<scp> CO ₂ </scp> Conversion Into Energy Rich Fuels Over Nascent <scp>COF</scp> Decorated‐Lead Free Halide Perovskites Hybrid Nano Catalysts: Experimental and Computational Investigation

Even though lead‐containing halide perovskites have been deemed emerging materials. However, the presence of toxic and carcinogenic lead (Pb) metal, small surface area, low charge separation, and a high charge‐carrier recombination rate mainly restrain their widespread utilization. To shake off these challenges, we designed a non‐toxic lead‐free halide perovskite (LFHPs: CsSnBr 3 ) nanocatalyst, which possesses suitable energy band positions, efficient activities, and lower toxicity as compared to lead‐containing halide perovskites (CsPbBr 3 , CsPbCl 3 , CsPbI 3 ). To further shine the overall efficacy of LFHPs‐CsSnBr 3 , we decorate it with a polyarylimide‐based covalent organic framework. The resultant fabricated COF/CsSnBr 3 hybrid nano catalysts possess appropriate band structures, low charge recombination rate, elevated charge separation, large surface area, active surface sites with high porosity, tuned energy band gaps, and improved visible light‐harvesting capability compared to pristine CsSnBr 3 and COF. The most active sample (5COF/CsSnBr 3 ) delivered 4‐time improved activities for photocatalytic CO 2 conversion into C1 products (CO, CH 4 ) and C2 products (C 2 H 6 , C 2 H 5 OH, C 2 H 4 ). Our DFT calculations and simulation‐based strategy give deeper insights and support for our experimental findings. Ultimately, our novel research work will unlock a new pathway for designing non‐hazardous lead‐free halide perovskite‐based nanocatalysts for photocatalytic CO 2 conversion, energy‐rich fuels production, and achieving China's commitment to control CO 2 emissions before 2030.