Intermarrying MOF Glass\nand Lead Halide Perovskites\nfor Artificial Photosynthesis

The development of efficient artificial photosynthesis\nsystems\nis crucial for sustainable chemical production, as they mimic natural\nprocesses to convert solar energy into chemical products, thereby\naddressing both energy and environmental challenges. The main bottlenecks\nin current research include fabricating highly selective, stable,\nand scalable catalysts, as well as effectively harnessing the full\nspectrum of light, particularly the low-energy, long-wavelength portion.\nHerein, we report a novel composite photocatalyst system based on\nlead halide perovskites embedded in functionalized MOF glass. The\nconstruction of a well-defined interface between the light-harvesting\nperovskite and stable Rh single-atom-containing MOF glass mimics the\nfunctions of photosystem I (PS I). This facilitates efficient photoinduced\nelectron generation under visible light and subsequent electron transfer\nfor coenzyme (NADH) regeneration with high selectivity. The regenerated\nNADH can then be consumed by immobilized enzymes for CO<sub>2</sub> reduction, realizing the artificial photosynthesis process for formic\nacid generation. This work also elucidates the interactions and optoelectronic\nresponses between MOF glass and perovskites, offering insights into\nthe design and fabrication of nanocomposite photocatalysts for other\nadvanced chemical syntheses.

Publication Details

Journal
Figshare
Published
2024-12-29
DOI
https://doi.org/10.1021/jacs.4c12619.s001
Primary Topic
Perovskite Materials and Applications
Type
article
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article

Intermarrying MOF Glass\nand Lead Halide Perovskites\nfor Artificial Photosynthesis

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Perovskite Materials and Applications
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Intermarrying MOF Glass\nand Lead Halide Perovskites\nfor Artificial Photosynthesis

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Abstract

The development of efficient artificial photosynthesis\nsystems\nis crucial for sustainable chemical production, as they mimic natural\nprocesses to convert solar energy into chemical products, thereby\naddressing both energy and environmental challenges. The main bottlenecks\nin current research include fabricating highly selective, stable,\nand scalable catalysts, as well as effectively harnessing the full\nspectrum of light, particularly the low-energy, long-wavelength portion.\nHerein, we report a novel composite photocatalyst system based on\nlead halide perovskites embedded in functionalized MOF glass. The\nconstruction of a well-defined interface between the light-harvesting\nperovskite and stable Rh single-atom-containing MOF glass mimics the\nfunctions of photosystem I (PS I). This facilitates efficient photoinduced\nelectron generation under visible light and subsequent electron transfer\nfor coenzyme (NADH) regeneration with high selectivity. The regenerated\nNADH can then be consumed by immobilized enzymes for CO<sub>2</sub> reduction, realizing the artificial photosynthesis process for formic\nacid generation. This work also elucidates the interactions and optoelectronic\nresponses between MOF glass and perovskites, offering insights into\nthe design and fabrication of nanocomposite photocatalysts for other\nadvanced chemical syntheses.

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