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Exploring unique single-atom sites capable of efficiently reducing O to H O while being inert to H O decomposition under light conditions is significant for H O photosynthesis, but it remains challenging. Herein, we report the facile design and fabrication of polymeric carbon nitride (CN) decorated with single-Zn sites that have tailorable local coordination environments, which is enabled by utilizing different Zn salt anions. Specifically, the O atom from acetate (OAc) anion participates in the coordination of single-Zn sites on CN, forming asymmetric Zn-N O moiety on CN (denoted as CN/Zn-OAc), in contrast to the obtained Zn-N sites when sulfate (SO ) is adopted (CN/Zn-SO ). Both experimental and theoretical investigations demonstrate that the Zn-N O moiety exhibits higher intrinsic activity for O reduction to H O than the Zn-N moiety. This is attributed to the asymmetric N/O coordination, which promotes the adsorption of O and the formation of the key intermediate *OOH on Zn sites due to their modulated electronic structure. Moreover, it is inactive for H O decomposition under both dark and light conditions. As a result, the optimized CN/Zn-OAc catalyst exhibits significantly improved photocatalytic H O production activity under visible light irradiation.
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