APM OpenIR
Reactivity descriptors of diverse copper-oxo species on ZSM-5 zeolite towards methane activation
Wang, Guiru1,2; Chen, Wei1,2; Huang, Ling1; Liu, Zhiqiang1; Sun, Xianyong1; Zheng, Anmin1,3
2019-11-01
Source PublicationCATALYSIS TODAY
ISSN0920-5861
Volume338Pages:108-116
AbstractCopper-containing ZSM-5 zeolite can facilitate the direct oxidation of methane to form methanol under mild condition with high selectivity. However, due to the limitation of the experimental characterization, the identification of the catalytic sites in Cu-exchanged zeolites still remains unclear. Herein, the reactivity of different [CuxOy] (x = 1, 2, 3; y = 1, 2, 3)- and [CuOH](+)-ZSM-5 active sites towards methane partial oxidation process has been elucidated by using density functional theory (DFT) calculations. It is indicated that i) C-H activation over five different active sites obeys the radical mechanism, and the reactivity follows the sequence: copper-oxyl [CuO](+) (S = 1) > tricopper [Cu3O3](2+) (S = 3/2) > bis-(mu-oxo)-dicopper [Cu2O2](2+) (S = 1) > mono-(mu-oxo)-dicopper [CuOCu](2+) (S = 1) > mono-copper [CuOH](1)(+) (S = 1/2); ii) The rate constants for C-H bond cleavage of methane at the reaction temperature are faster at the higher temperature; iii) The descriptors for C-H activation of methane on [CuxOy] (x = 1(similar to)3, y = 1 3)- and [CuOH](+)-ZSM-5 have been established, for which the active site with more spin density and less negative charge will induce the lower activation barriers for C-H activation of methane. Meanwhile, the stronger hydrogen affinity of the active site is, the lower the activation barriers of methane C-H activation will be. Taken the stability and activation barrier together, the catalytic performance of copper-oxyl site has been enhanced by the presence of water.
KeywordCu-oxo-species Zeolite Spin density Methane activation Descriptors
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Sinopec Corp. ; Sinopec Corp. ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Sinopec Corp. ; Sinopec Corp. ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Sinopec Corp. ; Sinopec Corp. ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Sinopec Corp. ; Sinopec Corp.
DOI10.1016/j.cattod.2019.05.007
WOS KeywordCOMBINED QUANTUM-MECHANICS ; GENERALIZED GRADIENT APPROXIMATION ; H BOND ACTIVATION ; DIRECT CONVERSION ; HYDROGEN-ATOM ; ACTIVE-SITE ; CATALYTIC CONVERSION ; MONONUCLEAR COPPER ; AB-INITIO ; OXIDATION
Language英语
Funding ProjectNational Natural Science Foundation of China[21522310] ; National Natural Science Foundation of China[21473244] ; National Natural Science Foundation of China[91645112] ; Natural Science Foundation of Hubei Province of China[2014CFA043] ; Key Research Program of Frontier Sciences, CAS[QYZDB-SSW-SLH026] ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase)[U1501501] ; Sinopec Corp.[417012-4]
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Sinopec Corp. ; Sinopec Corp. ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Sinopec Corp. ; Sinopec Corp. ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Sinopec Corp. ; Sinopec Corp. ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Natural Science Foundation of Hubei Province of China ; Natural Science Foundation of Hubei Province of China ; Key Research Program of Frontier Sciences, CAS ; Key Research Program of Frontier Sciences, CAS ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase) ; Sinopec Corp. ; Sinopec Corp.
WOS Research AreaChemistry ; Engineering
WOS SubjectChemistry, Applied ; Chemistry, Physical ; Engineering, Chemical
WOS IDWOS:000483921400012
PublisherELSEVIER
Citation statistics
Cited Times:4[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.apm.ac.cn/handle/112942/14869
Collection中国科学院武汉物理与数学研究所
Corresponding AuthorZheng, Anmin
Affiliation1.Chinese Acad Sci, Wuhan Inst Phys & Math, State Key Lab Magnet Resonance & Atom & Mol Phys, Natl Ctr Magnet Resonance,Wuhan Key Lab Magnet Re, Wuhan 430071, Hubei, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Huazhong Univ Sci & Technol, Wuhan Natl Lab Optoelect, Wuhan 430074, Hubei, Peoples R China
Recommended Citation
GB/T 7714
Wang, Guiru,Chen, Wei,Huang, Ling,et al. Reactivity descriptors of diverse copper-oxo species on ZSM-5 zeolite towards methane activation[J]. CATALYSIS TODAY,2019,338:108-116.
APA Wang, Guiru,Chen, Wei,Huang, Ling,Liu, Zhiqiang,Sun, Xianyong,&Zheng, Anmin.(2019).Reactivity descriptors of diverse copper-oxo species on ZSM-5 zeolite towards methane activation.CATALYSIS TODAY,338,108-116.
MLA Wang, Guiru,et al."Reactivity descriptors of diverse copper-oxo species on ZSM-5 zeolite towards methane activation".CATALYSIS TODAY 338(2019):108-116.
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