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Influence of Cobalt Crystal Structures on Activation of Nitrogen Molecule: A First-Principles Study
Zhang, Bing-Yan1,6; Chen, Pei-Pei1,6; Liu, Jin-Xun3; Su, Hai-Yan2; Li, Wei-Xue4,5
Corresponding AuthorLiu, Jin-Xun(jinxun@umich.edu) ; Li, Wei-Xue(wxli70@ustc.edu.cn)
Source PublicationJOURNAL OF PHYSICAL CHEMISTRY C
2019-05-02
ISSN1932-7447
DOI10.1021/acs.jpcc.9b00590
Volume123Issue:17Pages:10956-10966
Funding ProjectNational 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]
Funding OrganizationNational 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
WOS SubjectChemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS Research AreaChemistry ; Science & Technology - Other Topics ; Materials Science
WOS KeywordEVANS-POLANYI RELATION ; AMMONIA-SYNTHESIS ; CO ACTIVATION ; RUTHENIUM CATALYSTS ; EFFICIENT CATALYST ; MORPHOLOGY CHANGES ; PARTICLE-SIZE ; SURFACE ; DECOMPOSITION ; REDUCTION
AbstractIdentification 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.
Language英语
Funding OrganizationNational 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
WOS IDWOS:000466988600027
PublisherAMER CHEMICAL SOC
Citation statistics
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/165491
Collection中国科学院大连化学物理研究所
Corresponding AuthorLiu, Jin-Xun; Li, Wei-Xue
Affiliation1.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
Recommended Citation
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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