Breaking scaling relations to achieve low-temperature ammonia synthesis through LiH-mediated nitrogen transfer and hydrogenation

doi:10.1038/NCHEM.2595

	Breaking scaling relations to achieve low-temperature ammonia synthesis through LiH-mediated nitrogen transfer and hydrogenation
	Wang, Peikun 1,2; Chang, Fei 1,2; Gao, Wenbo 1,2; Guo, Jianping 1; Wu, Guotao 1; He, Teng 1; Chen, Ping 1,3,4
刊名	NATURE CHEMISTRY
	2017
卷号	9 期号:1 页码:64-70
ISSN号	1755-4330
DOI	10.1038/NCHEM.2595
文献子类	Article
英文摘要	Ammonia synthesis under mild conditions is a goal that has been long sought after. Previous investigations have shown that adsorption and transition-state energies of intermediates in this process on transition metals (TMs) scale with each other. This prevents the independent optimization of these energies that would result in the ideal catalyst: one that activates reactants well, but binds intermediates relatively weakly. Here we demonstrate that these scaling relations can be broken by intervening in the TM-mediated catalysis with a second catalytic site, LiH. The negatively charged hydrogen atoms of LiH act as strong reducing agents, which remove activated nitrogen atoms from the TM or its nitride (TMN), and as an immediate source of hydrogen, which binds nitrogen atoms to form LiNH2. LiNH2 further splits H-2 heterolytically to give off NH3 and regenerate LiH. This synergy between TM (or TMN) and LiH creates a favourable pathway that allows both early and late 3d TM-LiH composites to exhibit unprecedented lower-temperature catalytic activities.
WOS关键词	BIMETALLIC NITRIDE CATALYSTS ; DINITROGEN CLEAVAGE ; RUTHENIUM CATALYSTS ; LITHIUM HYDRIDE ; METAL NITRIDES ; REDUCTION ; COMPLEX ; MECHANISM ; KINETICS ; DECOMPOSITION
WOS研究方向	Chemistry
语种	英语
出版者	NATURE PUBLISHING GROUP
WOS记录号	WOS:000394540400014
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/169652]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Guo, Jianping; Chen, Ping
作者单位	1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China 4.Collaborat Innovat Ctr Chem Energy Mat, Dalian 116023, Peoples R China
推荐引用方式 GB/T 7714	Wang, Peikun,Chang, Fei,Gao, Wenbo,et al. Breaking scaling relations to achieve low-temperature ammonia synthesis through LiH-mediated nitrogen transfer and hydrogenation[J]. NATURE CHEMISTRY,2017,9(1):64-70.
APA	Wang, Peikun.,Chang, Fei.,Gao, Wenbo.,Guo, Jianping.,Wu, Guotao.,...&Chen, Ping.(2017).Breaking scaling relations to achieve low-temperature ammonia synthesis through LiH-mediated nitrogen transfer and hydrogenation.NATURE CHEMISTRY,9(1),64-70.
MLA	Wang, Peikun,et al."Breaking scaling relations to achieve low-temperature ammonia synthesis through LiH-mediated nitrogen transfer and hydrogenation".NATURE CHEMISTRY 9.1(2017):64-70.