首页|Understanding the Temperature Effect on Carbon-Carbon Coupling during CO2 and CO Electroreduction in Zero-Gap Electrolyzers

Understanding the Temperature Effect on Carbon-Carbon Coupling during CO2 and CO Electroreduction in Zero-Gap Electrolyzers

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Cu-catalyzed electrochemical CO2 reduction reaction(CO2RR)and CO reduction reaction(CORR)are of great interest due to their po-tential to produce carbon-neutral and value-added multicarbon(C2+)chemicals.In practice,CO2RR and CORR are typically operated at industrially relevant current densities,making the process exothermal.Although the increased operation temperature is known to af-fect the performance of CO2RR and CORR,the relationship between temperatures and kinetic parameters was not clearly elaborated,particularly in zero-gap reactors.In this study,we detail the effect of the temperature on Cu-catalyzed CO2RR and CORR.Our electro-chemical and operando spectroscopic studies show that high temperatures increase the activity of CO2RR to CO and CORR to C2H4 by enhancing the mass transfer of CO2 and CO.As the rates of these two processes are highly influenced by reactant diffusion,elevating the operating temperature results in high local CO2 and CO availability to accelerate product formation.Consequently,the*CO cover-age in both cases increases at higher temperatures.However,under CO2RR conditions,*CO desorption is more favorable than car-bon-carbon(C—C)coupling thermodynamically at high temperatures,causing the reduction in the Faradaic efficiency(FE)of C2H4.In CORR,the high-temperature-augmented CO diffusion overcomes the unfavorable adsorption thermodynamics,increasing the proba-bility of C—C coupling.

Zero-gap electrolyzersCO2 and CO reductionTemperature effectSelectivityC—C couplingAdsorption

Mengjiao Zhuansun、Xuan Wang、Wenzhi Teng、Yuhang Wang

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Institute of Functional Nano & Soft Materials(FUNSOM),Soochow University,199 Ren'ai Road,Suzhou,Jiangsu 215123,China

Jiangsu Key Laboratory for Advanced Negative Carbon Technologies,Soochow University,199 Ren'ai Road,Suzhou,Jiangsu 215123,China

2024

中国化学(英文版)
中国化学会 上海有机化学研究所

中国化学(英文版)

CSTPCD
影响因子:0.848
ISSN:1001-604X
年,卷(期):2024.42(22)