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Amorphous Strategy and Doping Copper on Metal-organic Framework Surface for Enhanced Photocatalytic CO2 Reduction to C2H4
Chemistry - A European Journal ( IF 3.9 ) Pub Date : 2024-07-22 , DOI: 10.1002/chem.202402031
Lixiao Zheng 1 , Huayong Yang 1 , Min Zhang 1 , Zhongjie Guan 1 , Qiuye Li 1 , Jianjun Yang 2
Affiliation  

Amorphous photocatalysts are characterized by numerous grain boundaries and abundant unsaturated sites, which enhance reaction efficiency from both kinetic and thermodynamic perspectives. However, amorphization strategies have rarely been used for photocatalytic CO2 reduction. Doping copper onto a metal–organic framework (MOF) surface can regulate the electronic structure of photocatalysts, promote electron transfer from the MOF to Cu, and improve the separation efficiency of electron-hole pairs. In this study, an amorphous photocatalyst MOFw-p/Cu containing highly dispersed Cu (0, I, II) sites was designed and synthesized by introducing a regulator and in situ copper species during the nucleation process of MOF (UiO-66-NH2). Various characterizations confirmed that the Cu species were anchored to the organometallic skeleton of the surface amorphization MOF structure. The synergistic effect of Cu doping and surface amorphization in MOFw-p/Cu can significantly enhance the CO and CH4 yields while promoting the formation of the multicarbon product C2H4. The approach holds promise for developing novel, highly efficient MOFs as photocatalysts for CO2 photoreduction, enabling the production of high-value-added C2 products.

中文翻译:


非晶策略和金属有机框架表面掺杂铜增强光催化 CO2 还原为 C2H4



非晶态光催化剂的特点是具有大量的晶界和丰富的不饱和位点,从动力学和热力学角度都提高了反应效率。然而,非晶化策略很少用于光催化二氧化碳还原。将铜掺杂到金属有机骨架(MOF)表面可以调节光催化剂的电子结构,促进电子从MOF转移到Cu,并提高电子-空穴对的分离效率。本研究通过在MOF(UiO-66-NH2)成核过程中引入调节剂和原位铜物种,设计并合成了含有高度分散的Cu(0,I,II)位点的非晶光催化剂MOFw-p/Cu 。各种表征证实 Cu 物质锚定在表面非晶化 MOF 结构的有机金属骨架上。 MOFw-p/Cu中Cu掺杂和表面非晶化的协同作用可以显着提高CO和CH4的产率,同时促进多碳产物C2H4的形成。该方法有望开发新型、高效的 MOF 作为 CO2 光还原的光催化剂,从而实现高附加值 C2 产品的生产。
更新日期:2024-07-26
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