skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Anion-Regulated Selective Generation of Cobalt Sites in Carbon: Toward Superior Bifunctional Electrocatalysis

Abstract

The introduction of active transition metal sites (TMSs) in carbon enables the synthesis of noble-metal-free electrocatalysts for clean energy conversion applications, however, there are often multiple existing forms of TMSs, which are of different natures and catalytic models. Regulating the evolution of distinctive TMSs is highly desirable but remains challenging to date. Anions, as essential elements involved in the synthesis, have been totally neglected previously in the construction of TMSs. Herein, the effects of anions on the creation of different types of TMSs is investigated for the first time. It is found that the active cobalt-nitrogen sites tend to be selectively constructed on the surface of N-doped carbon by using chloride, while metallic cobalt nanoparticles encased in protective graphite layers are the dominant forms of cobalt species with nitrate ions. The obtained catalysts demonstrate cobalt-sites-dependent activity for ORR and HER in acidic media. And the remarkably enhanced catalytic activities approaching that of benchmark Pt/C in acidic medium has been obtained on the catalyst dominated with cobalt-nitrogen sites, confirmed by the advanced spectroscopic . Our finding demonstrates a general paradigm of anion-regulated evolution of distinctive TMSs, providing a new pathway for enhancing performances of various targeted reactions related with TMSs.

Authors:
 [1];  [2];  [1];  [1];  [1];  [3];  [3];  [4]; ORCiD logo [4]
  1. State Key Laboratory of High Performance Ceramics and Superfine Microstructures, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding-xi Road Shanghai 200050 P. R. China; University of Chinese Academy of Sciences, Beijing 100049 P. R. China
  2. Chemical Science and Engineering Division, Argonne National Laboratory, 9700 Cass Avenue Lemont IL 60439 USA
  3. X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, 9700 Cass Avenue Lemont IL 60439 USA
  4. State Key Laboratory of High Performance Ceramics and Superfine Microstructures, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding-xi Road Shanghai 200050 P. R. China
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Key Basic Research Program of China; USDOE
OSTI Identifier:
1416001
DOE Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article
Resource Relation:
Journal Name: Advanced Materials; Journal Volume: 29; Journal Issue: 47
Country of Publication:
United States
Language:
English
Subject:
anions; cobalt-sites-dependent activities; electrocatalysis; selective generation; transition metal sites

Citation Formats

Wan, Gang, Yang, Ce, Zhao, Wanpeng, Li, Qianru, Wang, Ning, Li, Tao, Zhou, Hua, Chen, Hangrong, and Shi, Jianlin. Anion-Regulated Selective Generation of Cobalt Sites in Carbon: Toward Superior Bifunctional Electrocatalysis. United States: N. p., 2017. Web. doi:10.1002/adma.201703436.
Wan, Gang, Yang, Ce, Zhao, Wanpeng, Li, Qianru, Wang, Ning, Li, Tao, Zhou, Hua, Chen, Hangrong, & Shi, Jianlin. Anion-Regulated Selective Generation of Cobalt Sites in Carbon: Toward Superior Bifunctional Electrocatalysis. United States. doi:10.1002/adma.201703436.
Wan, Gang, Yang, Ce, Zhao, Wanpeng, Li, Qianru, Wang, Ning, Li, Tao, Zhou, Hua, Chen, Hangrong, and Shi, Jianlin. Mon . "Anion-Regulated Selective Generation of Cobalt Sites in Carbon: Toward Superior Bifunctional Electrocatalysis". United States. doi:10.1002/adma.201703436.
@article{osti_1416001,
title = {Anion-Regulated Selective Generation of Cobalt Sites in Carbon: Toward Superior Bifunctional Electrocatalysis},
author = {Wan, Gang and Yang, Ce and Zhao, Wanpeng and Li, Qianru and Wang, Ning and Li, Tao and Zhou, Hua and Chen, Hangrong and Shi, Jianlin},
abstractNote = {The introduction of active transition metal sites (TMSs) in carbon enables the synthesis of noble-metal-free electrocatalysts for clean energy conversion applications, however, there are often multiple existing forms of TMSs, which are of different natures and catalytic models. Regulating the evolution of distinctive TMSs is highly desirable but remains challenging to date. Anions, as essential elements involved in the synthesis, have been totally neglected previously in the construction of TMSs. Herein, the effects of anions on the creation of different types of TMSs is investigated for the first time. It is found that the active cobalt-nitrogen sites tend to be selectively constructed on the surface of N-doped carbon by using chloride, while metallic cobalt nanoparticles encased in protective graphite layers are the dominant forms of cobalt species with nitrate ions. The obtained catalysts demonstrate cobalt-sites-dependent activity for ORR and HER in acidic media. And the remarkably enhanced catalytic activities approaching that of benchmark Pt/C in acidic medium has been obtained on the catalyst dominated with cobalt-nitrogen sites, confirmed by the advanced spectroscopic . Our finding demonstrates a general paradigm of anion-regulated evolution of distinctive TMSs, providing a new pathway for enhancing performances of various targeted reactions related with TMSs.},
doi = {10.1002/adma.201703436},
journal = {Advanced Materials},
number = 47,
volume = 29,
place = {United States},
year = {Mon Nov 06 00:00:00 EST 2017},
month = {Mon Nov 06 00:00:00 EST 2017}
}