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Title: Modulating the electronic structure of ultrathin layered double hydroxide nanosheets with fluorine: an efficient electrocatalyst for the oxygen evolution reaction

Abstract

In this work, we effectively modulate the electronic structure of Co 3Fe layered double hydroxides (LDHs) by F-doping using a CHF 3-plasma etching technique. CHF 3-plasma can selectively fill oxygen vacancies with F– ions that can drastically tune the electronic structure with the highest electronegativity and create metal vacancies at the same time. The as-obtained F-Co 3Fe LDH ultrathin nanosheets exhibit excellent oxygen evolution reaction (OER) properties. The outstanding electrochemical activity can be attributed to the incorporation of F– ions that strongly modulate the charge distribution of surrounding atoms to facilitate the adsorption of OER intermediates. This report reflects a simple way to create metal vacancies and selectively fill oxygen vacancies with fluorine at the same time, and brings about a deep understanding of the electronic environment-activity relationship of LDHs for the OER.

Authors:
 [1]; ORCiD logo [2];  [3];  [4];  [4];  [5]; ORCiD logo [6];  [6]; ORCiD logo [7]; ORCiD logo [7]
  1. Hunan Univ., Changsha (China); Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Tamkang Univ. (Taiwan)
  3. National Synchrotron Radiation Research Center, Hsinchu (Taiwan)
  4. Stony Brook Univ., NY (United States)
  5. State Univ. of New York (SUNY) at Binghamton, Plattsburgh, NY (United States)
  6. Brookhaven National Lab. (BNL), Upton, NY (United States)
  7. Hunan Univ., Changsha (China)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1547017
Report Number(s):
BNL-211951-2019-JAAM
Journal ID: ISSN 2050-7488; JMCAET
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 7; Journal Issue: 24; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Liu, Zhijuan, Dong, Chung-Li, Huang, Yu-Cheng, Cen, Jiajie, Yang, Haotian, Chen, Xiaobo, Tong, Xiao, Su, Dong, Wang, Yanyong, and Wang, Shuangyin. Modulating the electronic structure of ultrathin layered double hydroxide nanosheets with fluorine: an efficient electrocatalyst for the oxygen evolution reaction. United States: N. p., 2019. Web. doi:10.1039/C9TA03882E.
Liu, Zhijuan, Dong, Chung-Li, Huang, Yu-Cheng, Cen, Jiajie, Yang, Haotian, Chen, Xiaobo, Tong, Xiao, Su, Dong, Wang, Yanyong, & Wang, Shuangyin. Modulating the electronic structure of ultrathin layered double hydroxide nanosheets with fluorine: an efficient electrocatalyst for the oxygen evolution reaction. United States. doi:10.1039/C9TA03882E.
Liu, Zhijuan, Dong, Chung-Li, Huang, Yu-Cheng, Cen, Jiajie, Yang, Haotian, Chen, Xiaobo, Tong, Xiao, Su, Dong, Wang, Yanyong, and Wang, Shuangyin. Thu . "Modulating the electronic structure of ultrathin layered double hydroxide nanosheets with fluorine: an efficient electrocatalyst for the oxygen evolution reaction". United States. doi:10.1039/C9TA03882E.
@article{osti_1547017,
title = {Modulating the electronic structure of ultrathin layered double hydroxide nanosheets with fluorine: an efficient electrocatalyst for the oxygen evolution reaction},
author = {Liu, Zhijuan and Dong, Chung-Li and Huang, Yu-Cheng and Cen, Jiajie and Yang, Haotian and Chen, Xiaobo and Tong, Xiao and Su, Dong and Wang, Yanyong and Wang, Shuangyin},
abstractNote = {In this work, we effectively modulate the electronic structure of Co3Fe layered double hydroxides (LDHs) by F-doping using a CHF3-plasma etching technique. CHF3-plasma can selectively fill oxygen vacancies with F– ions that can drastically tune the electronic structure with the highest electronegativity and create metal vacancies at the same time. The as-obtained F-Co3Fe LDH ultrathin nanosheets exhibit excellent oxygen evolution reaction (OER) properties. The outstanding electrochemical activity can be attributed to the incorporation of F– ions that strongly modulate the charge distribution of surrounding atoms to facilitate the adsorption of OER intermediates. This report reflects a simple way to create metal vacancies and selectively fill oxygen vacancies with fluorine at the same time, and brings about a deep understanding of the electronic environment-activity relationship of LDHs for the OER.},
doi = {10.1039/C9TA03882E},
journal = {Journal of Materials Chemistry. A},
number = 24,
volume = 7,
place = {United States},
year = {2019},
month = {5}
}

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