The electrochemical CO_(2)reduction reaction(CO_(2)RR)is considered a promising technology for converting atmospheric CO_(2)into valuable chemicals.It is a significant way to mitigate the shortage of fossil energy and...The electrochemical CO_(2)reduction reaction(CO_(2)RR)is considered a promising technology for converting atmospheric CO_(2)into valuable chemicals.It is a significant way to mitigate the shortage of fossil energy and store excessive renewable electricity in fuels to maintain carbon neutrality.Considering the substantially reduced cost of clean electricity,C1 molecule unitization has emerged as a competitive strategy for room-temperature electrolysis.However,the practical implementation of CO_(2)RR has been hindered by low desired product selectivity,high overpotential,and undesirable hydrogen evolution reactions(HER).Consequently,it is imperative to execute a timely assessment of advanced strategies in CO_(2)RR,with emphasis on catalytic design strategies,understanding of structure–activity relationships,and deactivation of catalysts.In this context,it is imperative to investigate the intrinsic active sites and reaction mechanisms.This review focuses on the design of novel catalysts and their active sites via operando techniques.The combination of advanced characterization techniques and theoretical calculations provides a high-throughput way to obtain a deeper understanding of the reaction mechanism.Furthermore,optimization of the interplay between the catalyst surface and reaction intermediate disturbs the linear correlation between the adsorption energies of the intermediates,resulting in a convoluted cascade system.The appropriate strategies for CO_(2)RR,challenges,and future approaches are projected in this review to stimulate major innovations.Moreover,the plausible research directions are discussed for producing C_(1)chemicals via electrochemical CO_(2)RR at room temperature.展开更多
The harsh corrosive environment and sluggish oxygen evolution reaction(OER)kinetics at the anode of proton exchange membrane water electrolysis(PEMWE)cells warrant the use of excess Ir,thereby hindering large-scale in...The harsh corrosive environment and sluggish oxygen evolution reaction(OER)kinetics at the anode of proton exchange membrane water electrolysis(PEMWE)cells warrant the use of excess Ir,thereby hindering large-scale industrialization.To mitigate these issues,the present study aimed at fabricating a robust low-Ir-loading electrode via one-pot synthesis for efficient PEMWE.The pre-electrode was first prepared by alloying through the co-electrodeposition of Ir and Co,followed by the fabrication of Ir–Co oxide(Co-incorporated Ir oxide)electrodes via electrochemical dealloying.Two distinct dealloying techniques resulted in a modified valence state of Ir,and the effects of Co incorporation on the activity and stability of the OER catalysts were clarified using density functional theory(DFT)calculations,which offered theoretical insights into the reaction mechanism.While direct experimental validation of the oxygen evolution mechanism remains challenging under the current conditions,DFT-based theoretical modeling provided valuable perspectives on how Co incorporation could influence key steps in oxygen evolution catalysis.The Ir–Co oxide electrode with a selectively modulated valence state showed impressive performance with an overpotential of 258 mV at 10 mA cm^(−2),a low Tafel slope of 29.4 mV dec^(−1),and stability for 100 h at 100 mA cm^(−2)in the OER,in addition to a low overpotential of 16 mV at−10 mA cm^(−2)and high stability for 24 h in the hydrogen evolution reaction.The PEMWE cell equipped with the bifunctional Ir–Co oxide electrode as the anode and cathode exhibited outstanding performance(11.4 A cm^(−2)at 2.3 Vcell)despite having a low noble-metal content of 0.4 mgNM cm^(−2).展开更多
基金funded by a National Research Council of Science&Technology grant from the Ministry of Science and ICT(MSIT),Republic of Korea(No.CAP21012-100)the Korea Institute of Energy Technology Evaluation and Planning(KETEP)under the Ministry of Trade,Industry&Energy(MOTIE),Republic of Korea(No.20224C10300010)。
文摘The electrochemical CO_(2)reduction reaction(CO_(2)RR)is considered a promising technology for converting atmospheric CO_(2)into valuable chemicals.It is a significant way to mitigate the shortage of fossil energy and store excessive renewable electricity in fuels to maintain carbon neutrality.Considering the substantially reduced cost of clean electricity,C1 molecule unitization has emerged as a competitive strategy for room-temperature electrolysis.However,the practical implementation of CO_(2)RR has been hindered by low desired product selectivity,high overpotential,and undesirable hydrogen evolution reactions(HER).Consequently,it is imperative to execute a timely assessment of advanced strategies in CO_(2)RR,with emphasis on catalytic design strategies,understanding of structure–activity relationships,and deactivation of catalysts.In this context,it is imperative to investigate the intrinsic active sites and reaction mechanisms.This review focuses on the design of novel catalysts and their active sites via operando techniques.The combination of advanced characterization techniques and theoretical calculations provides a high-throughput way to obtain a deeper understanding of the reaction mechanism.Furthermore,optimization of the interplay between the catalyst surface and reaction intermediate disturbs the linear correlation between the adsorption energies of the intermediates,resulting in a convoluted cascade system.The appropriate strategies for CO_(2)RR,challenges,and future approaches are projected in this review to stimulate major innovations.Moreover,the plausible research directions are discussed for producing C_(1)chemicals via electrochemical CO_(2)RR at room temperature.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(RS-2024-00340074,RS-2024-00409901,2022M3I3A1081901,and RS-2024-00413272)。
文摘The harsh corrosive environment and sluggish oxygen evolution reaction(OER)kinetics at the anode of proton exchange membrane water electrolysis(PEMWE)cells warrant the use of excess Ir,thereby hindering large-scale industrialization.To mitigate these issues,the present study aimed at fabricating a robust low-Ir-loading electrode via one-pot synthesis for efficient PEMWE.The pre-electrode was first prepared by alloying through the co-electrodeposition of Ir and Co,followed by the fabrication of Ir–Co oxide(Co-incorporated Ir oxide)electrodes via electrochemical dealloying.Two distinct dealloying techniques resulted in a modified valence state of Ir,and the effects of Co incorporation on the activity and stability of the OER catalysts were clarified using density functional theory(DFT)calculations,which offered theoretical insights into the reaction mechanism.While direct experimental validation of the oxygen evolution mechanism remains challenging under the current conditions,DFT-based theoretical modeling provided valuable perspectives on how Co incorporation could influence key steps in oxygen evolution catalysis.The Ir–Co oxide electrode with a selectively modulated valence state showed impressive performance with an overpotential of 258 mV at 10 mA cm^(−2),a low Tafel slope of 29.4 mV dec^(−1),and stability for 100 h at 100 mA cm^(−2)in the OER,in addition to a low overpotential of 16 mV at−10 mA cm^(−2)and high stability for 24 h in the hydrogen evolution reaction.The PEMWE cell equipped with the bifunctional Ir–Co oxide electrode as the anode and cathode exhibited outstanding performance(11.4 A cm^(−2)at 2.3 Vcell)despite having a low noble-metal content of 0.4 mgNM cm^(−2).
