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Photocatalytic CO2 reduction reaction (CO2RR) is an attractive process to convert CO2 into valuable chemicals. But this reaction is often restricted by the poor mass transfer of CO2 in the liquid phase. Here, we have developed a triphase photocatalytic CO2RR system by supporting Ag‐decorated TiO2 nanoparticles at a gas–water boundary with hydrophobic–hydrophilic abrupt interfacial wettability. Such a triphase system allows the rapid delivery of gas‐phase CO2 to the surface of photocatalysts while maintaining an efficient water supply and uncovered active sites. Ag‐TiO2 supported at the gas–water boundary showed a CO2 reduction rate of 305.7 μmol g−1 h−1, without hole scavengers, approximately 8 times higher than the nanoparticles dispersed in the liquid phase. Even using diluted CO2 (10 %) as the reactant, the CO2RR activity was superior to most reported Ag‐TiO2 based photocatalysts using pure CO2. The findings provide a general strategy to promote the interfacial CO2 mass transfer to improve photoactivity and selectivity. [ABSTRACT FROM AUTHOR]

Carbon‐supported NiII single‐atom catalysts with a tetradentate Ni‐N2O2 coordination formed by a Schiff base ligand‐mediated pyrolysis strategy are presented. A NiII complex of the Schiff base ligand (R,R)‐(−)‐N,N′‐bis(3,5‐di‐tert‐butylsalicylidene)‐1,2‐cyclohexanediamine was adsorbed onto a carbon black support, followed by pyrolysis of the modified carbon material at 300 °C in Ar. The Ni‐N2O2/C catalyst showed excellent performance for the electrocatalytic reduction of O2 to H2O2 through a two‐electron transfer process in alkaline conditions, with a H2O2 selectivity of 96 %. At a current density of 70 mA cm−2, a H2O2 production rate of 5.9 mol gcat.−1 h−1 was achieved using a three‐phase flow cell, with good catalyst stability maintained over 8 h of testing. The Ni‐N2O2/C catalyst could electrocatalytically reduce O2 in air to H2O2 at a high current density, still affording a high H2O2 selectivity (>90 %). A precise Ni‐N2O2 coordination was key to the performance. [ABSTRACT FROM AUTHOR]