Interplay Between Site Activity and Density of BCC Iron for Ammonia Synthesis Based on First-Principles Theory

doi:10.1002/cctc.201900175

	Interplay Between Site Activity and Density of BCC Iron for Ammonia Synthesis Based on First-Principles Theory
	Zhang, Bing-Yan 2,5; Su, Hai-Yan 3; Liu, Jin-Xun 1; Li, Wei-Xue 4
刊名	CHEMCATCHEM
	2019-04-04
卷号	11 期号:7 页码:1928-1934
关键词	Heterogeneous Catalysis Density Functional Calculations Iron Kinetics Ammonia synthesis
ISSN号	1867-3880
DOI	10.1002/cctc.201900175
通讯作者	Li, Wei-Xue(wxli70@ustc.edu.cn)
英文摘要	Site activity and density are two key factors in determining the overall activity of catalysts in heterogeneous catalysis. Combined DFT calculation, Wulff construction and micro-kinetic analysis, we reveal here a significant interplay between site activity and density of bcc iron catalyzed ammonia synthesis at low coverage regime. It is found that for large size particles, Fe (111) and (311) surfaces that consist of active C7 sites are limited by their low site density, whereas those with the most abundant sites are limited by their low activity. In contrast, Fe (221), (211) and (310) surfaces which consist of active C7 and/or B5 sites and remain abundant, dominate the overall reaction rate, turn-over-frequency and mass specific activity. Turn-over-frequency of the smaller Fe particles (2-6 nm) decreases by a factor of two or three due to the absence of (221) surface. For the particle size less than 2 nm, the corresponding activity decreases dramatically owing to the absence of all active C7 and/or B5 sites. Interplay of site abundance and intrinsic activity of catalysts is highlighted, and the insights revealed could be used to design and develop better catalysts for ammonia synthesis and other important reactions of technological interest.
资助项目	National Key R&D Program of China[2018YFA0208603] ; National Key R&D Program of China[2017YFB0602205] ; National Key R&D Program of China[2017YFA0204800] ; Chinese Academy of Sciences[QYZDJ-SSW-SLH054] ; Natural Science Foundation of China[91645202] ; Natural Science Foundation of China[21872136]
WOS关键词	EVANS-POLANYI RELATION ; STRUCTURE SENSITIVITY ; RUTHENIUM CATALYSTS ; MAGNETIC-PROPERTIES ; TRANSITION-METAL ; VOLCANO CURVE ; SURFACE ; NITROGEN ; CRYSTAL ; ADSORPTION
WOS研究方向	Chemistry
语种	英语
出版者	WILEY-V C H VERLAG GMBH
WOS记录号	WOS:000466791200011
资助机构	National Key R&D Program of China ; National Key R&D Program of China ; Chinese Academy of Sciences ; Chinese Academy of Sciences ; Natural Science Foundation of China ; Natural Science Foundation of China ; National Key R&D Program of China ; National Key R&D Program of China ; Chinese Academy of Sciences ; Chinese Academy of Sciences ; Natural Science Foundation of China ; Natural Science Foundation of China ; National Key R&D Program of China ; National Key R&D Program of China ; Chinese Academy of Sciences ; Chinese Academy of Sciences ; Natural Science Foundation of China ; Natural Science Foundation of China ; National Key R&D Program of China ; National Key R&D Program of China ; Chinese Academy of Sciences ; Chinese Academy of Sciences ; Natural Science Foundation of China ; Natural Science Foundation of China
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/165466]
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	Li, Wei-Xue
作者单位	1.Univ Michigan, Dept Chem Engn, Ann Arbor, MI 48109 USA 2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China 3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China 4.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Dept Chem Phys, Hefei 230026, Anhui, Peoples R China 5.Univ Chinese Acad Sci, Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式 GB/T 7714	Zhang, Bing-Yan,Su, Hai-Yan,Liu, Jin-Xun,et al. Interplay Between Site Activity and Density of BCC Iron for Ammonia Synthesis Based on First-Principles Theory[J]. CHEMCATCHEM,2019,11(7):1928-1934.
APA	Zhang, Bing-Yan,Su, Hai-Yan,Liu, Jin-Xun,&Li, Wei-Xue.(2019).Interplay Between Site Activity and Density of BCC Iron for Ammonia Synthesis Based on First-Principles Theory.CHEMCATCHEM,11(7),1928-1934.
MLA	Zhang, Bing-Yan,et al."Interplay Between Site Activity and Density of BCC Iron for Ammonia Synthesis Based on First-Principles Theory".CHEMCATCHEM 11.7(2019):1928-1934.