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题名: Peculiar hydrogenation reactivity of Ni-Ni delta+ clusters stabilized by ceria in reducing nitrobenzene to azoxybenzene
作者: 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
发表日期: 2017-09-01
DOI: 10.1016/j.jcat.2017.07.004
卷: 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
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.
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
语种: 英语
WOS记录号: WOS:000410468300013
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/150029
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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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

Recommended Citation:
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.
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