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利用无贵金属双(三联吡啶)铁(II)配合物和有机光敏剂实现水辅助高效光催化将CO还原为CO

Water-Assisted Highly Efficient Photocatalytic Reduction of CO to CO with Noble Metal-Free Bis(terpyridine)iron(II) Complexes and an Organic Photosensitizer.

作者信息

Wang Yanan, Liu Ting, Chen Longxin, Chao Duobin

机构信息

School of Materials Science and Chemical Engineering, Ningbo University, Ningbo, Zhejiang 315211, China.

出版信息

Inorg Chem. 2021 Apr 19;60(8):5590-5597. doi: 10.1021/acs.inorgchem.0c03503. Epub 2021 Feb 21.

Abstract

Photocatalytic CO reduction reaction is believed to be a promising approach for CO utilization. In this work, a noble metal-free photocatalytic system, composed of (terpyridine)iron(II) complexes and an organic thermally activated delayed fluorescence compound, has been developed for selective reduction of CO to CO with a maximum turnover number up to 6320, 99.4% selectivity, and turnover frequency of 127 min under visible-light irradiation in dimethylformamide/HO solution. More than 0.3 mmol CO was generated using 0.05 μmol catalyst after 2 h of light irradiation. The apparent quantum yield was found to be 9.5% at 440 nm (180 mW cm). Control experiments and UV-vis-NIR spectroscopy studies further demonstrated that water strongly promoted the photocatalytic cycle and terpyridine ligands rather than Fe(II) were initially reduced during the photocatalytic process.

摘要

光催化CO还原反应被认为是一种很有前景的CO利用方法。在这项工作中,已经开发出一种由(三联吡啶)铁(II)配合物和一种有机热活化延迟荧光化合物组成的无贵金属光催化体系,用于在二甲基甲酰胺/H₂O溶液中可见光照射下将CO选择性还原为CO,最大周转数高达6320,选择性为99.4%,周转频率为127 min⁻¹。光照2小时后,使用0.05 μmol催化剂产生了超过0.3 mmol的CO。在440 nm(180 mW cm⁻²)处发现表观量子产率为9.5%。对照实验和紫外-可见-近红外光谱研究进一步表明,水强烈促进了光催化循环,并且在光催化过程中三联吡啶配体而非Fe(II)最初被还原。

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