期刊
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
卷 164, 期 6, 页码 F645-F650出版社
ELECTROCHEMICAL SOC INC
DOI: 10.1149/2.1361706jes
关键词
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资金
- FAPESP (Fundacao de Amparo a Pesquisa do Estado de Sao Paulo) - Sao Paulo Research Foundation [2013/03408-0, 2014/11923-5, 2016/13323-0, 2013/16930-7]
- CNPq (Conselho Nacional de Desenvolvimento Cientifico e Tecnologico) [306469/2016-2, 306213/2013-3, 477153/2013-5]
- NSF [DGE-1650441]
- NSF MRSEC program [DMR-1120296]
- Fundacao de Amparo a Pesquisa do Estado de Sao Paulo (FAPESP) [16/13323-0, 13/03408-0] Funding Source: FAPESP
The development of active and stable oxygen reduction reaction (ORR) electrocatalysts using low-cost, abundant elements is of critical importance to the widespread adoption of proton-exchanged membrane fuel cells (PEMFCs). Tantalum-containing compounds, such as tantalum oxynitrides, can catalyze ORR in acid, with the degree of oxidation proposed to play a central role in controlling the ORR activity. Herein, we report the incorporation of aliovalent ions in tantalum oxynitrides (Ta-ON) and their effect on the ORR activity in acid. We synthesize Ta-ON by utilizing urea as the nitrogen source and use aliovalent (Ti4+) and isovalent (Nb5+) substitutions to evaluate the influence of the aliovalent substitution on the ORR activity. We found that an aliovalent Ti4+ substitution increases the ORR activity by 3x, which we attribute to improved electrical conductivity and increased ORR active sites. In comparison, isovalent Nb5+ substitution or carbon inclusion as oxycarbonitride did not positively affect the ORR activity. Our finding points to the important role of defects and conductivity in the Ta-based ORR electrocatalysts. (C) The Author(s) 2017. Published by ECS. All rights reserved.
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