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Insights into Interfacial Synergistic Catalysis over Ni@TiO2-x Catalyst toward Water-Gas Shift Reaction

文献类型：期刊论文

作者Xu, Ming4; Yao, Siyu1,5; Rao, Deming4; Niu, Yiming6; Liu, Ning4; Peng, Mi1,5; Zhai, Peng1,5; Man, Yi; Zheng, Lirong3; Wang, Bin2
刊名JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
出版日期2018-09-12
卷号140期号:36页码:11241-11251
ISSN号0002-7863
DOI10.1021/jacs.8b03117
通讯作者Wang, Bin(wangbin.bjhy@sinopec.com) ; Zhang, Bingsen(bszhang@imr.ac.cn) ; Ma, Ding(dma@pku.edu.cn) ; Wei, Min(weimin@mail.buct.edu.cn)
英文摘要The 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.
资助项目National 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研究方向Chemistry
语种英语
出版者AMER CHEMICAL SOC
WOS记录号WOS:000444793400021
资助机构National Key RAMP;D Program of China ; National Natural Science Foundation of China ; Fundamental Research Funds for the Central Universities
源URL[http://ir.imr.ac.cn/handle/321006/129465]  
专题金属研究所_中国科学院金属研究所
通讯作者Wang, Bin; Zhang, Bingsen; Ma, Ding; Wei, Min
作者单位1.Peking Univ, Coll Engn, BIC ESAT, Beijing 100871, Peoples R China
2.Sinopec Grp, Beijing Res Inst Chem Ind, Beijing 100013, Peoples R China
3.Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China
4.Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
5.Peking Univ, Coll Chem & Mol Engn, BIC ESAT, Beijing 100871, Peoples R China
6.Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Liaoning, Peoples R China
推荐引用方式
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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来源：金属研究所

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