Beyond Reduction Cocatalysts: Critical Role of Metal Cocatalysts in Photocatalytic Oxidation of Methane with Water**

Author:

Saito Hikaru1ORCID,Sato Hiromasa1ORCID,Higashi Taisuke1,Sugimoto Toshiki123ORCID

Affiliation:

1. Department of Materials Molecular Science Institute for Molecular Science Okazaki Aichi 444-8585 Japan

2. Graduate Institute for Advanced Studies (SOKENDAI) Okazaki Aichi 444-8585 Japan

3. Precursory Research for Embryonic Science and Technology (PRESTO) Japan Science and Technology Agency (JST) 4-1-8 Honcho Kawaguchi Saitama 332-0012 Japan

Abstract

AbstractEnvironmentally sustainable and selective conversion of methane to valuable chemicals under ambient conditions is pivotal for the development of next‐generation photocatalytic technology. However, due to the lack of microscopic knowledge about non‐thermal methane conversion, controlling and modulating photocatalytic oxidation processes driven by photogenerated holes remain a challenge. Here, we report novel function of metal cocatalysts to accept photogenerated holes and dominate selectivity of methane oxidation, which is clearly beyond the conventional concept in photocatalysis that the metal cocatalysts loaded on the surfaces of semiconductor photocatalysts mostly capture photogenerated electrons and dominate reduction reactions exclusively. The novel photocatalytic role of metal cocatalysts was verified by operando molecular spectroscopy combined with real‐time mass spectrometry for metal‐loaded Ga2O3 model photocatalysts under methane and water vapor at ambient temperature and pressure. Our concept of metal cocatalysts that work as active sites for both photocatalytic oxidation and reduction provides a new understanding of photocatalysis and a solid basis for controlling non‐thermal redox reactions by metal‐cocatalyst engineering.

Funder

Precursory Research for Embryonic Science and Technology

Japan Society for the Promotion of Science

Institute for Molecular Science

National Institutes of Natural Sciences

Ministry of the Environment, Government of Japan

Publisher

Wiley

Subject

General Medicine

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