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Insights into Interfacial Synergistic Catalysis over Ni@TiO2-x Catalyst toward Water-Gas Shift Reaction
Xu, Ming1; Yao, Siyu2,3; Rao, Deming1; Niu, Yiming4; Liu, Ning1; Peng, Mi2,3; Zhai, Peng2,3; Man, Yi; Zheng, Lirong6; Wang, Bin5; Zhang, Bingsen4; Ma, Ding2,3; Wei, Min1
Corresponding AuthorWang, Bin(wangbin.bjhy@sinopec.com) ; Zhang, Bingsen(bszhang@imr.ac.cn) ; Ma, Ding(dma@pku.edu.cn) ; Wei, Min(weimin@mail.buct.edu.cn)
2018-09-12
Source PublicationJOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN0002-7863
Volume140Issue:36Pages:11241-11251
AbstractThe mechanism on interfacial synergistic catalysis for supported metal catalysts has long been explored and investigated in several important heterogeneous catalytic processes (e.g., water-gas shift (WGS) reaction). The modulation of metal-support interactions imposes a substantial influence on activity and selectivity of catalytic reaction, as a result of the geometric/electronic structure of interfacial sites. Although great efforts have validated the key role of interfacial sites in WGS over metal catalysts supported on reducible oxides, direct evidence at the atomic level is lacking and the mechanism of interfacial synergistic catalysis is still ambiguous. Herein, Ni nanoparticles supported on TiO2-x (denoted as Ni@TiO2-x) were fabricated via a structure topotactic transformation of NiTi-layered double hydroxide (NiTi-LDHs) precursor, which showed excellent catalytic performance for WGS reaction. In situ microscopy was carried out to reveal the partially encapsulated structure of Ni@TiO2, catalyst. A combination study including in situ and operando EXAFS, in situ DRIFTS spectra combined with TPSR measurements substantiates a new redox mechanism based on interfacial synergistic catalysis. Notably, interfacial Ni species (electron -enriched Ni delta- site) participates in the dissociation of H2O molecule to generate H-2, accompanied by the oxidation of Ni delta--O-v-Ti3+ (O-v: oxygen vacancy) to Ni delta+-O-Ti4+ structure. Density functional theory calculations further verify that the interfacial sites of Ni@ TiO2-x catalyst serve as the optimal active site with the lowest activation energy barrier (similar to 0.35 eV) for water dissociation. This work provides a fundamental understanding on interfacial synergistic catalysis toward WGS reaction, which is constructive for the rational design and fabrication of high activity heterogeneous catalysts.
Funding OrganizationNational Key RAMP;D Program of China ; National Natural Science Foundation of China ; Fundamental Research Funds for the Central Universities
DOI10.1021/jacs.8b03117
Indexed BySCI
Language英语
Funding ProjectNational Key RAMP;D Program of China[2017YFA0206804] ; National Key RAMP;D Program of China[2017YFB0602200] ; National Natural Science Foundation of China[NSFC: 21521005] ; National Natural Science Foundation of China[21725301] ; National Natural Science Foundation of China[91645115] ; National Natural Science Foundation of China[21473003] ; National Natural Science Foundation of China[91545119] ; Fundamental Research Funds for the Central Universities[buctylkxj01]
WOS Research AreaChemistry
WOS SubjectChemistry, Multidisciplinary
WOS IDWOS:000444793400021
PublisherAMER CHEMICAL SOC
Citation statistics
Cited Times:70[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/129466
Collection中国科学院金属研究所
Corresponding AuthorWang, Bin; Zhang, Bingsen; Ma, Ding; Wei, Min
Affiliation1.Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
2.Peking Univ, Coll Chem & Mol Engn, BIC ESAT, Beijing 100871, Peoples R China
3.Peking Univ, Coll Engn, BIC ESAT, Beijing 100871, Peoples R China
4.Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Liaoning, Peoples R China
5.Sinopec Grp, Beijing Res Inst Chem Ind, Beijing 100013, Peoples R China
6.Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China
Recommended Citation
GB/T 7714
Xu, Ming,Yao, Siyu,Rao, Deming,et al. Insights into Interfacial Synergistic Catalysis over Ni@TiO2-x Catalyst toward Water-Gas Shift Reaction[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2018,140(36):11241-11251.
APA Xu, Ming.,Yao, Siyu.,Rao, Deming.,Niu, Yiming.,Liu, Ning.,...&Wei, Min.(2018).Insights into Interfacial Synergistic Catalysis over Ni@TiO2-x Catalyst toward Water-Gas Shift Reaction.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,140(36),11241-11251.
MLA Xu, Ming,et al."Insights into Interfacial Synergistic Catalysis over Ni@TiO2-x Catalyst toward Water-Gas Shift Reaction".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 140.36(2018):11241-11251.
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