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The origins of catalytic selectivity for the electrochemical conversion of carbon dioxide to methanol

Nano Research 2024年第1期17卷 5-17页

作者： Tian Wang Yating Wang Yuhang Li Chunzhong Li Key Laboratory for Ultrafine Materials of Ministry of Education Shanghai Engineering Research Center of Hierarchical NanomaterialsFrontiers Science Center for Materiobiology and Dynamic ChemistrySchool of Materials Science and EngineeringEast China University of Science&TechnologyShanghai 200237China School of Chemical Engineering East China University of Science&TechnologyShanghai 200237China

The electrocatalytic conversion of carbon dioxide(CO_(2))into useful fuels and chemical feedstocks is an emerging route to alleviate global warming and reduce reliance on fossil ***(CH_(3)OH),as one of the most significant and widely used liquid fuels that can be generated by CO_(2)reduction,is essential in the chemical *** this minireview,we unravel the origins of the selective formation of CH_(3)OH via CO_(2)reduction,including catalyst composition designs,local structure modulations,and electrolyte/catalyst interface ***,the remaining challenges and perspectives for the CO_(2)-to-CH_(3)OH reduction are proposed.

关键词： methanol carbon dioxide(CO_(2))reduction reaction electrochemistry electrocatalyst catalyst-electrolyte interface

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

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Fundamental Research 2021年第4期1卷 432-438页

作者： Wanyu Deng Tenghui Yuan Sai Chen Huimin Li Congling Hu Hao Dong Bo Wu Tuo Wang Jingkun Li Geoffrey A.Ozin Jinlong Gong Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin University300072China Collaborative Innovation Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China Department of Chemistry University of TorontoTorontoCanada

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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