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揭示光催化中痕量金属的显著存在:探索铁杂质效应。

Unraveling the Prominent Existence of Trace Metals in Photocatalysis: Exploring Iron Impurity Effects.

作者信息

Huang Yahao, Wang Miao, Liu Wei, Wu Qiang, Hu Peng

机构信息

Institute of Green Chemistry and Molecular Engineering, GBRCE for Functional Molecular Engineering, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-Sen University, Guangzhou 510006, P. R. China.

出版信息

J Org Chem. 2024 Mar 15;89(6):4156-4164. doi: 10.1021/acs.joc.4c00155. Epub 2024 Mar 7.

Abstract

Metal impurities can complicate the identification of active catalyst species in transition metal catalysis and electrocatalysis, potentially leading to misleading findings. This study investigates the influence of metal impurities on photocatalysis. Specifically, the photocatalytic reaction of inert alkanes using chlorides without the use of an external photocatalyst was studied, achieving successful C(sp)-H functionalization. The observations reveal that Fe and Cu impurities are challenging to avoid in a typical laboratory environment and are prominently present in normal reaction systems, and iron impurities play a dominant role in the aforementioned apparent 'metal-free' reaction. Additionally, iron exhibits significantly higher catalytic activity compared to Cu, Ce, and Ni at low metal concentrations in the photocatalytic C(sp)-H functionalization using chlorides. Considering the widespread presence of Fe and Cu impurities in typical laboratory environments, this study serves as a reminder of their involvement in reaction processes.

摘要

金属杂质会使过渡金属催化和电催化中活性催化剂物种的鉴定变得复杂,可能导致误导性的研究结果。本研究调查了金属杂质对光催化的影响。具体而言,研究了在不使用外部光催化剂的情况下,利用氯化物对惰性烷烃进行的光催化反应,实现了成功的C(sp)-H官能化。观察结果表明,在典型的实验室环境中难以避免铁和铜杂质,且它们在正常反应体系中显著存在,并且铁杂质在上述明显的“无金属”反应中起主导作用。此外,在使用氯化物进行光催化C(sp)-H官能化时,在低金属浓度下,铁的催化活性明显高于铜、铈和镍。鉴于典型实验室环境中铁和铜杂质的普遍存在,本研究提醒人们注意它们在反应过程中的参与情况。

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