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Influence of Cobalt Crystal Structures on Activation of Nitrogen Molecule: A First-Principles Study

文献类型：期刊论文

作者Zhang, Bing-Yan1,6; Chen, Pei-Pei1,6; Liu, Jin-Xun3; Su, Hai-Yan2; Li, Wei-Xue4,5
刊名JOURNAL OF PHYSICAL CHEMISTRY C
出版日期2019-05-02
卷号123期号:17页码:10956-10966
ISSN号1932-7447
DOI10.1021/acs.jpcc.9b00590
通讯作者Liu, Jin-Xun(jinxun@umich.edu) ; Li, Wei-Xue(wxli70@ustc.edu.cn)
英文摘要Identification of the structure sensitivity of nitrogen molecule (N-2) activation and ammonia synthesis on metal surfaces is important for the mechanistic understanding and rational design of more efficient catalysts. In the present work, density functional theory calculations together with microkinetic simulations were performed to study the influence of cobalt crystal structures including hexagonal close-packed (HCP) and face-centered cubic (FCC) on nitrogen molecule dissociation and ammonia synthesis. Molecular and dissociative adsorption energies of N-2 as well as dissociation barriers are calculated for a total of ten cobalt surfaces. It is found that molecular adsorption energies on Co surfaces vary modestly on the order of 0.25 eV, whereas dissociative adsorption energies and the corresponding barriers vary considerably in magnitude by about 0.80 eV. First-principles microkinetic simulations show that HCP Co displays higher activity than FCC cobalt for nitrogen molecule dissociation and ammonia synthesis due to the higher intrinsic activity and density of active sites of HCP cobalt. Nitrogen molecule dissociation is the rate-determining step of ammonia synthesis due to the weak interaction between nitrogen and cobalt. The crystal phase sensitivity of nitrogen molecule dissociation on cobalt is compared with the dissociation of an isoelectronic molecule, carbon monoxide on cobalt, ruthenium, and nickel. This work provides valuable insights into nitrogen molecule dissociation and ammonia synthesis on cobalt catalysts with different crystal phases, and highlights the interplay between activated molecules and catalyst composition on the crystal phase sensitivity.
WOS关键词EVANS-POLANYI RELATION ; AMMONIA-SYNTHESIS ; CO ACTIVATION ; RUTHENIUM CATALYSTS ; EFFICIENT CATALYST ; MORPHOLOGY CHANGES ; PARTICLE-SIZE ; SURFACE ; DECOMPOSITION ; REDUCTION
资助项目National Key R&D Program of China[2017YFB0602205] ; National Key R&D Program of China[2018YFA0208603] ; Natural Science Foundation of China[91645202] ; Natural Science Foundation of China[21872136] ; Chinese Academy of Sciences[QYZDJ-SSW-SLH054]
WOS研究方向Chemistry ; Science & Technology - Other Topics ; Materials Science
语种英语
出版者AMER CHEMICAL SOC
WOS记录号WOS:000466988600027
资助机构National Key R&D Program of China ; National Key R&D Program of China ; Natural Science Foundation of China ; Natural Science Foundation of China ; Chinese Academy of Sciences ; Chinese Academy of Sciences ; National Key R&D Program of China ; National Key R&D Program of China ; Natural Science Foundation of China ; Natural Science Foundation of China ; Chinese Academy of Sciences ; Chinese Academy of Sciences ; National Key R&D Program of China ; National Key R&D Program of China ; Natural Science Foundation of China ; Natural Science Foundation of China ; Chinese Academy of Sciences ; Chinese Academy of Sciences ; National Key R&D Program of China ; National Key R&D Program of China ; Natural Science Foundation of China ; Natural Science Foundation of China ; Chinese Academy of Sciences ; Chinese Academy of Sciences
源URL[http://cas-ir.dicp.ac.cn/handle/321008/165490]  
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Liu, Jin-Xun; Li, Wei-Xue
作者单位1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China
3.Univ Michigan, Dept Chem Engn, Ann Arbor, MI 48109 USA
4.Univ Sci & Technol China, Sch Chem & Mat Sci, Dept Chem Phys, Hefei 230026, Anhui, Peoples R China
5.Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China
6.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式
GB/T 7714		 Zhang, Bing-Yan,Chen, Pei-Pei,Liu, Jin-Xun,et al. Influence of Cobalt Crystal Structures on Activation of Nitrogen Molecule: A First-Principles Study[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2019,123(17):10956-10966.
APA Zhang, Bing-Yan,Chen, Pei-Pei,Liu, Jin-Xun,Su, Hai-Yan,&Li, Wei-Xue.(2019).Influence of Cobalt Crystal Structures on Activation of Nitrogen Molecule: A First-Principles Study.JOURNAL OF PHYSICAL CHEMISTRY C,123(17),10956-10966.
MLA Zhang, Bing-Yan,et al."Influence of Cobalt Crystal Structures on Activation of Nitrogen Molecule: A First-Principles Study".JOURNAL OF PHYSICAL CHEMISTRY C 123.17(2019):10956-10966.

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来源：大连化学物理研究所

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