2021
DOI: 10.1002/advs.202003579
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An Investigation of Active Sites for electrochemical CO2 Reduction Reactions: From In Situ Characterization to Rational Design

Abstract: The electrochemical carbon dioxide (CO2) reduction reaction (CO2RR) is among the most promising approaches used to transform greenhouse gas into useful fuels and chemicals. However, the reaction suffers from low selectivity, high overpotential, and low reaction rate. Active site identification in the CO2RR is vital for the understanding of the reaction mechanism and the rational development of new electrocatalysts with both high selectivity and stability. Herein, in situ characterization monitoring of active s… Show more

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Cited by 139 publications
(81 citation statements)
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“…In situ spectroscopic characterization could provide detailed information on the structure and surface states of the catalysts,a sw ell as the chemical properties and binding configurations of the surface-adsorbed intermediates under actual working conditions.R ecently,t he rapid development of in situ X-ray diffraction, surface-enhanced infrared adsorp-tion spectroscopy,s urface-enhanced Raman spectroscopy, and XAS offer efficient ways for exploring these problems. [187] Thec atalyst is at the heart of ac atalytic reaction and atremendous amount of work has been devoted to exploring electrocatalyst materials for the selective reduction of CO 2 to CO in the past few years (Table S1). Enhancing the intrinsic reactivity or the density of the active sites is considered to be an effective strategy to improve the electrocatalytic efficiencies.N anostructure engineering enables us to selectively expose active crystal surfaces and introduce defects such as vacancies and grain boundaries,t hereby resulting in higher electrocatalytic activity.I na ddition, heterogeneous atom doping can also regulate the surface binding energy of the catalyst to the intermediates,which may improve the CO 2 RR performance.W hent he dimensions of catalysts are reduced from the macroscale to the nanoscale,their surface areas will increase significantly,t hus creating more active sites for the electrochemical reaction.…”
Section: Discussionmentioning
confidence: 99%
“…In situ spectroscopic characterization could provide detailed information on the structure and surface states of the catalysts,a sw ell as the chemical properties and binding configurations of the surface-adsorbed intermediates under actual working conditions.R ecently,t he rapid development of in situ X-ray diffraction, surface-enhanced infrared adsorp-tion spectroscopy,s urface-enhanced Raman spectroscopy, and XAS offer efficient ways for exploring these problems. [187] Thec atalyst is at the heart of ac atalytic reaction and atremendous amount of work has been devoted to exploring electrocatalyst materials for the selective reduction of CO 2 to CO in the past few years (Table S1). Enhancing the intrinsic reactivity or the density of the active sites is considered to be an effective strategy to improve the electrocatalytic efficiencies.N anostructure engineering enables us to selectively expose active crystal surfaces and introduce defects such as vacancies and grain boundaries,t hereby resulting in higher electrocatalytic activity.I na ddition, heterogeneous atom doping can also regulate the surface binding energy of the catalyst to the intermediates,which may improve the CO 2 RR performance.W hent he dimensions of catalysts are reduced from the macroscale to the nanoscale,their surface areas will increase significantly,t hus creating more active sites for the electrochemical reaction.…”
Section: Discussionmentioning
confidence: 99%
“…In situ spectroscopic characterization could provide detailed information on the structure and surface states of the catalysts,a sw ell as the chemical properties and binding configurations of the surface-adsorbed intermediates under actual working conditions.R ecently,t he rapid development of in situ X-ray diffraction, surface-enhanced infrared adsorp-Angewandte Chemie tion spectroscopy,s urface-enhanced Raman spectroscopy, and XAS offer efficient ways for exploring these problems. [187] Thec atalyst is at the heart of ac atalytic reaction and atremendous amount of work has been devoted to exploring electrocatalyst materials for the selective reduction of CO 2 to CO in the past few years (Table S1). Enhancing the intrinsic reactivity or the density of the active sites is considered to be an effective strategy to improve the electrocatalytic efficiencies.N anostructure engineering enables us to selectively expose active crystal surfaces and introduce defects such as vacancies and grain boundaries,t hereby resulting in higher electrocatalytic activity.I na ddition, heterogeneous atom doping can also regulate the surface binding energy of the catalyst to the intermediates,which may improve the CO 2 RR performance.W hent he dimensions of catalysts are reduced from the macroscale to the nanoscale,their surface areas will increase significantly,t hus creating more active sites for the electrochemical reaction.…”
Section: Discussionmentioning
confidence: 99%
“…Thus, for a better understanding of catalyst materials, highly developed investigation, such as X‐ray absorption fine structure, X‐ray absorption near edge structure, and electron microscopies are introduced to the materials characterization, and the results are applied to the computational calculations 128,129 . Moreover, in situ or in operando investigations on catalytic reactions are frequently reported nowadays, where these techniques provide very important information during each reaction steps in the mechanism 130,131 . However, the abovementioned analysis of the reaction mechanism so far has been mainly applied to the electrochemical reactions and thermal reactions while the PEC or PC reactions were hardly tried.…”
Section: Conclusion and Outlooksmentioning
confidence: 99%