Design of frustrated Lewis pair in defective TiO2 for photocatalytic non-oxidative methane coupling

The efficient C–H polarization is the prerequisite for low-temperature photocatalytic CH 4 conversion, which restricted by poor stretching ability of short-distance adjacent lattice atoms. Here, a frustrated Lewis pair (FLP) composed doped metal in TiO 2 as acid (LA) and neighboring Ti–OH base (LB) with long distance (0.31–0.37 nm) was designed through DFT calculation fabricated hydrogenation treatment metal-doped –SiO macroporous-mesoporous structure. Benefitting from LA-LB matched acid-base intensity, hydrogenated Ga-doped composite achieves superior high conversion rate (139 ?mol g ?1 h ). photo-irradiation causes electron excitation Ga to according time-dependent situ EPR analysis, promotes formation coupling ·CH 3 . This work provides key underpinning regulating characteristics FLP activation C–C via light irradiation. • Frustrated defective 139 NOCM achieved under irradiation suitable intensity conducive Photo-irradiation serious greenhouse effect caused massive use fossil energy an inevitable environmental problem today’s world. In particular, methane 25 times that CO However, traditional process consumes great deal energy. study emphasizes driven green renewable solar mild conditions. Its fundamental principle generate charge using semiconductors. attributed unique active sites on , such magnets, attract C H, respectively, effectively break bond, high-value products action photogenerated charge. research does not require temperature pressure industry significance realize development protection beneficial all. Long LA–LB strong intensities promote bond. improving LA LB confirmed based transition LB, forming methyl hydrogen radicals further production H 6