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oai:figshare.com:article/34028749 2026-09-30T03:04:33Z category_1 category_4 category_146 category_14 category_19 category_272 category_873 category_734 portal_63 item_type_6 month_year_09_2026

Coupling Self-Sensitized CO₂ Photoreduction of Silicon(IV)-Terpyridine Complexes with Organic Synthesis Yilin Xue (12250172) Jinchi Han (10091216) Duobin Chao (10174527) Biophysics Biochemistry Space Science Molecular Biology Pharmacology Environmental Sciences not elsewhere classified Chemical Sciences not elsewhere classified Biological Sciences not elsewhere classified situ drifts measurements new molecular photocatalysts emission quenching experiments sensitized molecular photocatalysts based reduction processes co without requiring 2 </ sub sensitized process theoretical calculations spectroelectrochemical analysis selective reduction reductively quenched reduction products reduction occurring reduced state promising strategy potential electrolysis organic synthesis organic carbonylation light irradiation first use external photosensitizer direct utilization considerable interest bih ). The development of new molecular photocatalysts for CO₂ reduction has considerable interest. Furthermore, the direct utilization of CO₂ reduction products in organic synthesis is a promising strategy for the valorization of CO₂. Herein, we report the first use of main-group silicon(IV) coordination complexes as self-sensitized molecular photocatalysts for the near-unity-selective reduction of CO₂ to CO without requiring an external photosensitizer. Under visible-light irradiation, these Si(IV) complexes are photoexcited and can be reductively quenched by 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole (BIH). Mechanistic studies reveal five ligand-based reduction processes for Si(IV) complexes, with CO₂ reduction occurring at a five-electron-reduced state of the ligand. The self-sensitized process was further elucidated by theoretical calculations, spectroelectrochemical analysis, emission quenching experiments, controlled-potential electrolysis, and in situ DRIFTS measurements. Notably, a sunlight-driven tandem catalytic system has been established by integrating this Si(IV)-based CO₂ photoreduction with organic carbonylation to produce valuable carbonyl compounds. 2026-09-29T00:00:00Z Text Journal contribution 10.1021/acs.inorgchem.6c04041.s001 https://figshare.com/articles/journal_contribution/Coupling_Self-Sensitized_CO_sub_2_sub_Photoreduction_of_Silicon_IV_-Terpyridine_Complexes_with_Organic_Synthesis/34028749 CC BY-NC 4.0