction“. Chemical Science 8, Nr. 4 (2017): 2569–73. http://dx.doi.org/10.1039/c6sc04966d.
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Electrochemical promotion of catalysis was observed over Pd nanoparticles with a significant rate enhancement ratio (ρ) for catalyzing CO2 reduction to produce formate in 1 M KHCO3 solution at ambient temperature.
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Zhang, Hanguang, John Weiss, Luigi Osmieri und Piotr Zelenay. „M-N-C-Supported Catalysts for Carbon Dioxide Reduction Reaction“. ECS Meeting Abstracts MA2023-01, Nr. 26 (28.08.2023): 1703. http://dx.doi.org/10.1149/ma2023-01261703mtgabs.
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Electrochemical carbon dioxide reduction (CO2RR) is a promising approach to converting CO2 into value-added chemicals using renewable electricity and to ultimately reducing the dependence on fossil resources. However, achieving sufficient activity and selectivity in economically viable CO2 electrolyzers presents a great challenge for CO2RR catalysts.1 Carbons are an important and particularly suitable component of a majority of CO2RR catalysts due to their excellent electronic conductivity, relatively easily achievable high porosity and hierarchical pore structure.2, 3 Thanks to these benefits, the metal-nitrogen-carbon (M-N-C) materials, containing at least 95 at% of carbon, have attracted special interest due to their promising selectivity for CO in CO2RR.4 In particular, the Ni-N-C support has been used to improve selectivity of Cu-based CO2RR catalysts for ethylene, attributed to the enhancement of CO generation during CO2RR.5 However, a comprehensive study is still needed to understand the effect of composition and morphology of M-N-C materials as supports for CO2RR. In this presentation, we will summarize the results of our recent study that has focused on the effect of composition (e.g., different metal centers) and morphology (e.g., porosity) of M-N-C supports on the activity and selectivity of metal (e.g., Cu) nanoparticles. We will specifically concentrate on possible advantages/disadvantages of using M-N-C materials as performance enhancing supports rather than autonomous CO2RR electrocatalysts. Acknowledgement Research presented in this work was supported by the Laboratory Directed Research and Development program of Los Alamos National Laboratory under project number 20230065DR. References (1) Masel, R. I.; Liu, Z.; Yang, H.; Kaczur, J. J.; Carrillo, D.; Ren, S.; Salvatore, D.; Berlinguette, C. P. An industrial perspective on catalysts for low-temperature CO2 electrolysis. Nature Nanotechnology 2021, 16 (2), 118-128. (2) Jhong, H.-R. M.; Tornow, C. E.; Kim, C.; Verma, S.; Oberst, J. L.; Anderson, P. S.; Gewirth, A. A.; Fujigaya, T.; Nakashima, N.; Kenis, P. J. A. Gold Nanoparticles on Polymer-Wrapped Carbon Nanotubes: An Efficient and Selective Catalyst for the Electroreduction of CO2. ChemPhysChem 2017, 18 (22), 3274-3279. (3) Baturina, O. A.; Lu, Q.; Padilla, M. A.; Xin, L.; Li, W.; Serov, A.; Artyushkova, K.; Atanassov, P.; Xu, F.; Epshteyn, A.; et al. CO2 Electroreduction to Hydrocarbons on Carbon-Supported Cu Nanoparticles. ACS Catalysis 2014, 4 (10), 3682-3695. (4) Liang, S.; Huang, L.; Gao, Y.; Wang, Q.; Liu, B. Electrochemical Reduction of CO2 to CO over Transition Metal/N-Doped Carbon Catalysts: The Active Sites and Reaction Mechanism. Advanced Science 2021, 8 (24), 2102886. (5) Wang, X.; de Araújo, J. F.; Ju, W.; Bagger, A.; Schmies, H.; Kühl, S.; Rossmeisl, J.; Strasser, P. Mechanistic reaction pathways of enhanced ethylene yields during electroreduction of CO2–CO co-feeds on Cu and Cu-tandem electrocatalysts. Nature Nanotechnology 2019, 14 (11), 1063-1070.
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Tawil, Sumana, Hathaichanok Seelajaroen, Amorn Petsom, Niyazi Serdar Sariciftci und Patchanita Thamyongkit. „Clam-shaped cyclam-functionalized porphyrin for electrochemical reduction of carbon dioxide“. Journal of Porphyrins and Phthalocyanines 23, Nr. 04n05 (April 2019): 453–61. http://dx.doi.org/10.1142/s1088424619500548.
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A clam-shaped molecule comprising a Zn(II)-porphyrin and a Zn(II)-cyclam is synthesized and characterized. Its electrochemical behavior and catalytic activity for homogeneous electrochemical reduction of carbon dioxide (CO[Formula: see text] are investigated by cyclic voltammetry and compared with those of Zn(II)-meso-tetraphenylporphyrin and Zn(II)-cyclam. Under N2-saturated conditions, cyclic voltammetry of the featured complex has characteristics of its two constituents, but under CO2-saturated conditions, the target compound exhibits significant current enhancement. Iterative reduction under electrochemical conditions indicated the target compound has improved stability relative to Zn(II)-cyclam. Controlled potential electrolysis demonstrates that, without addition of water, methane (CH[Formula: see text] is the only detectable product with 1% Faradaic efficiency (FE). The formation of CH4 is not observed under the catalysis of the Zn(II)-porphyrin benchmark compound, indicating that the CO2-capturing function of the Zn(II)-cyclam unit contributes to the catalysis. Upon addition of 3% v/v water, the electrochemical reduction of CO2 in the presence of the target compound gives carbon monoxide (CO) with 28% FE. Dominance of CO formation under these conditions suggests enhancement of proton-coupled reduction. Integrated action of these Zn(II)-porphyrin and Zn(II)-cyclam units offers a notable example of a molecular catalytic system where the cyclam ring captures and brings CO2 into the proximity of the porphyrin catalysis center.
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Manan, Wan Nabilah, Wan Nor Roslam Wan Isahak und Zahira Yaakob. „CeO2-Based Heterogeneous Catalysts in Dry Reforming Methane and Steam Reforming Methane: A Short Review“. Catalysts 12, Nr. 5 (19.04.2022): 452. http://dx.doi.org/10.3390/catal12050452.
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Transitioning to lower carbon energy and environment sustainability requires a reduction in greenhouse gases such as carbon dioxide (CO2) and methane (CH4) that contribute to global warming. One of the most actively studied rare earth metal catalysts is cerium oxide (CeO2) which produces remarkable improvements in catalysts in dry reforming methane. This paper reviews the management of CO2 emissions and the recent advent and trends in bimetallic catalyst development utilizing CeO2 in dry reforming methane (DRM) and steam reforming methane (SRM) from 2015 to 2021 as a way to reduce greenhouse gas emissions. This paper focus on the identification of key trends in catalyst preparation using CeO2 and the effectiveness of the catalysts formulated.
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Cui, Yan, Pengxiang Ge, Mindong Chen und Leilei Xu. „Research Progress in Semiconductor Materials with Application in the Photocatalytic Reduction of CO2“. Catalysts 12, Nr. 4 (24.03.2022): 372. http://dx.doi.org/10.3390/catal12040372.
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The large-scale burning of non-renewable fossil fuels leads to the gradual increase of the CO2 concentration in the atmosphere, which is associated with negative impacts on the environment. The consequent need to reduce the emission of CO2 resulting from fossil fuel combustion has led to a serious energy crisis. Research reports indicate that the photocatalytic reduction of CO2 is one of the most effective methods to control CO2 pollution. Therefore, the development of novel high-efficiency semiconductor materials has become an important research field. Semiconductor materials need to have a structure with abundant catalytic sites, among other conditions, which is of great significance for the practical application of highly active catalysts for CO2 reduction. This review systematically describes various types of semiconductor materials, as well as adjustments to the physical, chemical and electronic characteristics of semiconductor catalysts to improve the performance of photocatalytic reduction of CO2. The principle of photocatalytic CO2 reduction is also provided in this review. The reaction types and conditions of photocatalytic CO2 reduction are further discussed. We believe that this review will provide a good basis and reference point for future design and development in this field.
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Tian, Pengfei, Bo Zhang, Jiacheng Chen, Jing Zhang, Libei Huang, Ruquan Ye, Bo Bao und Minghui Zhu. „Curvature-induced electronic tuning of molecular catalysts for CO2 reduction“. Catalysis Science & Technology 11, Nr. 7 (2021): 2491–96. http://dx.doi.org/10.1039/d0cy01589j.
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Wang, Luhui, Junang Hu, Hui Liu, Qinhong Wei, Dandan Gong, Liuye Mo, Hengcong Tao und Chengyang Zhang. „Three-Dimensional Mesoporous Ni-CeO2 Catalysts with Ni Embedded in the Pore Walls for CO2 Methanation“. Catalysts 10, Nr. 5 (08.05.2020): 523. http://dx.doi.org/10.3390/catal10050523.
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Mesoporous Ni-based catalysts with Ni confined in nanochannels are widely used in CO2 methanation. However, when Ni loadings are high, the nanochannels are easily blocked by nickel particles, which reduces the catalytic performance. In this work, three-dimensional mesoporous Ni-CeO2-CSC catalysts with high Ni loadings (20−80 wt %) were prepared using a colloidal solution combustion method, and characterized by nitrogen adsorption–desorption, X-ray diffraction (XRD), transmission electron microscopy (TEM) and H2 temperature programmed reduction (H2-TPR). Among the catalysts with different Ni loadings, the 50% Ni-CeO2-CSC with 50 wt % Ni loading exhibited the best catalytic performance in CO2 methanation. Furthermore, the 50% Ni-CeO2-CSC catalyst was stable for 50 h at 300° and 350 °C in CO2 methanation. The characterization results illustrate that the 50% Ni-CeO2-CSC catalyst has Ni particles smaller than 5 nm embedded in the pore walls, and the Ni particles interact with CeO2. On the contrary, the 50% Ni-CeO2-CP catalyst, prepared using the traditional coprecipitation method, is less active and selective for CO2 methanation due to the larger size of the Ni and CeO2 particles. The special three-dimensional mesoporous embedded structure in the 50% Ni-CeO2-CSC can provide more metal–oxide interface and stabilize small Ni particles in pore walls, which makes the catalyst more active and stable in CO2 methanation.
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Dharmasaroja, Nichthima, Tanakorn Ratana, Sabaithip Tungkamani, Thana Sornchamni, David S. A. Simakov und Monrudee Phongaksorn. „The Effects of CeO2 and Co Doping on the Properties and the Performance of the Ni/Al2O3-MgO Catalyst for the Combined Steam and CO2 Reforming of Methane Using Ultra-Low Steam to Carbon Ratio“. Catalysts 10, Nr. 12 (11.12.2020): 1450. http://dx.doi.org/10.3390/catal10121450.
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In this paper, the 10 wt% Ni/Al2O3-MgO (10Ni/MA), 5 wt% Ni-5 wt% Ce/Al2O3-MgO (5Ni5Ce/MA), and 5 wt% Ni-5 wt% Co/Al2O3-MgO (5Ni5Co/MA) catalysts were prepared by an impregnation method. The effects of CeO2 and Co doping on the physicochemical properties of the Ni/Al2O3-MgO catalyst were comprehensively studied by N2 adsorption-desorption, X-ray diffraction (XRD), transmission electron microscopy (TEM), H2 temperature programmed reduction (H2-TPR), CO2 temperature programmed reduction (CO2-TPD), and thermogravimetric analysis (TGA). The effects on catalytic performance for the combined steam and CO2 reforming of methane with the low steam-to-carbon ratio (S/C ratio) were evaluated at 620 °C under atmospheric pressure. The appearance of CeO2 and Co enhanced the oxygen species at the surface that decreased the coke deposits from 17% for the Ni/MA catalyst to 11–12% for the 5Ni5Ce/MA and 5Ni5Co/MA catalysts. The oxygen vacancies in the 5Ni5Ce/MA catalyst promoted water activation and dissociation, producing surface oxygen with a relatively high H2/CO ratio (1.6). With the relatively low H2/CO ratio (1.3), the oxygen species at the surface was enhanced by CO2 activation-dissociation via the redox potential in the 5Ni5Co/MA catalyst. The improvement of H2O and CO2 dissociative adsorption allowed the 5Ni5Ce/MA and 5Ni5Co/MA catalysts to resist the carbon formation, requiring only a low amount of steam to be added.
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Hong, Xiaolei, Haiyan Zhu, Dianchen Du, Quanshen Zhang und Yawei Li. „Research Progress of Copper-Based Bimetallic Electrocatalytic Reduction of CO2“. Catalysts 13, Nr. 2 (09.02.2023): 376. http://dx.doi.org/10.3390/catal13020376.
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Fossil fuels are still the main source of energy in today’s society, so emissions of CO2 are inevitable, but when the CO2 level in the atmosphere is too high, many environmental problems will arise, such as the greenhouse effect, among others. Electrocatalytic reduction of CO2 is one of the most important methods that one can use to reduce the amount of CO2 in the atmosphere. This paper reviews bimetallic catalysts prepared on the basis of copper materials, such as Ag, Au, Zn and Ni. The effects of different ratios of metal atoms in the bimetallic catalysts on the selectivity of CO2RR were investigated and the effects of bimetallic catalysts on the CO2RR of different ligands were also analysed. Finally, this paper points out that the real reaction of CO2RR still needs to be studied and analysed, and the effect of the specific reaction environment on selectivity has not been thoroughly studied. This article also describes some of the problems encountered so far.
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Leung, Chi-Fai, und Pui-Yu Ho. „Molecular Catalysis for Utilizing CO2 in Fuel Electro-Generation and in Chemical Feedstock“. Catalysts 9, Nr. 9 (10.09.2019): 760. http://dx.doi.org/10.3390/catal9090760.
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Processes for the conversion of CO2 to valuable chemicals are highly desired as a result of the increasing CO2 levels in the atmosphere and the subsequent elevating global temperature. However, CO2 is thermodynamically and kinetically inert to transformation and, therefore, many efforts were made in the last few decades. Reformation/hydrogenation of CO2 is widely used as a means to access valuable products such as acetic acids, CH4, CH3OH, and CO. The electrochemical reduction of CO2 using hetero- and homogeneous catalysts recently attracted much attention. In particular, molecular CO2 reduction catalysts were widely studied using transition-metal complexes modified with various ligands to understand the relationship between various catalytic properties and the coordination spheres above the metal centers. Concurrently, the coupling of CO2 with various electrophiles under homogeneous conditions is also considered an important approach for recycling CO2 as a renewable C-1 substrate in the chemical industry. This review summarizes some recent advances in the conversion of CO2 into valuable chemicals with particular focus on the metal-catalyzed reductive conversion and functionalization of CO2.
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Liu, Di-Jia. „(Invited) Understanding the Electrocatalytic Mechanisms of Oxygen and Carbon Dioxide Reduction Reactions“. ECS Meeting Abstracts MA2022-01, Nr. 35 (07.07.2022): 1468. http://dx.doi.org/10.1149/ma2022-01351468mtgabs.
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Oxygen reduction reaction (ORR) is one of the most important reactions in the field of electrocatalysis today. ORR represents a key cathodic reaction in hydrogen fuel cell, which typically needs to be promoted by the platinum group metals (PGMs), particularly Pt. The high cost of Pt adds significant barrier to the widespread implementation of the fuel cell technology. During the last two decades, substantially amount of effort has been invested in searching for low-cost replacements, or PGM-free catalysts for ORR. Although significant progress has been made, such catalysts still face major challenge in durability. By adding small amount of Pt over PGM-free catalytic substrate, we have found that both activity and stability will be significantly improved through synergistic interaction. [1] To better define synergistic effect in ORR catalysis, however, requires a carefully designed experiment that can separates multiple factors during the catalyst synthesis that can potentially influence the overall activity. In this report, we will discuss our recent study in understanding of the ORR catalysis synergy between Pt/PGM-free components in rationally designed catalyst systems. Another fast developing area of electrocatalysis is CO2 reduction reaction (CO2RR), which promises to electrochemically convert CO2 to fuels and chemicals using renewable electricity. While CO2RR via 2-electron transfer, such as the conversion to CO or formate, has been proven high selective with fast kinetics, conversions to C2+ chemicals require significantly stronger binding between the catalytic site and CO2 to complete multiple electron transfers (8 to 16) and C-C bond coupling steps, therefore are more challenging. More recently, we develop a new amalgamated lithium metal (ALM) synthesis method to preparing highly selective and active CO2RR catalyst for C2+ chemicals such as ethanol production. [2] In this presentation, we will discuss the hypothesis driven CO2RR catalyst design, combined with the mechanistic study for preparing effective catalysts. We will also share some critical insight on CO2RR mechanism through advanced structural characterization and computational modelling. Acknowledgement: This work is supported by U. S. Department of Energy, Hydrogen and Fuel Cell Technologies Office through Office of Energy Efficiency and Renewable Energy and by Office of Science, U.S. Department of Energy under Contract DE-AC02-06CH11357. [1] L. Chong, J. Wen, J. Kubal, F. G. Sen, J. Zou, J. Greeley, M. Chan, H. Barkholtz, W. Ding, and D.-J. Liu, “Ultralow-loading Platinum-Cobalt Fuel Cell Catalysts Derived from Imidazolate Frameworks,” Science (2018) 362, 1276 [2] “Highly selective electrocatalytic CO2 reduction to ethanol by metallic clusters dynamically formed from atomically dispersed copper” Haiping Xu, Dominic Rebollar, Haiying He, Lina Chong, Yuzi Liu, Cong Liu, Cheng-Jun Sun, Tao Li, John V. Muntean, Randall E. Winans, Di-Jia Liu and Tao Xu, (2020) Nature Energy, 5, 623–632
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Cai, Fan, Dunfeng Gao, Hu Zhou, Guoxiong Wang, Ting He, Huimin Gong, Shu Miao, Fan Yang, Jianguo Wang und Xinhe Bao. „Correction: Electrochemical promotion of catalysis over Pd nanoparticles for CO2 reduction“. Chemical Science 8, Nr. 4 (2017): 3277. http://dx.doi.org/10.1039/c7sc90011b.
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Chen, Pengfei, Yiao Huang, Zuhao Shi, Xingzhu Chen und Neng Li. „Improving the Catalytic CO2 Reduction on Cs2AgBiBr6 by Halide Defect Engineering: A DFT Study“. Materials 14, Nr. 10 (11.05.2021): 2469. http://dx.doi.org/10.3390/ma14102469.
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Pb-free double halide perovskites have drawn immense attention in the potential photocatalytic application, due to the regulatable bandgap energy and nontoxicity. Herein, we first present a study for CO2 conversion on Pb-free halide perovskite Cs2AgBiBr6 under state-of-the-art first-principles calculation with dispersion correction. Compared with the previous CsPbBr3, the cell parameter of Cs2AgBiBr6 underwent only a small decrease of 3.69%. By investigating the adsorption of CO, CO2, NO, NO2, and catalytic reduction of CO2, we found Cs2AgBiBr6 exhibits modest adsorption ability and unsatisfied potential determining step energy of 2.68 eV in catalysis. We adopted defect engineering (Cl doping, I doping and Br-vacancy) to regulate the adsorption and CO2 reduction behavior. It is found that CO2 molecule can be chemically and preferably adsorbed on Br-vacancy doped Cs2AgBiBr6 with a negative adsorption energy of −1.16 eV. Studying the CO2 reduction paths on pure and defect modified Cs2AgBiBr6, Br-vacancy is proved to play a critical role in decreasing the potential determining step energy to 1.25 eV. Finally, we probe into the electronic properties and demonstrate Br-vacancy will not obviously promote the process of catalysis deactivation, as there is no formation of deep-level electronic states acting as carrier recombination center. Our findings reveal the process of gas adsorption and CO2 reduction on novel Pb-free Cs2AgBiBr6, and propose a potential strategy to improve the efficiency of catalytic CO2 conversion towards practical implementation.
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Wang, Nannan, Wenbin Jiang, Jing Yang, Haisong Feng, Youbin Zheng, Sheng Wang, Bofan Li et al. „Contact-electro-catalytic CO2 reduction from ambient air“. Nature Communications 15, Nr. 1 (13.07.2024). http://dx.doi.org/10.1038/s41467-024-50118-1.
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AbstractTraditional catalytic techniques often encounter obstacles in the search for sustainable solutions for converting CO2 into value-added products because of their high energy consumption and expensive catalysts. Here, we introduce a contact-electro-catalysis approach for CO2 reduction reaction, achieving a CO Faradaic efficiency of 96.24%. The contact-electro-catalysis is driven by a triboelectric nanogenerator consisting of electrospun polyvinylidene fluoride loaded with single Cu atoms-anchored polymeric carbon nitride (Cu-PCN) catalysts and quaternized cellulose nanofibers (CNF). Mechanistic investigation reveals that the single Cu atoms on Cu-PCN can effectively enrich electrons during contact electrification, facilitating electron transfer upon their contact with CO2 adsorbed on quaternized CNF. Furthermore, the strong adsorption of CO2 on quaternized CNF allows efficient CO2 capture at low concentrations, thus enabling the CO2 reduction reaction in the ambient air. Compared to the state-of-the-art air-based CO2 reduction technologies, contact-electro-catalysis achieves a superior CO yield of 33 μmol g−1 h−1. This technique provides a solution for reducing airborne CO2 emissions while advancing chemical sustainability strategy.
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Yun, Ruirui, Beibei Zhang, Ruiming Xu, Shichang Song, Junjie Mao und Zhaoxu Wang. „Atomically Dispersed Copper Catalysts for Highly Selective CO2 Reduction“. Inorganic Chemistry Frontiers, 2022. http://dx.doi.org/10.1039/d2qi02288e.
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Support substrates play an important and magical role in the catalysis process. Herein, atomically dispersed CuN3 catalysts supported by two different types of zirconia (defined as CuN3/NC/T-ZrO2 and CuN3/NC/M-ZrO2) have...
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Wang, Hongming, Liming Hong, Xian Liu, Baozhu Chi und Guomin Xia. „Diatomic Molecule Catalysts toward Synergistic Electrocatalytic Carbon Dioxide Reduction“. Journal of Materials Chemistry A, 2023. http://dx.doi.org/10.1039/d2ta09831h.
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Synergistic catalysis with diatomic catalysts is an effective means to boost carbon dioxide (CO2) electroreduction efficiency and product selectivity; studies in this field also contribute to an atomic-level understanding of...