Study on reaction mechanism of CO2 electro-reduction to CO in organic medium: Revealed by experimental and spectroscopic Investigations

被引：0

作者：

Shen, Fengxia ^{[1
,2
]}

Wu, Shuai ^{[1
]}

Kurniawan, Mario ^{[2
]}

Ostheimer, David ^{[3
]}

Shi, Jin ^{[1
]}

Chen, Tianyou ^{[4
]}

Bund, Andreas ^{[2
]}

Hannappel, Thomas ^{[3
]}

Liu, Jianxiong ^{[1
]}

Zhao, Pengchong ^{[1
]}

Miao, Shipeng ^{[1
]}

机构：

[1] Kunming Univ Sci & Technol, Coll Met & Energy Engn, State Key Lab Complex Nonferrous Met Resources Cle, 121 St,Wenchang Rd 68, Kunming 650093, Peoples R China

[2] Tech Univ Ilmenau, Electrochem & Electroplating Grp, Gustav Kirchhoff Str 5, D-98693 Ilmenau, Germany

[3] Tech Univ Ilmenau, Fundamentals Energy Mat Grp, Gustav Kirchhoff Str 6, D-98693 Ilmenau, Germany

[4] Kunming Univ Sci & Technol, Engn Training Ctr, 121 St,Wenchang Rd 68, Kunming 650093, Peoples R China

来源：

APPLIED SURFACE SCIENCE | 2025年 / 681卷

基金：

中国国家自然科学基金;

关键词：

CO; 2; electro-reduction; TMAC/PC organic electrolyte; DEMS; In-situ ATR-IRAS/Raman spectroscopy; DFT calculation; ELECTROCHEMICAL REDUCTION; CARBON-DIOXIDE; TETRAALKYLAMMONIUM SALTS; SUPPORTING ELECTROLYTES; IONIC LIQUID; ELECTROREDUCTION; GOLD; INSIGHTS; IR; MOLECULES;

D O I：

10.1016/j.apsusc.2024.161459

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

CO2 2 electrocatalytic reduction (CO2RR) 2 RR) to CO in organic electrolytes has received considerable attention due to its potential industrial application prospect. However, the reaction mechanism is not fully understood. In this study, we employed experimental observation, in-situ ATR-IRAS and Raman spectroscopy to elucidate the reaction mechanism of CO2 2 electro-reduction to CO in an organic medium. The reaction intermediates *CO2 center dot-, 2 center dot- , * (CO 2 ) 2 center dot- and *CO has been identified during CO2RR. 2 RR. Based on these results, the reaction mechanism has been discussed extensively. Density Functional Theory (DFT) analysis further indicates that the electrolytic CO2 2 reduction to CO in organic electrolyte is relatively more difficult than that in aqueous solutions.

引用

页数：9

共 72 条

[1] CO2 Electrolysis via Surface-Engineering Electrografted Pyridines on Silver Catalysts [J].

Abdinejad, Maryam ;

Irtem, Erdem ;

Farzi, Amirhossein ;

Sassenburg, Mark ;

Subramanian, Siddhartha ;

Van Montfort, Hugo-Pieter Iglesias ;

Ripepi, Davide ;

Li, Mengran ;

Middelkoop, Joost ;

Seifitokaldani, Ali ;

Burdyny, Thomas .

ACS CATALYSIS, 2022, 12 (13) :7862-7876

[2] Organic, Organometallic and Bioorganic Catalysts for Electrochemical Reduction of CO2 [J].

Apaydin, Dogukan Hazar ;

Schlager, Stefanie ;

Portenkirchner, Engelbert ;

Sariciftci, Niyazi Serdar .

CHEMPHYSCHEM, 2017, 18 (22) :3094-3116

[3] Toward Unifying the Mechanistic Concepts in Electrochemical CO2 Reduction from an Integrated Material Design and Catalytic Perspective [J].

Bagchi, Debabrata ;

Roy, Soumyabrata ;

Sarma, Saurav Ch ;

Peter, Sebastian C. .

ADVANCED FUNCTIONAL MATERIALS, 2022, 32 (51)

[4] Mechanistic Insights into the Reduction of CO2 on Tin Electrodes using in Situ ATR-IR Spectroscopy [J].

Baruch, Maor F. ;

Pander, James E., III ;

White, James L. ;

Bocarsly, Andrew B. .

ACS CATALYSIS, 2015, 5 (05) :3148-3156

[5] Revealing Mechanistic Processes in Gas-Diffusion Electrodes During CO2 Reduction via Impedance Spectroscopy [J].

Bienen, Fabian ;

Kopljar, Dennis ;

Loewe, Armin ;

Geiger, Simon ;

Wagner, Norbert ;

Klemm, Elias ;

Friedrich, Kaspar Andreas .

ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 2020, 8 (36) :13759-13768

[6] IMPROVED TETRAHEDRON METHOD FOR BRILLOUIN-ZONE INTEGRATIONS [J].

BLOCHL, PE ;

JEPSEN, O ;

ANDERSEN, OK .

PHYSICAL REVIEW B, 1994, 49 (23) :16223-16233

[7] Heteroatoms Induce Localization of the Electric Field and Promote a Wide Potential-Window Selectivity Towards CO in the CO2 Electroreduction [J].

Cai, Chao ;

Liu, Bao ;

Liu, Kang ;

Li, Pengcheng ;

Fu, Junwei ;

Wang, Yanqiu ;

Li, Wenzhang ;

Tian, Chen ;

Kang, Yicui ;

Stefancu, Andrei ;

Li, Hongmei ;

Kao, Cheng-Wei ;

Chan, Ting-Shan ;

Lin, Zhang ;

Chai, Liyuan ;

Cortes, Emiliano ;

Liu, Min .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2022, 61 (44)

[8] In Situ Characterization for Boosting Electrocatalytic Carbon Dioxide Reduction [J].

Cao, Xueying ;

Tan, Dongxing ;

Wulan, Bari ;

Hui, K. S. ;

Hui, K. N. ;

Zhang, Jintao .

SMALL METHODS, 2021, 5 (10)

[9] In-situ/operando Raman techniques for in-depth understanding on electrocatalysis [J].

Chen, Mingpeng ;

Liu, Di ;

Qiao, Lulu ;

Zhou, Pengfei ;

Feng, Jinxian ;

Ng, Kar Wei ;

Liu, Qingju ;

Wang, Shuangpeng ;

Pan, Hui .

CHEMICAL ENGINEERING JOURNAL, 2023, 461

[10] On the origin of the elusive first intermediate of CO2 electroreduction [J].

Chernyshova, Irina, V ;

Somasundaran, Ponisseril ;

Ponnurangam, Sathish .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2018, 115 (40) :E9261-E9270

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