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, M; Yao, SY; Rao, DM; Niu, YM; Liu, N; Peng, M; Zhai, P; Man, Y; Zheng, LR ; Wang, B
|
| 刊名 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
 |
| 出版日期 | 2018 |
| 卷号 | 140期号:36页码:11241-11251 |
| ISSN号 | 0002-7863 |
| DOI | 10.1021/jacs.8b03117 |
| 文献子类 | Article |
| 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. |
| WOS关键词 | GENERALIZED GRADIENT APPROXIMATION ; METAL-SUPPORT INTERACTION ; IN-SITU ; CO OXIDATION ; CERIA NANOPARTICLES ; AMBIENT-PRESSURE ; AU NANOPARTICLES ; CHARGE-TRANSFER ; OXIDE CATALYST ; TEMPERATURE |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| WOS记录号 | WOS:000444793400021 |
| 源URL | [http://ir.ihep.ac.cn/handle/311005/286341]  |
| 专题 | 高能物理研究所_多学科研究中心 |
| 作者单位 | 中国科学院高能物理研究所 |
| 推荐引用方式 GB/T 7714 | Xu, M,Yao, SY,Rao, DM,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, M.,Yao, SY.,Rao, DM.,Niu, YM.,Liu, N.,...&郑黎荣.(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, M,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. |
入库方式： OAI收割
来源：高能物理研究所
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