Computational Screening of Single Atoms Anchored on Defective Mo2CO2 MXene Nanosheet as Efficient Electrocatalysts for the Synthesis of Ammonia

doi:10.1002/adem.202100405

CORC > 力学研究所 > 中国科学院力学研究所 > 高温气体动力学国家重点实验室

	Computational Screening of Single Atoms Anchored on Defective Mo2CO2 MXene Nanosheet as Efficient Electrocatalysts for the Synthesis of Ammonia
	Wang, Shuo 7; Li, Lei 6; San Hui, Kwan 5; Bin F(宾峰)4; Zhou, Wei 3; Fan, Xi 2; Zalnezhad, E.1; Li, Jing 7; Hui, Kwun Nam 7
刊名	ADVANCED ENGINEERING MATERIALS
	2021-07-22
页码	8
关键词	density functional theory calculations electrocatalysis MXene nitrogen reduction reaction single-atom catalysts
ISSN号	1438-1656
DOI	10.1002/adem.202100405
通讯作者	Li, Lei(uestclilei@163.com) ; San Hui, Kwan(k.hui@uea.ac.uk) ; Li, Jing(victor_li_glv@hotmail.com) ; Hui, Kwun Nam(bizhui@um.edu.mo)
英文摘要	The electrochemical nitrogen reduction reaction (NRR) over single-atom catalysts (SACs) anchored on Mo vacancies of Mo2CO2 MXene nanosheets under ambient conditions suffers from poor selectivity, low yield, and low Faradaic efficiency because of their sluggish kinetics and the competing hydrogen evolution reaction. Herein, density functional theory calculations are performed to improve the understanding of the selectivity and yielding of ammonia through NRR over various isolated SACs, that is, from Sc to Au, anchored on the Mo vacancy of the Mo2CO2 MXene nanosheet (denoted as MO2CO2-M-SA). The potential-determining step of the NRR shows that eight candidates (i.e., Y, Zr, Nb, Hf, Ta, W, Re, and Os) confined on the defective Mo2CO2 layer could promote the electroreduction from N-2 to NH3. Among these, Mo2CO2-Y-SA presented the lowest reported reaction Presents the lowest reported reaction energy barrier (0.08 eV) through the distal pathway and high selectivity to NRR compared with the previously synthesized Mo2CO2-Ru-SA with a relatively high energy barrier (0.65 eV) and poor selectivity. In addition, the formation energy of Mo2CO2-Y-SA is more negative than that of the Mo2CO2-Ru-SA catalyst, suggesting that the experimental preparation of the Mo2CO2-Y-SA catalyst is highly feasible. This work lays a solid foundation for improving the rational design of MXene-based systems as efficient electrocatalysts for the synthesis of ammonia.
分类号	二类
资助项目	Science and Technology Development Fund, Macau SAR[0191/2017/A3] ; Science and Technology Development Fund, Macau SAR[0041/2019/A1] ; Science and Technology Development Fund, Macau SAR[0046/2019/AFJ] ; Science and Technology Development Fund, Macau SAR[0021/2019/AIR] ; University of Macau[MYRG2017-00216-FST] ; University of Macau[MYRG2018-00192-IAPME] ; UEA ; Biomechacin, Texas, USA[BMC200101]
WOS关键词	HYDROGEN EVOLUTION REACTION ; NITROGEN REDUCTION ; N-2 FIXATION ; CATALYSTS ; MONOLAYER ; NITRIDE
WOS研究方向	Materials Science
语种	英语
WOS记录号	WOS:000675530700001
资助机构	Science and Technology Development Fund, Macau SAR ; University of Macau ; UEA ; Biomechacin, Texas, USA
其他责任者	Li, Lei ; San Hui, Kwan ; Li, Jing ; Hui, Kwun Nam
内容类型	期刊论文
源URL	[http://dspace.imech.ac.cn/handle/311007/87064]
专题	力学研究所_高温气体动力学国家重点实验室
作者单位	1.Univ Texas San Antonio, Dept Chem & Biomed Engn, San Antonio, TX USA 2.Chinese Acad Sci, Ningbo Inst Mat Technol, Engn, Ningbo 315201, Peoples R China; 3.Xiamen Univ, Dept Mech & Elect Engn, Xiamen 361005, Peoples R China; 4.Chinese Acad Sci, Inst Mech, State Key Lab High Temp Gas Dynam, Beijing 100190, Peoples R China; 5.Univ East Anglia, Fac Sci, Sch Engn, Norwich NR4 7TJ, Norfolk, England; 6.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Collaborat Innovat Ctr Chem Energy Mat, Hefei 230026, Peoples R China; 7.Univ Macau, Inst Appl Phys & Mat Engn, Minist Educ, Joint Key Lab, Ave Univ, Taipa, Macau, Peoples R China;
推荐引用方式 GB/T 7714	Wang, Shuo,Li, Lei,San Hui, Kwan,et al. Computational Screening of Single Atoms Anchored on Defective Mo2CO2 MXene Nanosheet as Efficient Electrocatalysts for the Synthesis of Ammonia[J]. ADVANCED ENGINEERING MATERIALS,2021:8.
APA	Wang, Shuo.,Li, Lei.,San Hui, Kwan.,宾峰.,Zhou, Wei.,...&Hui, Kwun Nam.(2021).Computational Screening of Single Atoms Anchored on Defective Mo2CO2 MXene Nanosheet as Efficient Electrocatalysts for the Synthesis of Ammonia.ADVANCED ENGINEERING MATERIALS,8.
MLA	Wang, Shuo,et al."Computational Screening of Single Atoms Anchored on Defective Mo2CO2 MXene Nanosheet as Efficient Electrocatalysts for the Synthesis of Ammonia".ADVANCED ENGINEERING MATERIALS (2021):8.