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author:

Xu, Jiaqi (Xu, Jiaqi.) [1] | Yang, Siheng (Yang, Siheng.) [2] | Ji, Li (Ji, Li.) [3] | Mao, Jiawei (Mao, Jiawei.) [4] | Zhang, Wei (Zhang, Wei.) [5] | Zheng, Xueli (Zheng, Xueli.) [6] | Fu, Haiyan (Fu, Haiyan.) [7] | Yuan, Maolin (Yuan, Maolin.) [8] | Yang, Chengkai (Yang, Chengkai.) [9] | Chen, Hua (Chen, Hua.) [10] | Li, Ruixiang (Li, Ruixiang.) [11]

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EI CSCD

Abstract:

CO2 electroreduction has been regarded as an appealing strategy for renewable energy storage. Recently, bismuth (Bi) electrocatalysts have attracted much attention due to their excellent formate selectivity. However, many reported Bi electrocatalysts suffer from low current densities, which are insufficient for industrial applications. To reach the goal of high current CO2 reduction to formate, we fabricate Bi nanosheets (NS) with high activity through edge/terrace control and defect engineering strategy. Bi NS with preferential exposure sites are obtained by topotactic transformation, and the processes are clearly monitored by in-situ Raman and ex-situ X-ray diffraction (XRD). Bi NS-1 with a high fraction of edge sites and defect sites exhibits excellent performance, and the current density is up to ca. 870 mA·cm−2 in the flow cell, far above the industrially applicable level (100 mA·cm−2), with a formate Faradaic efficiency greater than 90%. In-situ Fourier transform infrared (FT-IR) spectra detect *OCHO, and theoretical calculations reveal that the formation energy of *OCHO on edges is lower than that on terraces, while the defects on edges further reduce the free energy changes (ΔG). The differential charge density spatial distributions reveal that the presence of defects on edges causes charge enrichment around the C-H bond, benefiting the stabilization of the *OCHO intermediate, thus remarkably lowering the ΔG. [Figure not available: see fulltext.] © 2022, Tsinghua University Press.

Keyword:

Bismuth Carbon dioxide Defect engineering Electrocatalysts Electrolytic reduction Free energy Nanosheets

Community:

  • [ 1 ] [Xu, Jiaqi]Key Laboratory of Green Chemistry & Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu; 610064, China
  • [ 2 ] [Yang, Siheng]Key Laboratory of Green Chemistry & Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu; 610064, China
  • [ 3 ] [Ji, Li]Sichuan Research Institute of Chemical Quality and Safety Testing, Chengdu; 610031, China
  • [ 4 ] [Mao, Jiawei]Sichuan Institute of Product Quality Supervision and Inspection, Chengdu; 610100, China
  • [ 5 ] [Zhang, Wei]Key Laboratory of Green Chemistry & Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu; 610064, China
  • [ 6 ] [Zheng, Xueli]Key Laboratory of Green Chemistry & Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu; 610064, China
  • [ 7 ] [Fu, Haiyan]Key Laboratory of Green Chemistry & Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu; 610064, China
  • [ 8 ] [Yuan, Maolin]Key Laboratory of Green Chemistry & Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu; 610064, China
  • [ 9 ] [Yang, Chengkai]Key Laboratory of Advanced Materials Technologies, College of Materials Science and Engineering, Fuzhou University, Fuzhou; 350108, China
  • [ 10 ] [Chen, Hua]Key Laboratory of Green Chemistry & Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu; 610064, China
  • [ 11 ] [Li, Ruixiang]Key Laboratory of Green Chemistry & Technology of Ministry of Education, College of Chemistry, Sichuan University, Chengdu; 610064, China

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Source :

Nano Research

ISSN: 1998-0124

Year: 2023

Issue: 1

Volume: 16

Page: 53-61

9 . 6

JCR@2023

9 . 6 0 0

JCR@2023

ESI HC Threshold:30

JCR Journal Grade:1

CAS Journal Grade:2

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count: 9

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 3

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