Nitrogen electroreduction performance of transition metal dimers embedded into N-doped graphene: a theoretical prediction

doi:10.1039/c9ta13599e

IMR OpenIR

	Nitrogen electroreduction performance of transition metal dimers embedded into N-doped graphene: a theoretical prediction
	Li, Hongyan 1; Zhao, Zhifeng 2; Cai, Qinghai 1; Yin, Lichang 3; Zhao, Jingxiang 1
通讯作者	Yin, Lichang(lcyin@imr.ac.cn) ; Zhao, Jingxiang(xjz_hmily@163.com)
	2020-02-28
发表期刊	JOURNAL OF MATERIALS CHEMISTRY A
ISSN	2050-7488
卷号	8 期号:8 页码:4533-4543
摘要	The electrocatalytic nitrogen reduction reaction (eNRR) under ambient conditions using sustainable energy sources is a fascinating approach for ammonia (NH3) production to replace the industrial Haber-Bosch process with enormous energy input and continuous CO2 emissions. However, the eNRR process remains a coveted goal due to the poor product selectivity, low activity, and stability of traditional catalysts. Inspired by recent experimental advances in dual-atom catalysts, herein, by means of comprehensive spin-polarized density functional theory (DFT) computations, the catalytic performance of various binary transition metals dispersed in nitrogen-doped porous graphene (NPG) for the eNRR was systematically evaluated. Our results revealed that the N atoms around vacancies in the substrate can strongly stabilize the metal dimers by forming metal-N bonds. Among FeFe, FeCo, FeNi, FeCu, FeRh, FeRu, FePd, MoFe, MoCo, MoCu, MoRu, and MoMo, the binary FeRh embedded in NPG was identified as the best catalyst due to its lowest limiting potential (-0.22 V) and high selectivity towards the eNRR. Our results further suggested that the good eNRR catalytic activity of the dispersed FeRh mainly originates from its optimal eNRR intermediates' adsorption/desorption features, obvious suppressing effects on the hydrogen evolution reaction, and great promise for synthesis. Our work not only opens a new door to advance sustainable NH3 production by tailoring the electronic structures of binuclear metal atoms, but also provides deeper insight into the structure-performance relationships of dual sites for eNRR electrocatalysts.
资助者	Natural Science Funds for Distinguished Young Scholar of Heilongjiang Province ; National Natural Science Foundation of China ; Project of Introducing Talent of Guangdong University of Petrochemical Technology
DOI	10.1039/c9ta13599e
收录类别	SCI
语种	英语
资助项目	Natural Science Funds for Distinguished Young Scholar of Heilongjiang Province[JC2018004] ; National Natural Science Foundation of China[51972312] ; National Natural Science Foundation of China[51472249] ; Project of Introducing Talent of Guangdong University of Petrochemical Technology[519614] ; Project of Introducing Talent of Guangdong University of Petrochemical Technology[519162]
WOS研究方向	Chemistry ; Energy & Fuels ; Materials Science
WOS类目	Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
WOS记录号	WOS:000519704200034
出版者	ROYAL SOC CHEMISTRY
引用统计	被引频次：141[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/137707
专题	中国科学院金属研究所
通讯作者	Yin, Lichang; Zhao, Jingxiang
作者单位	1.Harbin Normal Univ, Minist Educ, Coll Chem & Chem Engn, Key Lab Photon & Elect Bandgap Mat, Harbin 150025, Peoples R China 2.Guangdong Univ Petrochem Technol, Coll Chem, Maoming 525000, Peoples R China 3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
推荐引用方式 GB/T 7714	Li, Hongyan,Zhao, Zhifeng,Cai, Qinghai,et al. Nitrogen electroreduction performance of transition metal dimers embedded into N-doped graphene: a theoretical prediction[J]. JOURNAL OF MATERIALS CHEMISTRY A,2020,8(8):4533-4543.
APA	Li, Hongyan,Zhao, Zhifeng,Cai, Qinghai,Yin, Lichang,&Zhao, Jingxiang.(2020).Nitrogen electroreduction performance of transition metal dimers embedded into N-doped graphene: a theoretical prediction.JOURNAL OF MATERIALS CHEMISTRY A,8(8),4533-4543.
MLA	Li, Hongyan,et al."Nitrogen electroreduction performance of transition metal dimers embedded into N-doped graphene: a theoretical prediction".JOURNAL OF MATERIALS CHEMISTRY A 8.8(2020):4533-4543.