Bifunctional Metal–Organic Layer for Selective Photocatalytic Carbon Dioxide Reduction to Carbon Monoxide

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2024-11-01 DOI:10.1021/acscatal.4c04772

Yingling Liao, Zitong Wang, Jinhong Li, Yingjie Fan, David Wang, Li Shi, Wenbin Lin

引用次数: 0

Abstract

We report a bifunctional metal–organic layer (MOL) as a photocatalyst for CO₂ reduction to CO under visible light irradiation with a turnover number of 6990 in 24 h and a CO selectivity of 99%. The fully accessible and modifiable Hf₁₂ secondary building units and the coordinating porphyrin linkers of the MOL allow for the integration of both Ru photosensitizers and catalytic Fe-porphyrin sites into one single platform. The close distance (∼11 Å) between the Ru photosensitizer and the catalytic center leads to enhanced electron transfer and promotes photocatalytic CO₂ reduction. This strategy leads to an increase of the CO₂-to-CO turnover number for the bifunctional MOL catalyst over a combination of a homogeneous Ru photosensitizer and an Fe-porphyrin complex. The mechanism of MOL-catalyzed CO₂ photoreduction was also studied by photophysical and electrochemical experiments.

Abstract Image

查看原文本刊更多论文

用于选择性光催化二氧化碳还原成一氧化碳的双功能金属有机层

我们报告了一种双功能金属有机层（MOL）光催化剂，可在可见光照射下将二氧化碳还原为一氧化碳，24 小时周转次数达 6990 次，一氧化碳选择性达 99%。MOL 的 Hf12 二级结构单元和配位卟啉连接体完全可触及和修改，因此可将 Ru 光敏剂和催化铁卟啉位点整合到一个平台中。Ru 光敏剂与催化中心之间的距离很近（∼11 Å），从而增强了电子传递，促进了光催化二氧化碳还原。与均相 Ru 光敏剂和铁卟啉复合物的组合相比，这种策略提高了双功能 MOL 催化剂的 CO2-CO转化率。此外，还通过光物理和电化学实验研究了 MOL 催化 CO2 光还原的机理。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.