<p>Hybrid lead halides have demonstrated great promise for CO<sub>2</sub> 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 C<sub>2</sub> production in near-infrared-driven CO<sub>2</sub> photoreduction, achieving notable C<sub>2</sub> production rates of up to 14.2 <i>μ</i>mol g<sup>-1</sup> h<sup>-1</sup> 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.</p>

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Near-infrared-driven photocatalytic CO2 reduction to C2 hydrocarbons by bis(terpyridine)-metal functionalized lead halide frameworks

  • Yukong Li,
  • Ziyi Wang,
  • Xiaoyang He,
  • Chen Sun,
  • Qikai Zheng,
  • Yilin Jiang,
  • Zuofeng Chen,
  • Honghan Fei

摘要

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.