Issue 20, 2023

A combined theoretical and experimental investigation on the photocatalytic hydrogenation of CO2 on Cu/ZnO polar surface

Abstract

The photocatalytic hydrogenation of CO2 by Cu-deposited ZnO (Cu/ZnO) polar surfaces is investigated through density functional theory (DFT) calculations combined with experimental work. The DFT results demonstrate that, without Cu-loading, CO2 and H2 present weak physisorption on the clean ZnO polar surface, except that H2 undergoes strong chemisorption on the ZnO(000[1 with combining macron]) surface. Cu deposition on the ZnO polar surface could remarkably enhance the CO2 chemisorption ability, due to the induced charge redistribution on the interface of the Cu/ZnO polar surface systems. Additionally, a Cu-nanoisland, which was simulated using a Cu(111) slab model, exhibited strong ability to chemically adsorb H2. Thus, H2 may act as an adsorption competitor to CO2 on the Cu/ZnO(000[1 with combining macron]), while, in contrast, CO2 and H2 (syngas) may have more opportunity to simultaneously adsorb on Cu/ZnO(0001) to promote the CO2 hydrogenation. These facet-dependent properties lead us to assume that Cu/ZnO(0001) should be a favorable photocatalyst for CO2 hydrogenation. This assumption is further verified by our photocatalysis experiment based on a ZnO single crystal. According to the theoretical and experimental results, the optimal HCOO* reaction pathway for the photocatalytic hydrogenation of CO2 on Cu/ZnO(0001) is proposed. In this optimal HCOO* path, the hydrogenation of CO2* step and hydrogenation of HCOO* step could be promoted by the coupling of a photo-generated spillover proton and a photoelectron on the interface of Cu/ZnO(0001). This research demonstrates the feasibility of the photocatalytic reduction of CO2 on Cu/ZnO(0001), and will help to develop related high-efficiency catalysts.

Graphical abstract: A combined theoretical and experimental investigation on the photocatalytic hydrogenation of CO2 on Cu/ZnO polar surface

Supplementary files

Article information

Article type
Paper
Submitted
11 شعبان 1444
Accepted
01 شوال 1444
First published
01 شوال 1444

Nanoscale, 2023,15, 9040-9048

A combined theoretical and experimental investigation on the photocatalytic hydrogenation of CO2 on Cu/ZnO polar surface

H. Xiao, Y. Lian, S. Zhang, M. Zhang, J. Zhang and C. Li, Nanoscale, 2023, 15, 9040 DOI: 10.1039/D3NR01001E

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements