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Intermarrying MOF Glass and Lead Halide Perovskites for Artificial Photosynthesis
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-12-29 , DOI: 10.1021/jacs.4c12619
Wengang Huang, Bun Chan, Yuwei Yang, Peng Chen, Jingjing Wang, Lachlan Casey, Cesare Atzori, Tobias Schulli, Olivier Mathon, Haira G. Hackbarth, Nicholas M. Bedford, Dominique Appadoo, Xuemei Li, Tongen Lin, Rijia Lin, Jaeho Lee, Zhiliang Wang, Vicki Chen, Anthony K. Cheetham, Lianzhou Wang, Jingwei Hou

The development of efficient artificial photosynthesis systems is crucial for sustainable chemical production, as they mimic natural processes to convert solar energy into chemical products, thereby addressing both energy and environmental challenges. The main bottlenecks in current research include fabricating highly selective, stable, and scalable catalysts, as well as effectively harnessing the full spectrum of light, particularly the low-energy, long-wavelength portion. Herein, we report a novel composite photocatalyst system based on lead halide perovskites embedded in functionalized MOF glass. The construction of a well-defined interface between the light-harvesting perovskite and stable Rh single-atom-containing MOF glass mimics the functions of photosystem I (PS I). This facilitates efficient photoinduced electron generation under visible light and subsequent electron transfer for coenzyme (NADH) regeneration with high selectivity. The regenerated NADH can then be consumed by immobilized enzymes for CO2 reduction, realizing the artificial photosynthesis process for formic acid generation. This work also elucidates the interactions and optoelectronic responses between MOF glass and perovskites, offering insights into the design and fabrication of nanocomposite photocatalysts for other advanced chemical syntheses.

中文翻译:


MOF 玻璃和氢化铅钙钛矿的交配用于人工光合作用



开发高效的人工光合作用系统对于可持续化学品生产至关重要,因为它们模仿自然过程将太阳能转化为化学产品,从而应对能源和环境挑战。当前研究的主要瓶颈包括制造高选择性、稳定和可扩展的催化剂,以及有效利用全光谱光,特别是低能量、长波长部分。在此,我们报道了一种基于嵌入功能化 MOF 玻璃中的卤化铅钙钛矿的新型复合光催化剂系统。在光捕获钙钛矿和稳定的 Rh 单原子包含 MOF 玻璃之间构建一个定义明确的界面,模拟了光系统 I (PS I) 的功能。这有助于在可见光下高效产生光诱导电子,并随后以高选择性进行辅酶 (NADH) 再生的电子转移。然后,再生的 NADH 可以被固定化酶消耗以减少 CO2,实现生成甲酸的人工光合作用过程。这项工作还阐明了 MOF 玻璃和钙钛矿之间的相互作用和光电响应,为用于其他先进化学合成的纳米复合光催化剂的设计和制造提供了见解。
更新日期:2024-12-29
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