Promoting CH 4 photoconversion by reconstruction of polaron states

Selective oxidation of methane (CH 4 ) has attractive potentials for mitigating global warming and producing value-added chemicals, while the activation of highly inert CH 4 remains challenging. Herein, we developed a single-atomic Pt-doped WO 3 (Pt 1 -WO 3 ) 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 CH 4 activation and conversion efficiency. Under 150 mW·cm −2 light intensity and aqueous conditions, the Pt 1 -WO 3 photocatalyst exhibited a peak CH 4 -to-CH 3 OH conversion yield of 1151 μmol·g cat −1 ·h −1 without the use of photosensitizers, sacrificial reagents or strong oxidizers like O 2 or H 2 O 2 , exceeding the previous reports on photocatalytic CH 4 oxidation under similar conditions, thus suggesting the capability of tuning polaron states for enhanced photocatalysis.