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Hybrid lead halides have demonstrated great promise for CO2 photoreduction due to their excellent photophysical properties. However, developing a single-component hybrid lead halide that combines high intrinsic stability with near-infrared absorption remains a significant challenge. Herein, to address both issues, we design a series of nine highly stable lead halide frameworks functionalized by bis(terpyridine)-metal complexes, which exhibit strong light absorption extending into the near-infrared region up to 1150 nm. Unlike their symmetric chloride and bromide analogues, the charge-polarized lead iodide sites in bis(terpyridine)-metal-functionalized frameworks serve as highly efficient C–C coupling centers for C2 production in near-infrared-driven CO2 photoreduction, achieving notable C2 production rates of up to 14.2 μmol g-1 h-1 with electron selectivities as high as 86%. These performances match the state-of-the-art among all reported single-component, near-infrared-responsive photocatalysts. This work highlights the potential of coordination-driven assembly of highly stable lead halide frameworks for near-infrared-driven artificial photosynthesis. A family of bis(terpyridine)-metal-functionalized lead halide frameworks is synthesized with both near-infrared absorption and charge-polarized sites, demonstrating efficient near-infrared-driven CO2 photoreduction to C2 hydrocarbon products.
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