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Issue 14, 2021
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The impact of surface Cu2+ of ZnO/(Cu1−xZnx)O heterostructured nanowires on the adsorption and chemical transformation of carbonyl compounds

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Abstract

The surface cation composition of nanoscale metal oxides critically determines the properties of various functional chemical processes including inhomogeneous catalysts and molecular sensors. Here we employ a gradual modulation of cation composition on a ZnO/(Cu1−xZnx)O heterostructured nanowire surface to study the effect of surface cation composition (Cu/Zn) on the adsorption and chemical transformation behaviors of volatile carbonyl compounds (nonanal: biomarker). Controlling cation diffusion at the ZnO(core)/CuO(shell) nanowire interface allows us to continuously manipulate the surface Cu/Zn ratio of ZnO/(Cu1−xZnx)O heterostructured nanowires, while keeping the nanowire morphology. We found that surface exposed copper significantly suppresses the adsorption of nonanal, which is not consistent with our initial expectation since the Lewis acidity of Cu2+ is strong enough and comparable to that of Zn2+. In addition, an increase of the Cu/Zn ratio on the nanowire surface suppresses the aldol condensation reaction of nonanal. Surface spectroscopic analysis and theoretical simulations reveal that the nonanal molecules adsorbed at surface Cu2+ sites are not activated, and a coordination-saturated in-plane square geometry of surface Cu2+ is responsible for the observed weak molecular adsorption behaviors. This inactive surface Cu2+ well explains the mechanism of suppressed surface aldol condensation reactions by preventing the neighboring of activated nonanal molecules. We apply this tailored cation composition surface for electrical molecular sensing of nonanal and successfully demonstrate the improvements of durability and recovery time as a consequence of controlled surface molecular behaviors.

Graphical abstract: The impact of surface Cu2+ of ZnO/(Cu1−xZnx)O heterostructured nanowires on the adsorption and chemical transformation of carbonyl compounds

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Supplementary files

Article information


Submitted
05 Feb 2021
Accepted
22 Feb 2021
First published
08 Mar 2021

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2021,12, 5073-5081
Article type
Edge Article

The impact of surface Cu2+ of ZnO/(Cu1−xZnx)O heterostructured nanowires on the adsorption and chemical transformation of carbonyl compounds

J. Liu, K. Nagashima, Y. Nagamatsu, T. Hosomi, H. Saito, C. Wang, W. Mizukami, G. Zhang, B. Samransuksamer, T. Takahashi, M. Kanai, T. Yasui, Y. Baba and T. Yanagida, Chem. Sci., 2021, 12, 5073
DOI: 10.1039/D1SC00729G

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    [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the European Society for Photobiology, the European Photochemistry Association, and RSC.
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    [Original citation] - Published by The Royal Society of Chemistry.

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