Enhanced Photocatalytic Conversion of CO2 by H2O over Ag@Cr Cocatalyst-Modified ZnTa2O6

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-02-21 DOI:10.1021/acscatal.4c06530

Kio Kawata, Shoji Iguchi, Shimpei Naniwa, Masamu Nishimoto, Kentaro Teramura

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Abstract

A zinc tantalate (ZnTa₂O₆) photocatalyst modified with an Ag cocatalyst via ultrasonic reduction (denoted as Ag(USR)/ZnTa₂O₆) exhibited higher activity for the photocatalytic conversion of CO₂ by H₂O than Ag/ZnTa₂O₆ prepared by other widely used methods. However, the CO formation rate was low. In this study, a photocatalyst was prepared by coating the Ag nanoparticles of Ag(USR)/ZnTa₂O₆ with Cr(OH)₃·xH₂O via the photodeposition (PD) method (denoted as Cr(PD)/Ag(USR)/ZnTa₂O₆) to increase the CO formation rate. Cr(PD)/Ag(USR)/ZnTa₂O₆ produced CO at the maximum formation rate of ∼600 μmol h^–1, which was 50 and 8.5 times higher than those of bare ZnTa₂O₆ and Ag(USR)/ZnTa₂O₆, respectively. Furthermore, an induction period was observed during the time course of photocatalytic activity. The scanning electron microscopy images highlighted that Ag nanoparticles migrate to a specific site on the surface of ZnTa₂O₆ as photoirradiation proceeded, causing the rearrangement of Ag nanoparticles during this period. This rearrangement caused the separation of the photocatalytic reaction field, achieving high activity toward the photocatalytic conversion of CO₂ because of the efficient reduction and oxidation reactions. Moreover, inductively coupled plasma mass spectrometry and ultraviolet–visible absorption spectroscopy revealed that Cr³⁺ in Cr(PD)/Ag(USR)/ZnTa₂O₆ is oxidized to dissolvable CrO₄^2– during the induction period. These CrO₄^2– anions in solution were found to play a crucial role in maintaining the Cr layer of Cr(PD)/Ag(USR)/ZnTa₂O₆.

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.