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

被引：62

作者：

Cai, Chao ^{[1
]}

Liu, Bao ^{[1
]}

Liu, Kang ^{[1
]}

Li, Pengcheng ^{[1
]}

Fu, Junwei

Wang, Yanqiu ^{[2
]}

Li, Wenzhang ^{[2
]}

Tian, Chen ^{[3
]}

Kang, Yicui ^{[4
]}

Stefancu, Andrei ^{[4
]}

Li, Hongmei ^{[1
,5
]}

Kao, Cheng-Wei ^{[6
]}

Chan, Ting-Shan ^{[6
]}

Lin, Zhang ^{[3
]}

Chai, Liyuan ^{[3
]}

Cortes, Emiliano ^{[4
]}

Liu, Min ^{[1
]}

机构：

[1] Cent South Univ, Hunan Joint Int Res Ctr Carbon Dioxide Resource U, Sch Phys & Elect, State Key Lab Powder Met, Changsha 410083, Peoples R China

[2] Cent South Univ, Sch Chem & Chem Engn, Changsha 410083, Peoples R China

[3] Cent South Univ, Sch Met & Environm, Changsha 410083, Hunan, Peoples R China

[4] Ludwig Maximilians Univ Munchen, Nanoinst Munchen, Fak Phys, D-80539 Munich, Germany

[5] Zhengzhou Univ, Sch Mat Sci & Engn, Zhengzhou 450001, Peoples R China

[6] Natl Synchrotron Radiat Res Ctr, Hsinchu 30076, Taiwan

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2022年 / 61卷 / 44期

基金：

中国博士后科学基金;

关键词：

Ag-Based; Electric Filed; Electrochemical CO2 Reduction; Heteroatoms; Intermediate; ELECTROCHEMICAL REDUCTION; MECHANISTIC INSIGHTS;

D O I：

10.1002/anie.202212640

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Carbon dioxide electroreduction (CO2RR) is a sustainable way of producing carbon-neutral fuels. Product selectivity in CO2RR is regulated by the adsorption energy of reaction-intermediates. Here, we employ differential phase contrast-scanning transmission electron microscopy (DPC-STEM) to demonstrate that Sn heteroatoms on a Ag catalyst generate very strong and atomically localized electric fields. In situ attenuated total reflection infrared spectroscopy (ATR-IR) results verified that the localized electric field enhances the adsorption of *COOH, thus favoring the production of CO during CO2RR. The Ag/Sn catalyst exhibits an approximately 100 % CO selectivity at a very wide range of potentials (from -0.5 to -1.1 V, versus reversible hydrogen electrode), and with a remarkably high energy efficiency (EE) of 76.1 %.

引用

页数：6

共 44 条

[1] Hierarchically 3D Porous Ag Nanostructures Derived from Silver Benzenethiolate Nanoboxes: Enabling CO2 Reduction with a Near-Unity Selectivity and Mass-Specific Current Density over 500 A/g [J].

Abeyweera, Sasitha C. ;

Yu, Jie ;

Perdew, John P. ;

Yan, Qimin ;

Sun, Yugang .

NANO LETTERS, 2020, 20 (04) :2806-2811

[2]

[Anonymous], 2020, ANGEW CHEM, V132, P12153

[3]

[Anonymous], 2021, ANGEW CHEM, V133, P20795

[4]

[Anonymous], 2021, ANGEW CHEM, V133, P6235

[5]

[Anonymous], 2016, ANGEW CHEM, V128, P9900

[6]

[Anonymous], 2018, ANGEW CHEM, V130, P12483

[7]

[Anonymous], 2019, ANGEW CHEM, V131, P4717

[8]

[Anonymous], 2022, ANGEW CHEM, V134

[9] 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

[10] Optimizing Hydrogen Binding on Ru Sites with RuCo Alloy Nanosheets for Efficient Alkaline Hydrogen Evolution [J].

Cai, Chao ;

Liu, Kang ;

Zhu, Yuanmin ;

Li, Pengcheng ;

Wang, Qiyou ;

Liu, Bao ;

Chen, Shanyong ;

Li, Huangjingwei ;

Zhu, Li ;

Li, Hongmei ;

Fu, Junwei ;

Chen, Yu ;

Pensa, Evangelina ;

Hu, Junhua ;

Lu, Ying-Rui ;

Chan, Ting-Shan ;

Cortes, Emiliano ;

Liu, Min .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2022, 61 (04)

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