Peculiar hydrogenation reactivity of Ni-Ni delta+ clusters stabilized by ceria in reducing nitrobenzene to azoxybenzene
Heggen, Marc3,4; Li, Mingrun1; Lu, Jianmin1; Zhang, Jian1; Wang, Yehong1; Hou, Tingting1,5; Wang, Feng1; Sievers, Carsten2
刊名JOURNAL OF CATALYSIS
2017-09-01
卷号353页码:107-115
关键词Ceria N-Ni delta+ clusters Heterogeneous catalysis Supported catalyst Nitrobenzene reduction
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.
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
收录类别SCI
语种英语
WOS记录号WOS:000410468300013
内容类型期刊论文
源URL[http://cas-ir.dicp.ac.cn/handle/321008/150029]  
专题大连化学物理研究所_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.Georgia Inst Technol, Sch Chem & Biomol Engn, 311 Ferst Dr NW, Atlanta, GA 30332 USA
3.Forschungszentrum Julich, Peter Grunberg Inst, D-52425 Julich, Germany
4.Forschungszentrum Julich, Ernst Ruska Ctr Microscopy & Spect Electrons, D-52425 Julich, Germany
5.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式
GB/T 7714
Heggen, Marc,Li, Mingrun,Lu, Jianmin,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 Heggen, Marc.,Li, Mingrun.,Lu, Jianmin.,Zhang, Jian.,Wang, Yehong.,...&Sievers, Carsten.(2017).Peculiar hydrogenation reactivity of Ni-Ni delta+ clusters stabilized by ceria in reducing nitrobenzene to azoxybenzene.JOURNAL OF CATALYSIS,353,107-115.
MLA Heggen, Marc,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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