Dissertations / Theses on the topic 'Electrocatalytic CO2 reduction'
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Xue, Congcong. "Electrocatalytic and Photocatalytic CO2 Reduction by Ru-Re Bimetallic Complexes." The Ohio State University, 2016. http://rave.ohiolink.edu/etdc/view?acc_num=osu1462205030.
Full textLi, Xiang. "Investigation of Interfacial Properties under Electrocatalytic Reduction Conditions:." Thesis, Boston College, 2021. http://hdl.handle.net/2345/bc-ir:109096.
Full textHeterogeneous electrocatalytic reduction is an environmentally friendly method for the conversion of abundant feedstock molecules into valuable products. Examples include the reduction of carbon dioxide to hydrocarbons and the reduction of nitrate to ammonia. Heterogeneous electrocatalysis occurs at the interface between an electrode and an electrolyte. Interfacial properties, such as surface morphology, interfacial electric field, interfacial water structure, and local pH, can substantially influence the activity and selectivity of electrocatalytic reduction processes. However, a comprehensive, molecular-level understanding of how these interfacial properties control electrocatalysis is still largely lacking to date. To develop such an understanding, it is essential to probe the properties of the electrocatalytic interface under operating conditions. This great experimental challenge is further compounded by the fact that the interface often undergoes dynamic changes during catalysis. In this thesis, we took a multimodal approach to characterize the aqueous electrolyte/copper interface during CO2/CO reduction and hydrogen evolution. Copper is the only pure metal that promotes the reduction of CO2/CO to hydrocarbons at significant reaction rates. The hydrogen evolution reaction is the main competing reaction in aqueous electrolytes. It is therefore essential to understand how these reactions are controlled by the properties of the interface. In the first part of this thesis, we employed in-situ surface-enhanced infrared absorption spectroscopy (SEIRAS) and surface-enhanced Raman spectroscopy (SERS) to investigate dynamic changes of the copper electrode surface. We found that the polycrystalline copper electrode surface undergoes a reconstruction process upon adsorption of CO. The formation of nanoscale metal clusters on the electrode manifests itself by the appearance of a new CO stretch band, which arises from a CO sub-population bound to undercoordinated copper atoms. The formation of these clusters is reversible, that is, they disappear upon desorption of CO. This work demonstratesthat a reaction intermediate such as CO can induce dynamic and reversible changes in the surface morphology of a heterogeneous catalyst. Because the changes are reversible, they would escape ex situ measurements. Our findings highlight the need for probing catalytic surfaces under operating conditions. In the second part of this thesis, we focused on how the electrolyte influences electrocatalysis at the aqueous electrolyte/copper electrode interface. Specifically, we explored the mechanisms by which cations of the supporting electrolyte affect the reduction of CO and the hydrogen evolution reaction on copper. With differential electrochemical mass spectrometry (DEMS), we determined to what extent the reduction of CO to ethylene is affected by the identity of the cations of the supporting electrolyte. Ethylene is produced in the presence of methyl4N+ and ethyl4N+ cations, whereas this product is not synthesized in propyl4N+- and butyl4N+-containing electrolytes. With SEIRAS, we found that an intermolecular interaction between surface-adsorbed CO and interfacial water is disrupted in the presence of the two larger cations. This observation suggests that this interaction promotes the hydrogenation of surface-bound CO to ethylene. This work illustrates that weak intermolecular interactions can substantially influence electrocatalytic processes. In a related study, we examined the effect of alkali metal cations of the supporting electrolyte on the hydrogen evolution reaction. We found that, in alkaline conditions, changing the cation from Na+ to Cs+ has no measurable effect on the HER. Because it is well-established that Cs+ promotes the reduction of CO2/CO to hydrocarbons, the results illustrate the changing the alkali cation enables the selective promotion of this pathway under alkaline conditions. Further, we found that in 0.1 M solutions of NaOH and CsOH of the highest commercially available purity grades, trace impurities of iron deposit on the copper electrode during the hydrogen evolution reaction. Because iron is a better catalyst for the hyrogen evolution reaction than copper, the rate of the hydrogen evolution reaction is enhanced by up to a factor of 5. These findings demonstrate that trace impurities of this ubiquitous metal pose a great challenge for the development of selective catalytic processes for CO2/CO reduction. This thesis provides a critical study of how the interfacial properties change under the electrocatalytic reduction of CO2/CO and hydrogen evolution conditions. The properties of both Cu electrode and the electrolyte contribute to the control of the selectivity of these complex electrocatalytic processes
Thesis (PhD) — Boston College, 2021
Submitted to: Boston College. Graduate School of Arts and Sciences
Discipline: Chemistry
Hicks, Robert Paul. "Probing Electrocatalytic and Photocatalytic Processes with Structure-Specific Spectroscopies:." Thesis, Boston College, 2019. http://hdl.handle.net/2345/bc-ir:108657.
Full textStudying the adsorption and reaction kinetics of surface-bound chemical species, on different metal catalysts or electrodes, is of paramount importance in the development of inhomogeneous catalytic methodology. Our study of the oxidation of CO on platinum was accomplished by designing a thin layer flow cell in an external reflection configuration. A charge-injection circuit was successfully implemented which decreased the time required to charge the double layer in the electrochemical cell. We were able to obtain a signal via Stark shift spectrum, of the adsorbed CO, using the thin layer cell configuration. Additionally, electrochemical impedance spectroscopy was used as a diagnostic tool to assess the effect of electrode geometry, on the voltage response, in the thin layer cell. The coupling of visible light-driven photoexciation with transition metal catalytic plat- forms is emerging as a synthetic strategy to achieve unique reactivity that has previously been inaccessible. One such example is the iridium/nickel-dipyridyl system discovered recently. Characterizing the interactions between the iridium and nickel catalysts, under reaction conditions, is important to develop a better understanding of the system. In order to apply infrared spectroscopic measurement techniques, in-situ, we made modifications to the synthetic scheme by changing the solvent and by utilizing different iridium catalysts for the synthesis of the desired methyl 4-(benzoyloxy)benzoate product. Using our trans- mission infrared setup we effectively demonstrated in-situ product detection of the aryl- ester coupled product. Additionally, after constructing a transient infrared pump-probe setup, we collected preliminary results of the triplet state lifetime of the iridium dye. The surface morphology of copper has been shown to affect the electrochemical reduction of CO2. Using surface-enhanced Raman spectroscopies, the reversible formation of nanoscale metal clusters on a copper electrode was revealed at sufficiently cathodic potentials where we observed the appearance of a new band at 2080 cm-1 corresponding to C≡O adsorbed to undercoordinated copper defect sites. The formation of new undercoordinated sites additionally resulted in the surface enhancement of the Raman scattering which amplified the intensity of the other spectral bands
Thesis (MS) — Boston College, 2019
Submitted to: Boston College. Graduate School of Arts and Sciences
Discipline: Chemistry
Berro, Patrick. "Exploring Photocatalytic and Electrocatalytic Reduction of CO2 with Re(I) and Zn(II) Complexes and Attempts to Employ a Novel Carbene Ligand to this Endeavor." Thesis, Université d'Ottawa / University of Ottawa, 2021. http://hdl.handle.net/10393/41625.
Full textMigliaccio, Luca. "Bimetallic catalysts for CO2 electroreduction." Master's thesis, Alma Mater Studiorum - Università di Bologna, 2017. http://amslaurea.unibo.it/14470/.
Full textHernández, Ibáñez Naiara. "Exploration of novel materials in (bio)electrocatalysis: sensing in complex media and biocathodes for the CO2 reduction." Doctoral thesis, Universidad de Alicante, 2018. http://hdl.handle.net/10045/88207.
Full textKour, Gurpreet. "First principles investigations on transition metal based electrocatalysts for efficient clean energy conversion." Thesis, Queensland University of Technology, 2022. https://eprints.qut.edu.au/232798/1/Gurpreet_Kour_Thesis.pdf.
Full textZhang, Ting. "I Doctorate Program in Materials Science PhD Thesis Zn-Based Metal-Organic Frameworks Derived Materials for High-Efficient Carbon Dioxide Electrochemical Reduction." Doctoral thesis, Universitat Autònoma de Barcelona, 2021. http://hdl.handle.net/10803/673731.
Full textLa combustión excesiva de combustibles fósiles da como resultado la emisión de dióxido de carbono (CO2), que desencadenó crecientes problemas ambientales, como el calentamiento global, el aumento del nivel del mar, el clima extremo y la extinción de especies. Por lo tanto, las tecnologías para la conversión de CO2 en otros productos de valor jugaron un papel vital para eliminar la concentración de CO2 en la atmósfera. En ese sentido, la conversión electroquímica de CO2 alimentado por energía renovable en productos químicos útiles se considera una solución elegante para lograr el ciclo del carbono. Sin embargo, debido a la interioridad de las moléculas de CO2 y la reacción competitiva de evolución de hidrógeno (HER), los principales desafíos en el campo CO2 RR son el alto requerimiento de sobrepotencial que representa la termodinámica desfavorable y la baja eficiencia faradaica (FE) para los productos objetivo. Por lo tanto, la búsqueda de un electrocatalizador económico y de alta eficiencia es sensato y necesario para aplicaciones prácticas. En las últimas décadas, las estructuras organometálicas (MOF) absorbieron las enormes consideraciones en el campo de la electrocatálisis debido a su gran área de superficie específica, rica estructura de poros y sitios activos uniformemente dispersos. Aunque con grandes potenciales en electrocatálisis, la mayoría de los materiales MOF todavía sufren de actividad insuficiente, baja conductividad y poca estabilidad, lo que dificultaría sus aplicaciones prácticas. Especialmente, en el campo de CO2 RR, se deben considerar muchos parámetros importantes, incluida la alta eficiencia faradaica (FE), bajo sobrepotencial, gran densidad de corriente y estabilidad robusta, etc. Por lo tanto, el diseño racional de MOF para cumplir con los requisitos anteriores tanto como sea posible es crucial para explotar sus futuras aplicaciones de CO2 RR. Por lo tanto, en esta disertación, hicimos muchos esfuerzos para desarrollar catalizadores basados en MOFs / derivados de MOF con eficiencia, actividad y estabilidad superiores para aumentar el rendimiento de CO2 RR. Esta disertación se divide en 5 capítulos: El capítulo 1 es la información sobre los conceptos fundamentales sobre la CO2 RR electroquímico, que incluye la celda fundamental de la CO2 RR electroquímico, revisa los productos de reducción comunes y sus vías simples. Mientras tanto, la descripción general de los parámetros importantes que afectan la CO2 RR, incluidos los diferentes catalizadores en los últimos años y el electrolito, y las métricas relevantes que evalúan los electrocatalizadores. El Capítulo 2 trata de la fabricación de ZIF-8 modificado en superficie como electrodo basado en MOF para CO2 RR electroquímico para generar CO. En este trabajo, se preparó un ZIF-8 modificado en superficie mediante la introducción de una proporción muy pequeña de ácido 2,5-dihidroxitereftálico (DOBDC) en ZIF-8, logrando una densidad de corriente de CO mayor. En el Capítulo 3, se utiliza una ruta fácil para introducir grupos que contienen O con enlaces axiales en un catalizador de Fe-N-C a través de la pirólisis de estructuras orgánicas metálicas a base de Zn dopado con Fe (IRMOF-3), formando átomos únicos de Fe altamente dispersos con sitios activos HO-FeN4. Debido a la modulación del ambiente local inducida por tales grupos -OH, el catalizador D-Fe-N-C exhibe una actividad CO2 RR mejorada, incluida una alta selectividad con alta eficiencia Faradaica de CO y una estabilidad sólida. En el capítulo 4, proponemos que la introducción de átomos de Fe en catalizadores de Ni-N-C fabrica catalizadores de un solo átomo de metal doble (Ni/Fe-N-C) hacia CO2 RR para lograr una alta selectividad y actividad simultáneamente. El catalizador de doble metal optimizado mostró excelentes rendimientos, obteniendo una alta selectividad con eficiencia faradaica CO a un bajo sobrepotencial, superior a las contrapartes de un solo metal. Finalmente, el Capítulo 5 resume las conclusiones generales.
The excessive combustion of fossil fuels results in the emission of carbon dioxide (CO2), which triggers increasing environmental problems, such as, global warming, rising sea levels, extreme weather, and species extinction. Therefore, the technologies for conversion of CO2 into other value products plays a vital role in order to eliminate the CO2 concentration in atmosphere. Thereinto, electrochemical conversion of CO2 powered by renewable energy to useful chemicals is considered as an elegant solution to achieve the carbon cycle. However, due to the innerness of CO2 molecules and competitive hydrogen evolution reaction (HER), the main challenges in the field CO2 RR are the high overpotential requirement that represents the unfavourable thermodynamics and low Faradaic efficiency (FE) for the target products. Therefore, searching for a high-efficient and cost-friendly electrocatalyst is sensible and necessary for practical applications. In the past decades, metal-organic frameworks (MOFs) engrossed the enormous considerations in the field of electrocatalysis because of their large specific surface area, rich pore structure, and uniformly dispersed active sites. Although they have a great potential in electrocatalysis, most MOFs materials still suffer from insufficient activity, low conductivity, and poor stability, which would hinder their practical applications. Especially, in the field of CO2 RR, many important parameters, including high FE, low overpotential, large current density and robust stability among others, should be considered. Thus, the rational design of MOFs to fulfil the above requirements as much as possible is crucial for exploiting their future in CO2 RR applications. Therefore, in this dissertation, we made many efforts to develop MOFs-based/derived catalysts with superior efficiency, activity, and stability for boosting the CO2 RR performance. This dissertation is divided into 5 chapters: Chapter 1 is the insights on the fundamental concepts about electrochemical CO2 RR, which includes the fundamental cell of electrochemical CO2 RR, reviews the common reduction products and their simple pathways. Meanwhile, the overview of important parameters affecting CO2 RR, including different catalysts over the past years, electrolyte, and the relevant metrics evaluating the electrocatalysts as well as limitations of electrochemical CO2 reduction are also presented in this chapter. In addition, this chapter summarizes the fundamental concepts about MOFs materials and their high-temperature pyrolysis derived materials as the electrocatalysts. Chapter 2 deals with the fabrication of surface modified ZIF-8 as MOFs-based electrode for electrochemical CO2 RR to generate CO. In this work, a surface modified ZIF-8 has been prepared through introducing a very small proportion 2,5-dihidroxyterephthalic acid (DOBDC) into ZIF-8, achieving a higher current density of CO and a boosted Faradaic efficiency. In Chapter 3, a facile route is used to introduce axial bonded O-containing groups into a Fe-N-C catalyst through pyrolysis of Fe-doped Zn-based metal organic frameworks (IRMOF-3), forming highly dispersed Fe single atoms with HO-FeN4 active sites. Due to the local environment modulation induced by such -OH groups, the D-Fe-N-C catalyst exhibits an enhanced CO2 RR activity, including a high selectivity with CO Faradaic efficiency, and a robust stability, which is higher than that of the reported normal FeN4 sites without -OH groups. In Chapter 4, we proposed that introducing Fe atoms into Ni-N-C catalysts fabricates double metal (bimetallic) single-atom catalysts (Ni/Fe-N-C) towards CO2 RR to achieve a high selectivity and activity simultaneously. The optimized double-metal Ni/Fe-N-C catalyst showed an excellent performance, obtaining a high selectivity with a high CO Faradaic efficiency at a low overpotential. The performance obtained is superior to both single metal counterparts and other state-of-the-art M-N-C catalysts, proving that regulating single active sites with a second metal site potentially breaks the single metal-based activity benchmark to obtain the high selectivity and activity in CO2 RR, simultaneously. Finally, Chapter 5 summarizes the general conclusions.
Universitat Autònoma de Barcelona. Programa de Doctorat en Ciència de Materials
Fugate, Elizabeth Anne. "Investigation of Electronic Structure Effects of Transition Metal Oxides toward Water Oxidation and CO2 Reduction Catalysis." The Ohio State University, 2016. http://rave.ohiolink.edu/etdc/view?acc_num=osu1462868623.
Full textMoraes, Ricardo Sgarbi de. "Investigação da eletrocatálise de interconversão do par dióxido de carbono/íons formato para aplicação em ciclos de estocagem de hidrogênio." Universidade de São Paulo, 2016. http://www.teses.usp.br/teses/disponiveis/75/75134/tde-19042016-150431/.
Full textWith the increase CO2 emissions into atmosphere caused mainly by the energy dependence on fossil fuels, systems for generation or storage of clean energy has been studied to couple CO2 as feedstock. This work proposed a hydrogen storage cycle based on electrocatalytic steps of pair CO2/HCOO-, such electroreduction and electrooxidation. For electroreduction process were used carbon-supported tin-based electrocatalysts (Sn/C) and tin modified with cobalt (Co-Sn/C), copper (Cu-Sn/C) and palladium (Sn-Pd/C). The materials were synthesized by impregnation method followed of thermal treatment, and X Ray Diffraction (XRD) and Energy Dispersive X-ray Spectroscopy (EDS) techniques were used for physical characterization. Electrochemical tests were performed via chronoamperometry (electrolysis) and the quantification of formate ions by High Performance Liquid Chromatography (HPLC) and cyclic voltammetry (CV). Results of synthesized nanostructured materials showed crystalline structures with tin as SnO2 species, but tin oxide suffering electroreduction to SnO or SnOH in situ conditions. Electrochemical results presented that the Sn/C catalyzes the CO2 reduction to HCOO-, with an increase peak current until electrolysis potential of -1.6 V vs. Ag/AgCl/Cl- quantified by CV on palladium and platinum electrodes. Moreover, electrolysis measurements demonstrated the linear increase of HCOO- concentration after polarization for 6 hours, which indicates the high stability of Sn/C electrocatalyst. The electrocatalytic activity of tin-based electrocatalysts for CO2 reduction into HCOO- was attributed to two aspects: (i) tin favors the adsorption or interaction of CO2 through oxygen atoms, which enables the proton and electron transfer without breaking C-O bond and/or; (ii) the presence on surface of SnOH species allows the interaction with CO2 even at low potential, and leads to the formation of reactive intermediates adsorbed that undergo addition of protons and electrons to form HCOO-. Maximum Faradaic efficiency for HCOO- formation was near 7% with Hydrogen Evolution Reaction (HER) as parallel route. Investigation of the influence of the electrocatalyst nature showed inactivity of CO-Sn/C material, but the activity of CO2 electroreduction increased on Cu-Sn/C material as compared to Sn/C pure.
Sahin, Nihat Ege. "Réduction électrochimique du dioxyde de carbone sur des électrocatalyseurs à base de cuivre." Thesis, Poitiers, 2016. http://www.theses.fr/2016POIT2313/document.
Full textThe anthropogenic emissions of carbon dioxide (CO2) are the major cause of global warming. The selective CO2 reduction reaction (CO2RR) of has been proposed as a promising, convenient and efficient method for sustainable energy conversion systems. The reduction of CO2 to energetically valuable products requires the use of an appropriate electrode material. This study focuses on the preparation of Cu-based electrocatalysts supported on different types of carbon materials such as Vulcan XC-72R, mesoporous carbon CMK-3, mesoporous carbon FDU-15 and tannin based mesoporous carbon IS2M for the CO2RR under mild conditions. Besides, Vulcan XC-72R carbon supported bimetallic copper/palladium alloy materials were prepared for increasing the Faradaic yield. These copper-based catalysts were electrochemically characterized and preparative electrolyses set at constant potential were carried out in order to investigate the reduction products distribution and Faradaic yields as a function of the applied potential and catalyst loading. Chemicals such as HCOOH, CO and H2 issued from the CO2RR, were determined with in-situ and ex-situ complementary (electro)analytical and spectroscopic techniques. The significant difference in the product distribution is probably due to the ensemble (geometry and ligand) effects in the bimetallic CuPd materials, and textural structure of the supporting substrates. Selective CO2 to-HCOOH conversion has been successfully undertaken on Cu50Pd50/C with 62 % Faradaic efficiency
Dunand-Sauthier, Marie-Noe͏̈lle. "Propriétés électrochimiques et photochimiques de complexes mono(2,2'-bipyridine) carbonyle de ruthénium (II) : applications à la réduction électrocatalytique du CO2 et à la photoimagerie." Grenoble 1, 1993. http://www.theses.fr/1993GRE10105.
Full textZsoldos, Daniela. "Complexes mono et bis bipyridine carbonyle de ruthénium(II), précurseurs de polymères organométalliques : propriétés électrochimiques et applications à l'électrocatalyse de la réduction du CO2 en milieu aqueux." Université Joseph Fourier (Grenoble), 1997. http://www.theses.fr/1997GRE10027.
Full textLin, Jing-Yu, and 林靜瑜. "Study on electrocatalytic reduction of H2O and CO2 using pyrazolate-containing DNIC." Thesis, 2016. http://ndltd.ncl.edu.tw/handle/95793881457658092615.
Full text中原大學
化學研究所
104
For the past few years, untilization of fossil fuel as main energy source caused the serious greenhouse effect. Scientists attempted to develop an alternative energy source to solve the problem and reduce the CO2 emission. In this work, we successfully synthesized dinuclear DNICs containing pyrazolate bridging ligands [(NO)2Fe(μ-RPyr)2Fe(NO)2] (Pyr = pyrazolate, R = Me, NH2). These complexes show two electron reversible redox interconversion between {Fe(NO)2}9-{Fe(NO)2}9, {Fe(NO)2}9-{Fe(NO)2}10 and {Fe(NO)2}10-{Fe(NO)2}10. We try as whether catalytic reduction of water into hydrogen and electrocatalytic reduction with CO2. In the aqueous phase, our complexes have lower onset potential of electrocatalytic reduction of water -1.40 V(vs. SCE) and good stability in the prolonged electrolysis, and the Faraday efficiency of hydrogen generation reaches 100%. However, 1-Me and 1-NH2 can electrochemical react with CO2 in methanol, although about 80% of the electrons used in generating hydrogen when the process of electrolysis, we succeed reduce CO2 to formic, and the low conversion efficiency is the problem to be overcome in the future.
Bo-ShengWang and 王柏升. "On the electrocatalytic activity of transition metal nitroso-R complexes towards the reduction of CO2." Thesis, 2016. http://ndltd.ncl.edu.tw/handle/cxnb6j.
Full text國立成功大學
化學工程學系
104
In this study, the electrochemical reduction of CO2 using the electrocatalytic systems, which consists of four types of surface-modified fluorine-doped tin oxide coated glass electrodes (FTO) and three kinds of transition metal (Co2+, Ni2+, Fe2+) nitroso–R complexes was investigated. By reducing the CO2 into methanol, it can not only eliminate the excess emission of CO2 in atmosphere but also generate an alternative energy to solve both severe greenhouse effect and the energy crisis. The four types of surface-modified FTO electrodes include bare FTO, Prussian blue modified FTO (FTO|PB), Platinum (Pt) modified FTO (FTO|Pt), and Prussian blue modified FTO|Pt (FTO|Pt|PB) electrodes. The PB thin film, prepared by electrodeposition, acts as the electron transfer mediator in this work, whereas the transition metal nitroso-R complexes was used as the electrocatalysts electrocatalyzing the electrochemical reduction of CO2. It was found that the electrocatalytic system containing cobalt nitroso-R complex showed best electrocatalytic activity towards the reduction of CO2; methanol production was noticed for all the four types of electrodes, and the maximal Faradaic efficiency of 52.83 ± 17.10% can be achieved using FTO|Pt|PB. The electrocatalyst system containing ferrous nitroso-R complex exhibited second best activity; the maximal Faradaic efficiency of 11.50 ± 12.14% can be achieved using FTO|Pt|PB. The electrocatalyst system containing nickel nitroso-R complex didn’t exhibit any activity towards the electrochemical reduction of CO2 into methanol. These results is quite different from the previous work done by Ogura group in 1980s, in which they employ Pt|PB as the working electrode and ferrous nitroso-R complex showed the best activity to methanol production with a Faradaic efficiency of 83%. The lower or ignorable activity of electrocatalytic systems containing ferrous nitroso-R complex and nickel nitroso-R complex could be attributed to the fact that the instability of these two complexes under cathodic conditions or other byproducts, which cannot be detected and quantified using gas chromatography, formed during the electrochemical reduction of CO2.
Baptista, Rita Helena Duarte. "Electrocatalysis of Formate Dehydrogenase Towards CO2 Reduction." Master's thesis, 2021. http://hdl.handle.net/10362/110680.
Full textZhong, Shenghong. "Electrochemical CO2 Reduction to Value-added Chemicals on Copper-based Catalysts." Diss., 2019. http://hdl.handle.net/10754/660147.
Full textXu, Chaochen. "Transition Metal-Based Electrocatalysts for Highly Selective C02 Reduction." Thesis, 2020. http://hdl.handle.net/2440/129118.
Full textThesis (Ph.D.) -- University of Adelaide, School of Chemical Engineering and Advanced Materials, 2020