Promoting CH4 photoconversion by reconstruction of polaron states
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![[(DPEPhos)(bcp)Cu]PF6: A General and Broadly Applicable Copper-Based Photoredox Catalyst](/_next/image?url=https%3A%2F%2Fcloudfront.jove.com%2FCDNSource%2Fteasers%2F59739.jpg&w=3840&q=50)
[(DPEPhos)(bcp)Cu]PF6: A General and Broadly Applicable Copper-Based Photoredox Catalyst
Published on: May 21, 2019
Shuya Hao1, Yuanyuan Xue1, Ximeng Lv1
1Laboratory of Advanced Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Shanghai Academy of Natural Sciences; Fudan University, Shanghai 200438, China.
Abstract:
Selective oxidation of methane (CH4) has attractive potentials for mitigating global warming and producing value-added chemicals, while the activation of highly inert CH4 remains challenging. Herein, we developed a single-atomic Pt-doped WO3 (Pt1-WO3) catalyst, which enabled to reconstruct polaron states from W to Pt-O sites. This polaron reconstruction allows for fast separation of photogenerated charge carriers and tuning of reactant adsorption sites, and greatly improves the photocatalytic CH4 activation and conversion efficiency. Under 150 mW·cm-2 light intensity and aqueous conditions, the Pt1-WO3 photocatalyst exhibited a peak CH4-to-CH3OH conversion yield of 1151 μmol·gcat-1·h-1 without the use of photosensitizers, sacrificial reagents or strong oxidizers like O2 or H2O2, exceeding the previous reports on photocatalytic CH4 oxidation under similar conditions, thus suggesting the capability of tuning polaron states for enhanced photocatalysis.
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