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Peculiar hydrogenation reactivity of Ni-Ni delta+ clusters stabilized by ceria in reducing nitrobenzene to azoxybenzene
Hou, Tingting1,2; Wang, Yehong1; Zhang, Jian1; Li, Mingrun1; Lu, Jianmin1; Heggen, Marc3,4; Sievers, Carsten5; Wang, Feng1
关键词Ceria N-ni Delta++ Clusters Heterogeneous Catalysis Supported Catalyst Nitrobenzene Reduction
刊名JOURNAL OF CATALYSIS
2017-09-01
DOI10.1016/j.jcat.2017.07.004
353页:107-115
收录类别SCI
文章类型Article
WOS标题词Science & Technology ; Physical Sciences ; Technology
类目[WOS]Chemistry, Physical ; Engineering, Chemical
研究领域[WOS]Chemistry ; Engineering
关键词[WOS]SUPPORTED NICKEL NANOPARTICLES ; TOTAL-ENERGY CALCULATIONS ; LIQUID-PHASE OXIDATION ; WAVE BASIS-SET ; SELECTIVE HYDROGENATION ; GOLD NANOPARTICLES ; SECONDARY ALCOHOLS ; ALUMINA SUPPORTS ; CO HYDROGENATION ; CATALYSTS
英文摘要In many catalytic processes, metastable reaction intermediates are more valuable and desirable than final products. Here, we report Ni-Ni delta+ clusters on ceria where the extent of reduction of nickel oxide/ceria in H-2 has been optimized. This catalyst shows high selectivity in reducing nitrobenzene to azoxybenzene, the latter usually being metastable. Due to strong electronic metal support interactions between Ni and ceria, mixed Ni-Ni delta+ clusters are formed on ceria even after reduction at 500 degrees C in hydrogen. The Ni-Ni delta+ clusters are highly dispersed on ceria, as observed by high-angle annular dark-field scanning transmission electron microscopy and energy-dispersive X-ray spectroscopy element mapping. This structural uniqueness is clearly reflected in the inhibition of azoxybenzene hydrogenation to aniline, and therefore the catalyst shows high azoxybenzene selectivity (92%). In comparison, the Ni metal catalyst mostly gives aniline and the NiO catalyst has low activity. This study shows how to steer catalytic reactions toward metastable intermediate products by tuning the extent of reduction of metal oxides deposited on reducible oxides. (C) 2017 Elsevier Inc. All rights reserved.
语种英语
WOS记录号WOS:000410468300013
引用统计
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/150029
专题中国科学院大连化学物理研究所
作者单位1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, State Key Lab Catalysis, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Forschungszentrum Julich, Ernst Ruska Ctr Microscopy & Spect Electrons, D-52425 Julich, Germany
4.Forschungszentrum Julich, Peter Grunberg Inst, D-52425 Julich, Germany
5.Georgia Inst Technol, Sch Chem & Biomol Engn, 311 Ferst Dr NW, Atlanta, GA 30332 USA
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Hou, Tingting,Wang, Yehong,Zhang, Jian,et al. Peculiar hydrogenation reactivity of Ni-Ni delta+ clusters stabilized by ceria in reducing nitrobenzene to azoxybenzene[J]. JOURNAL OF CATALYSIS,2017,353:107-115.
APA Hou, Tingting.,Wang, Yehong.,Zhang, Jian.,Li, Mingrun.,Lu, Jianmin.,...&Wang, Feng.(2017).Peculiar hydrogenation reactivity of Ni-Ni delta+ clusters stabilized by ceria in reducing nitrobenzene to azoxybenzene.JOURNAL OF CATALYSIS,353,107-115.
MLA Hou, Tingting,et al."Peculiar hydrogenation reactivity of Ni-Ni delta+ clusters stabilized by ceria in reducing nitrobenzene to azoxybenzene".JOURNAL OF CATALYSIS 353(2017):107-115.
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