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Currently, conventional dimethoxymethane synthesis methods are environmentally unfriendly. Here, we report a photo-redox catalysis system to generate dimethoxymethane using a silver and tungsten co-modified blue titanium dioxide catalyst (Ag.W-BTO) by coupling CO2 reduction and CH3OH oxidation under mild conditions. The Ag.W-BTO structure and its electron and hole transfer are comprehensively investigated by combining advanced characterizations and theoretical studies. Strikingly, Ag.W-BTO achieve a record photocatalytic activity of 5702.49 µmol g−1 with 92.08% dimethoxymethane selectivity in 9 h of ultraviolet-visible irradiation without sacrificial agents. Systematic isotope labeling experiments, in-situ diffuse reflectance infrared Fourier-transform analysis, and theoretical calculations reveal that the Ag and W species respectively catalyze CO2 conversion to *CH2O and CH3OH oxidation to *CH3O. Subsequently, an asymmetric carbon-oxygen coupling process between these two crucial intermediates produces dimethoxymethane. This work presents a CO2 photocatalytic reduction system for multi-carbon production to meet the objectives of sustainable economic development and carbon neutrality. This study unravels the efficient photocatalytic route for synthesizing dimethoxymethane by coupling CO2 reduction integrated with CH3OH oxidation by using a silver and tungsten comodified blue titanium dioxide catalyst under mild conditions. [ABSTRACT FROM AUTHOR]

Recently, lead halide perovskites have attracted significant attention as promising absorber materials for photoelectrochemical (PEC) solar water splitting. However, charge‐accumulation‐induced ion migration at the interface causes perovskite degradation and efficiency loss. To suppress the charge accumulation and improve the PEC performance of the perovskite photoanode, a simple interface engineering is proposed by decorating the SnO2/perovskite interface with a mixture of polyethylenimine ethoxylated (PEIE) and chlorobenzenesulfonic acid (CBSA). The mixed CBSA+PEIE treatment effectively passivates the oxygen vacancies in SnO2 and adjusts the band alignment between SnO2 and the perovskite. The synergistic effects of the mixture treatment facilitate an effective carrier extraction at the SnO2/perovskite interface, enhance the PEC performance, and improve the stability of the device. The perovskite photoanode exhibits an impressive applied bias photon‐to‐current efficiency of 12.9% with an outstanding durability for 225 h. Furthermore, an unbiased solar water splitting is achieved using all the perovskite photoelectrodes, resulting in a remarkable unassisted solar‐to‐hydrogen efficiency of 10.9% and a continuous 22 h stable operation. [ABSTRACT FROM AUTHOR]