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Yin and Yang Dual Characters of CuOx Clusters for C-C Bond Oxidation Driven by Visible Light
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
2017-06-01
DOI10.1021/acscatal.7b00629
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
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
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.
语种英语
WOS记录号WOS:000402851600014
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文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/152188
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, 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
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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.
APA Hou, Tingting.,Luo, Nengchao.,Li, Hongji.,Heggen, Marc.,Lu, Jianmin.,...&Wang, Feng.(2017).Yin and Yang Dual Characters of CuOx Clusters for C-C Bond Oxidation Driven by Visible Light.ACS CATALYSIS,7,3850-3859.
MLA Hou, Tingting,et al."Yin and Yang Dual Characters of CuOx Clusters for C-C Bond Oxidation Driven by Visible Light".ACS CATALYSIS 7(2017):3850-3859.
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