Stabilizing *CO2 Intermediates at the Acidic Interface using Molecularly Dispersed Cobalt Phthalocyanine as Catalysts for CO2 Reduction

Author:

Feng Shijia1,Wang Xiaojun12ORCID,Cheng Dongfang3,Luo Yao4,Shen Mengxin1,Wang Jingyang1,Zhao Wei1,Fang Susu4,Zheng Hongzhi1,Ji Liyao1,Zhang Xing1,Xu Weigao4,Liang Yongye5,Sautet Philippe36,Zhu Jia12ORCID

Affiliation:

1. National Laboratory of Solid State Microstructures Collaborative Innovation Center of Advanced Microstructures College of Engineering and Applied Sciences Nanjing University Nanjing Jiangsu 210023 P. R. China

2. School of Sustainable Energy and Resources Nanjing University Suzhou 215163 P. R. China

3. Department of Chemical and Biomolecular Engineering University of California, Los Angeles Los Angeles CA 90095 USA

4. Key Laboratory of Mesoscopic Chemistry of Ministry of Education School of Chemistry and Chemical Engineering Nanjing University Nanjing 210023 P. R. China

5. Department of Materials Science and Engineering Guangdong Provincial Key Laboratory of Energy Materials for Electric Power Southern University of Science and Technology Shenzhen China

6. Department of Chemistry and Biochemistry University of California, Los Angeles Los Angeles CA 90095 USA

Abstract

AbstractCO2 electroreduction (CO2R) operating in acidic media circumvents the problems of carbonate formation and CO2 crossover in neutral/alkaline electrolyzers. Alkali cations have been universally recognized as indispensable components for acidic CO2R, while they cause the inevitable issue of salt precipitation. It is therefore desirable to realize alkali‐cation‐free CO2R in pure acid. However, without alkali cations, stabilizing *CO2 intermediates by catalyst itself at the acidic interface poses as a challenge. Herein, we first demonstrate that a carbon nanotube‐supported molecularly dispersed cobalt phthalocyanine (CoPc@CNT) catalyst provides the Co single‐atom active site with energetically localized d states to strengthen the adsorbate‐surface interactions, which stabilizes *CO2 intermediates at the acidic interface (pH=1). As a result, we realize CO2 conversion to CO in pure acid with a faradaic efficiency of 60 % at pH=2 in flow cell. Furthermore, CO2 is successfully converted in cation exchanged membrane‐based electrode assembly with a faradaic efficiency of 73 %. For CoPc@CNT, acidic conditions also promote the intrinsic activity of CO2R compared to alkaline conditions, since the potential‐limiting step, *CO2 to *COOH, is pH‐dependent. This work provides a new understanding for the stabilization of reaction intermediates and facilitates the designs of catalysts and devices for acidic CO2R.

Funder

National Natural Science Foundation of China

Publisher

Wiley

Subject

General Chemistry,Catalysis

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