Effect of bicarbonate on CO_(2) electroreduction over cathode catalysts

查看全文 作　　者：Wanyu [1,2]Deng;Tenghui [1,2]Yuan;Sai [1,2]Chen;Huimin [1,2]Li;Congling [1,2]Hu;Hao [1,2]Dong;Bo [1,2]Wu;Tuo [1,2]Wang;Jingkun [1,2]Li;Geoffrey [4]A.Ozin;Jinlong [1,2,3]Gong

机构地区：[1]Key Laboratory for Green Chemical Technology of Ministry of Education,School of Chemical Engineering and Technology,Tianjin University,300072,China;[2]Collaborative Innovation Center of Chemical Science and Engineering(Tianjin),Tianjin 300072,China;[3]Joint School of National University of Singapore and Tianjin University,International Campus of Tianjin University,Binhai New City,Fuzhou 350207,China;[4]Department of Chemistry,University of Toronto,Toronto,Canada

出　　处：《Fundamental Research》索引2021年第1卷第4期,共7页

基　　金：This work is supported by the National Key Research and Development Program of China(2016YFB0600901);the National Natural Science Foundation of China(21525626,22038009,51861125104);the Program of Introducing Talents of Discipline to Universities(No.BP0618007)for financial support. 摘　　要：CO_(2) electroreduction (CO_(2) ER) using renewable energy is ideal for mitigating the greenhouse effect and closing the carbon cycle. Bicarbonate (HCO_(3)−) is most commonly employed as the electrolyte anion because it is known to facilitate CO_(2) ER. However, its dynamics in the electric double layer remains obscure and requires more in-depth investigation. Herein, we investigate the refined reduction process of bicarbonate by employing in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy. By comparing the product distributions in Ar-saturated KCl and KHCO_(3) electrolytes, we confirmed CO production from HCO_(3)^(−) in the absence of an external CO_(2) source. Notably, in contrast to an electric compulsion, negatively charged HCO_(3)− anions were found to accumulate near the electrode surface. A reduction mechanism of HCO3− is proposed in that HCO3− is not adsorbed over a catalyst, but may be enriched near the electrode surface and converted to CO_(2) and react over Au and Cu electrodes. The dependence of the CO_(2) ER activity on the local HCO3− concentration was subsequently discovered, which was in turn dependent on the bulk HCO3− concentration and cathodic potential. In particular, the local HCO3− concentration was limited by the cathodic potential, leading to a plateau in the CO_(2) ER activity. The proposed mechanism provides insights into the interaction between the catalyst and the electrolyte in CO_(2) ER. 关键词：Electrochemical reduction of CO_(2) ATR-SEIRAS BICARBONATE Catalyst-electrolyte interface

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Effect of bicarbonate on CO_(2) electroreduction over cathode catalysts

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