Fe Isolated Single Atoms on S, N Codoped Carbon by Copolymer Pyrolysis Strategy for Highly Efficient Oxygen Reduction Reaction

doi:10.1002/adma.201800588

	Fe Isolated Single Atoms on S, N Codoped Carbon by Copolymer Pyrolysis Strategy for Highly Efficient Oxygen Reduction Reaction
	Fu, NH; Gu, L; Zhuang, ZB; Chen, C; Wang, DS; Xiao, H; Chen, WX; Li, QH; Li, J; Gong, Y
刊名	ADVANCED MATERIALS
	2018
卷号	30 期号:25 页码:1800588
关键词	copolymer pyrolysis Fe-isolated single atoms oxygen reduction reaction sulfur-nitrogen codoped carbon
ISSN号	0935-9648
DOI	10.1002/adma.201800588
文献子类	Article
英文摘要	Heteroatom-doped Fe-NC catalyst has emerged as one of the most promising candidates to replace noble metal-based catalysts for highly efficient oxygen reduction reaction (ORR). However, delicate controls over their structure parameters to optimize the catalytic efficiency and molecular-level understandings of the catalytic mechanism are still challenging. Herein, a novel pyrrole-thiophene copolymer pyrolysis strategy to synthesize Fe-isolated single atoms on sulfur and nitrogen-codoped carbon (Fe-ISA/SNC) with controllable S, N doping is rationally designed. The catalytic efficiency of Fe-ISA/SNC shows a volcano-type curve with the increase of sulfur doping. The optimized Fe-ISA/SNC exhibits a half-wave potential of 0.896 V (vs reversible hydrogen electrode (RHE)), which is more positive than those of Fe-isolated single atoms on nitrogen codoped carbon (Fe-ISA/NC, 0.839 V), commercial Pt/C (0.841 V), and most reported nonprecious metal catalysts. Fe-ISA/SNC is methanol tolerable and shows negligible activity decay in alkaline condition during 15 000 voltage cycles. X-ray absorption fine structure analysis and density functional theory calculations reveal that the incorporated sulfur engineers the charges on N atoms surrounding the Fe reactive center. The enriched charge facilitates the rate-limiting reductive release of OH* and therefore improved the overall ORR efficiency.
电子版国际标准刊号	1521-4095
WOS关键词	FUEL-CELLS ; PARTICLE-SIZE ; ACIDIC MEDIA ; CATALYSTS ; IRON ; ELECTROCATALYSTS ; PERFORMANCE ; NITROGEN ; SULFUR ; OXIDATION
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
语种	英语
WOS记录号	WOS:000435258600025
内容类型	期刊论文
源URL	[http://ir.ihep.ac.cn/handle/311005/286029]
专题	高能物理研究所_多学科研究中心高能物理研究所_实验物理中心
作者单位	中国科学院高能物理研究所
推荐引用方式 GB/T 7714	Fu, NH,Gu, L,Zhuang, ZB,et al. Fe Isolated Single Atoms on S, N Codoped Carbon by Copolymer Pyrolysis Strategy for Highly Efficient Oxygen Reduction Reaction[J]. ADVANCED MATERIALS,2018,30(25):1800588.
APA	Fu, NH.,Gu, L.,Zhuang, ZB.,Chen, C.,Wang, DS.,...&Peng, Q.(2018).Fe Isolated Single Atoms on S, N Codoped Carbon by Copolymer Pyrolysis Strategy for Highly Efficient Oxygen Reduction Reaction.ADVANCED MATERIALS,30(25),1800588.
MLA	Fu, NH,et al."Fe Isolated Single Atoms on S, N Codoped Carbon by Copolymer Pyrolysis Strategy for Highly Efficient Oxygen Reduction Reaction".ADVANCED MATERIALS 30.25(2018):1800588.