Bioinspired catalytic pocket promotes CO(2)-to-ethanol photoconversion on colloidal quantum wells.

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作者:Pan Rongrong, Wang Qi, Zhao Yan, Feng Zhendong, Xu Yanjun, Wang Zhuan, Li Yapeng, Zhang Xiuming, Zhang Haoqing, Liu Jia, Gu Xiang-Kui, Zhang Jiangwei, Weng Yuxiang, Zhang Jiatao
Sluggish surface reaction is a critical factor that strongly governs the efficiency of photocatalytic solar fuel production, particularly in CO(2)-to-ethanol photoconversion. Here, inspired by the principles underlying enzyme catalytic proficiency and specificity, we report a biomimetic photocatalyst that affords superior CO(2)-to-ethanol photoreduction efficiency (5.5 millimoles gram(-1) hour(-1) in average with 98.2% selectivity) distinctly surpassing the state of the art. The key is to create a class of catalytic pocket, which contains spatially organized NH(2)…Cu-Se(-Zn) multiple functionalities at close range, over ZnSe colloidal quantum wells. Such structure offers a platform to mimic the concerted cooperation between the active site and surrounding secondary/outer coordination spheres in enzyme catalysis. This is manifested by the chemical adsorption and activation of CO(2) via a bent geometry, favorable stabilization toward a variety of important intermediates, promotion of multielectron/proton transfer processes, etc. These results highlight the potential of incorporating enzyme-like features into the design of photocatalysts to overcome the challenges in CO(2) reduction.

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