Journal Article

FZJ-2017-06686

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Yin and Yang Dual Characters of CuOx Clusters for C-C Band Oxidation Driven by Visible Light

Hou, T. ; Luo, N. ; Li, H. ; Heggen, M.FZJ* ; Lu, J. ; Wang, Y. ; Wang, F. (Corresponding author)

2017
ACS Washington, DC

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Please use a persistent id in citations: http://hdl.handle.net/2128/15328  doi:10.1021/acscatal.7b00629

Abstract: 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 β-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 (oxy-dehydrogenation 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 β-carbon by photogenerated holes is a vital step in the conversion.

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Contributing Institute(s):

1. Physik Nanoskaliger Systeme (ER-C-1)

Research Program(s):

1. 143 - Controlling Configuration-Based Phenomena (POF3-143) (POF3-143)

Appears in the scientific report 2017

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Database coverage:
; ; Current Contents - Physical, Chemical and Earth Sciences ; Free to read ; IF >= 5 ; JCR ; NCBI Molecular Biology Database ; SCOPUS ; Science Citation Index Expanded ; Thomson Reuters Master Journal List ; Web of Science Core Collection

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