首页|Mechanism of surface oxygen-containing species promoted electrocatalytic CO2 reduction

Mechanism of surface oxygen-containing species promoted electrocatalytic CO2 reduction

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Oxygen-containing species have been demonstrated to play a key role in facilitating electrocatalytic CO2 reduction(CO2RR),particularly in enhancing the selectivity towards multi-carbon(C2+)products.However,the underlying promotion mechanism is still under debate,which greatly limits the rational optimization of the catalytic performance of CO2RR.Herein,taking CO2 and O2 co-electrolysis over Cu as the prototype,we successfully clarified how O2 boosts CO2RR from a new perspective by employing comprehensive theoretical simulations.Our results demonstrated that O2 in feed gas can be rapidly reduced into *OH,leading to the partial oxidation of Cu surface under reduction conditions.Surface*OH accelerates the formation of quasi-specifically adsorbed K+due to the electrostatic interaction between *OH and K+ions,which significantly increases the concentration of K+near the Cu surface.These quasi-specifically adsorbed K+ions can not only lower the C-C coupling barriers but also promote the hydrogenation of CO2 to improve the CO yield rate,which are responsible for the remarkably enhanced efficiency of C2+products.During the whole process,O2 co-electrolysis plays an indispensable role in stabilizing surface *OH.This mechanism can be also adopted to understand the effect of high pH of electrolyte and residual O in oxide-derived Cu(OD-Cu)on the catalytic efficiency towards C2+products.Therefore,our work provides new insights into strategies for improving C2+products on the Cu-based cat-alysts,i.e.,maintaining partial oxidation of surface under reduction conditions.

CO2 reductionFirst-principles calculationsOxygen-containing speciesReaction mechanism

Zhanzhao Fu、Yixin Ouyang、Mingliang Wu、Chongyi Ling、Jinlan Wang

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Key Laboratory of Quantum Materials and Devices of Ministry of Education,School of Physics,Southeast University,Nanjing 21189,China

国家重点研发计划国家重点研发计划国家自然科学基金国家自然科学基金国家自然科学基金Basic Research Program of Jiangsu ProvinceBasic Research Program of Jiangsu Province中央高校基本科研业务费专项Big Data Computing Center of Southeast UniversityNational Supercomputing Center of Tianjin

2022YFA15031002021YFA1500700220330029226111222303011BK20220800BK202220072242023R40016

2024

10.1016/j.scib.2024.03.012

科学通报(英文版)
中国科学院

科学通报(英文版)

CSTPCD
ISSN：1001-6538
年,卷(期)：2024.69(10)
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