Atom vacancies induced electron-rich surface of ultrathin Bi nanosheet for efficient electrochemical CO2 reduction

被引：145

作者：

Zhao, Meiming ^{[1
]}

Gu, Yaliu ^{[1
]}

Gao, Weicheng ^{[2
]}

Cui, Peixin ^{[3
]}

Tang, Huang ^{[1
]}

Wei, Xinying ^{[1
]}

Zhu, Heng ^{[1
]}

Li, Guoqiang ^{[4
]}

Yan, Shicheng ^{[1
]}

Zhang, Xiuyun ^{[2
]}

Zou, Zhigang ^{[1
,5
]}

机构：

[1] Nanjing Univ, Natl Lab Solid State Microstruct, Collaborat Innovat Ctr Adv Microstruct, Coll Engn & Appl Sci,ERERC, 22 Hankou Rd, Nanjing 210093, Jiangsu, Peoples R China

[2] Yangzhou Univ, Coll Phys Sci & Technol, Yangzhou 225002, Jiangsu, Peoples R China

[3] Chinese Acad Sci, Inst Soil Sci, Key Lab Soil Environm & Pollut Remediat, Nanjing 210008, Jiangsu, Peoples R China

[4] Henan Univ, Key Lab Photovolta Mat Henan Prov, Kaifeng 475004, Henan, Peoples R China

[5] Nanjing Univ, Sch Phys, Jiangsu Key Lab Nano Technol, 22 Hankou Rd, Nanjing 210093, Jiangsu, Peoples R China

来源：

APPLIED CATALYSIS B-ENVIRONMENTAL | 2020年 / 266卷 / 266期

基金：

中国国家自然科学基金;

关键词：

Bi nanosheet; Atom vacancies; Topological transformation; Electrochemical CO2 reduction; DENSITY-FUNCTIONAL THEORY; IN-SITU; CARBON-DIOXIDE; BISMUTH; OXIDATION; AU; FORMALDEHYDE; ADSORPTION; ENERGETICS; CHEMISTRY;

D O I：

10.1016/j.apcatb.2020.118625

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：

The overpotential and selectivity of electrochemical CO2 reduction over metal electrodes are closely related to the adsorption strength of key intermediate. Defect engineering of the materials can modulate the energetic difference between the antibonding states and the Fermi level, thus strengthening the surface-adsorbate chemical bonds and boosting the steady progress of the electrochemical reaction. Here, we proposed an efficient strategy to electrochemically reduced layered Bi2O2CO3 to Bi nanosheet with (001) dominant facet and atom vacancies. The Bi nanosheet exhibits 90 % CO2-to-formate Faradaic efficiency at a low overpotential of 420 mV and excellent stability over 100 h in 0.1 M KHCO3 electrolyte. Spectroscopic and computational studies confirm that the Bi atom vacancies induced the electron-rich surface, leading the movement of p states towards the Fermi level, hence decreasing the activation energy of CO2 to CO2-* radical and promoting the stability of OCHO* intermediate via p orbitals hybridization between the O in carbon-containing intermediates and the Bi electrode.

引用

页数：8

共 48 条

[1] Electrodeposition of Tin-Based Electrocatalysts with Different Surface Tin Species Distributions for Electrochemical Reduction of CO2 to HCOOH [J].