Anion-Regulated Selective Generation of Cobalt Sites in Carbon: Toward Superior Bifunctional Electrocatalysis
Abstract
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 are 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 oxygen reduction reaction and hydrogen evolution reaction in acidic media. The remarkably enhanced catalytic activities approaching that of benchmark Pt/C in an acidic medium have been obtained on the catalyst dominated with cobalt–nitrogen sites, confirmed by the advanced spectroscopic characterization. This finding demonstrates a general paradigm of anion‐regulated evolution of distinctive TMSs, providing a new pathway for enhancing performances of various targetedmore »
- Authors:
-
[3]
- Chinese Academy of Sciences, Shanghai (China); University of Chinese Academy of Sciences, Beijing (China)
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Chinese Academy of Sciences, Shanghai (China)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE; National Key Basic Research Program of China
- OSTI Identifier:
- 1416001
- Alternate Identifier(s):
- OSTI ID: 1407824
- Grant/Contract Number:
- AC02-06CH11357; DE‐AC02‐06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Materials
- Additional Journal Information:
- Journal Volume: 29; Journal Issue: 47; Journal ID: ISSN 0935-9648
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 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. https://doi.org/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. https://doi.org/10.1002/adma.201703436. https://www.osti.gov/servlets/purl/1416001.
@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 = {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 are 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 oxygen reduction reaction and hydrogen evolution reaction in acidic media. The remarkably enhanced catalytic activities approaching that of benchmark Pt/C in an acidic medium have been obtained on the catalyst dominated with cobalt–nitrogen sites, confirmed by the advanced spectroscopic characterization. This 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 = {2017},
month = {11}
}
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Figures / Tables:
Figure 1: Illustration of anion-regulated selective generation of catalytic cobalt sites in carbon via pyrolysis with NO3- or Cl- anions for hydrogen evolution and oxygen reduction in acidic medium.
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