TY - JOUR
T1 - Template free mild hydrothermal synthesis of core-shell Cu2O(Cu)@CuO visible light photocatalysts for N-acetyl-para-aminophenol degradation
AU - Karthikeyan, Sekar
AU - Chuaicham, Chitiphon
AU - Pawar, Radheshyam R.
AU - Sasaki, Keiko
AU - Li, Wei
AU - Lee, Adam F.
AU - Wilson, Karen
N1 - Funding Information:
S. K. and K. S. would like to thank the Japan Society for the Promotion of Science (JSPS) for providing a postdoctoral fellowship for foreign researchers (P18387) and the research grant (KAKENHI JP18F18387). We thank Prof. Kuniyoshi Shi-mizu and Mr Dedi Satria at Graduate School of Agriculture, Kyushu University for supporting LC-MS analysis. XANES measurements were performed at Kyushu University Beamline (SAGA-LS/BL06 with proposal No. 2019IK004). FE-SEM and HR(S)TEM performed at the Ultra-microscopy Research Centre (URC) at Kyushu University and X-ray photoelectron spectra were collected at Advanced Analytical Centre (Nanotechnology Platform), Kyushu University under the proposal No. S-18-KU-0043.
Publisher Copyright:
© 2019 The Royal Society of Chemistry.
PY - 2019
Y1 - 2019
N2 - Solar photocatalytic processes are a promising approach to environmental remediation, however their implementation requires improvements in visible light harvesting and conversion and a focus on low cost, Earth abundant materials. Semiconducting copper oxides are promising visible light photocatalysts for solar fuels and wastewater depollution. Here we report the mild, hydrothermal (template-free) synthesis of core-shell Cu2O(Cu)@CuO photocatalytic architectures for the visible light photocatalytic degradation of N-acetyl-para-aminophenol (APAP). Hollow and rattle-like core-shell nanosphere aggregates with diameters between 200 nm and 2.5 μm formed under different synthesis conditions; all comprised an inner Cu2O shell, formed of 10-50 nm nanoparticles, surrounded by a protective corona of CuO nanoparticles. High reductant and structure-directing agent concentrations promoted the formation of a yolk-like Cu2O/Cu core, associated with improved photophysical properties, notably a high oxidation potential and suppressed charge carrier recombination, that correlated with the highest apparent quantum efficiency (8%) and rate of APAP removal (7 μmol g-1 min-1). Trapping experiments demonstrated hydroxyl radicals were the primary active species responsible for APAP oxidation to quinones and short chain carboxylic acids. Rattle-like core-shell Cu2O/Cu@CuO nanospheres exhibited excellent physiochemical stability and recyclability for APAP photocatalytic degradation.
AB - Solar photocatalytic processes are a promising approach to environmental remediation, however their implementation requires improvements in visible light harvesting and conversion and a focus on low cost, Earth abundant materials. Semiconducting copper oxides are promising visible light photocatalysts for solar fuels and wastewater depollution. Here we report the mild, hydrothermal (template-free) synthesis of core-shell Cu2O(Cu)@CuO photocatalytic architectures for the visible light photocatalytic degradation of N-acetyl-para-aminophenol (APAP). Hollow and rattle-like core-shell nanosphere aggregates with diameters between 200 nm and 2.5 μm formed under different synthesis conditions; all comprised an inner Cu2O shell, formed of 10-50 nm nanoparticles, surrounded by a protective corona of CuO nanoparticles. High reductant and structure-directing agent concentrations promoted the formation of a yolk-like Cu2O/Cu core, associated with improved photophysical properties, notably a high oxidation potential and suppressed charge carrier recombination, that correlated with the highest apparent quantum efficiency (8%) and rate of APAP removal (7 μmol g-1 min-1). Trapping experiments demonstrated hydroxyl radicals were the primary active species responsible for APAP oxidation to quinones and short chain carboxylic acids. Rattle-like core-shell Cu2O/Cu@CuO nanospheres exhibited excellent physiochemical stability and recyclability for APAP photocatalytic degradation.
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U2 - 10.1039/c9ta07009e
DO - 10.1039/c9ta07009e
M3 - Article
AN - SCOPUS:85072313875
VL - 7
SP - 20767
EP - 20777
JO - Journal of Materials Chemistry A
JF - Journal of Materials Chemistry A
SN - 2050-7488
IS - 36
ER -