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Photoreduction of CO2 to hydrocarbons encounters two significant challenges: low product yields and poor selectivity. Furthermore, the difficulty of C-C coupling reactions hinders the formation of higher-value twocarbon products. This paper presents a strategy to address these challenges by fabricating a van der Waals heterostructure photocatalyst through the surface modification of TiO2 nanotubes (TNTs) with monolayer Nb2O5, denoted as 3 %Nb2O5/TNTs. Compared with TNTs, the acetic acid yield of heterostructures reached 28.4 μmol gcat -1 h 1, and the selectivity rose from 48 % to 69 %. The van der Waals heterostructures reduced the photogenerated electron-hole recombination, extending the lifetime of charge carriers. The reduction of resistance and the presence of built-in fields accelerated the migration of charge carriers, thereby showing an enhanced photocatalytic performance. Surface modification of monolayer Nb2O5 promoted the activation adsorption of CO2 to CO2⋅, facilitating the following C-C coupling reaction. Furthermore, its surface acidity sites modulated the hydrogenation reactions following C-C coupling, thereby increasing both the yield and selectivity
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