Improvement of CO2 Reduction Photocatalysis of a Ru(II)–Re(I) Complex and Carbon Nitride Hybrid by Coadsorption of an Os(II) Complex Photosensitizer

IF 13.1 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2024-12-06 DOI:10.1021/acscatal.4c06134

Toshiya Tanaka, Mitsuhiko Shizuno, Yusuke Tamaki, Kazuhiko Maeda, Osamu Ishitani

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Abstract

Photocatalytic CO₂ reduction has attracted attention as a prospective technology for addressing global warming and the reduction in fossil fuel resources. Hybrid photocatalysts comprising a visible light-absorbing semiconductor and a supramolecular photocatalyst with photosensitizer and catalyst units in one molecule have been developed for CO₂ reduction. As an example, a hybrid of TiO₂-loaded polymeric carbon nitride (PCN) and a Ru(II)–Re(I) supramolecular photocatalyst (RuRe/TiO₂/PCN) works as a CO₂ reduction photocatalyst in the presence of triethanolamine (TEOA) to give CO with a high selectivity. However, its durability is low, and the maximum turnover number of CO formations (TON_CO) is less than 100. In this study, a system was constructed with coadsorption of an Os(II)-complex photosensitizer (OsP) on the surface of RuRe/TiO₂/PCN to improve the low durability of the hybrid photocatalyst by promoting a more rapid electron supply to the Re catalyst unit of RuRe. The coadsorption of OsP increased the TON_CO of RuRe/TiO₂/PCN to 239.

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Os（II）配合物光敏剂对Ru(II) -Re (I)配合物和氮化碳杂化物CO2还原光催化性能的改进

光催化CO2还原技术作为应对全球变暖和减少化石燃料资源的一项有前景的技术而受到关注。混合光催化剂包括可见光吸收半导体和具有光敏剂和催化剂单元在一个分子中的超分子光催化剂已被开发用于CO2还原。例如，负载TiO2的聚合物氮化碳（PCN）和Ru(II) -Re (I)超分子光催化剂（RuRe/TiO2/PCN）在三乙醇胺（TEOA）存在下作为CO2还原光催化剂，使CO具有高选择性。但其耐久性较低，最大CO地层周转数（TONCO）不足100个。本研究构建了Os(II)-络合物光敏剂（OsP）在RuRe/TiO2/PCN表面的共吸附体系，通过促进RuRe的Re催化剂单元更快的电子供应来改善杂化光催化剂的低耐久性。OsP的共吸附使RuRe/TiO2/PCN的TONCO达到239。

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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.