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题名: Yin and Yang Dual Characters of CuOx Clusters for C-C Bond Oxidation Driven by Visible Light
作者: Hou, Tingting1, 2;  Luo, Nengchao1, 2;  Li, Hongji1, 2;  Heggen, Marc3, 4;  Lu, Jianmin1;  Wang, Yehong1;  Wang, Feng1
关键词: heterogeneous catalysis ;  visible light ;  ceria ;  copper ;  titania ;  C-C bond ;  benzaldehyde
刊名: ACS CATALYSIS
发表日期: 2017-06-01
DOI: 10.1021/acscatal.7b00629
卷: 7, 页:3850-3859
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical
研究领域[WOS]: Chemistry
英文摘要: Selective cleavage of C-C bonds is pursued as a useful chemical transformation method in biomass utilization. Herein, we report a hybrid CuOx/ceria/anatase nanotube catalyst in the selective oxidation of C-C bonds under visible light irradiation. Using the lignin fi-1 model as a substrate offers 96% yields of benzaldehydes. Characterization results by high angle annular dark field scanning transmission electron microscopy (HAADF-STEM) and energy-dispersive X-ray spectroscopy element (EDX) mapping reveal that CuOx clusters are highly dispersed on the exposed anatase surface as well as on the nanosized ceria domains. In-depth investigations by Raman and ultraviolet visible diffuse reflectance spectra (UV vis DRS), together with density functional theory (DFT) calculations, further verify that the CuOx clusters present on the ceria domains increase the concentration of surface defects (Ce3+) ions and oxygen vacancies) and accordingly improve the photocatalytic activity (Yang character); the CuOx clusters decorating on anatase suppress the side reaction (oxydehydrogenation without C-C bond cleavage) because of an upward shift in the valence band (VB) edge of anatase (Yin character). Mechanism investigation indicates hydrogen abstraction from beta-carbon by photogenerated holes is a vital step in the conversion.
关键词[WOS]: TOTAL-ENERGY CALCULATIONS ;  DEFINED SURFACE PLANES ;  LIGNIN MODEL COMPOUNDS ;  AUGMENTED-WAVE METHOD ;  PHOTOCATALYTIC OXIDATION ;  CERIA CATALYST ;  CEO2 NANOCRYSTALS ;  AEROBIC OXIDATION ;  TUNGSTEN-OXIDE ;  MODIFIED TIO2
语种: 英语
WOS记录号: WOS:000402851600014
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/152188
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, State Key Lab Catalysis, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Forschungszentrum Julich GmbH, Ernst Ruska Ctr Microscopy & Spect Electrons, D-52425 Julich, Germany
4.Forschungszentrum Juelich GmbH, Peter Grunberg Inst, D-52425 Julich, Germany

Recommended Citation:
Hou, Tingting,Luo, Nengchao,Li, Hongji,et al. Yin and Yang Dual Characters of CuOx Clusters for C-C Bond Oxidation Driven by Visible Light[J]. ACS CATALYSIS,2017,7:3850-3859.
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