羰基化
二胺
基质(水族馆)
化学
催化作用
光催化
光化学
配体(生物化学)
分子
表面改性
作者
Yingcong Wei,Wenying Zha,Lu Wang,Xiongfeng Ma,Shaohui Zhang,Rongjian Sa,Huaxiang Lin,Zhengxin Ding,Jinlin Long,Xianzhi Fu,Rusheng Yuan
标识
DOI:10.1016/j.apcatb.2022.121103
摘要
Tailoring the surficial chemical environment of two-dimensional materials by organic modification is an effective way to optimize their catalytic behaviors. Herein, we present a dynamic coordination approach to improve the photocatalytic performance of ultrathin Co 2 CO 3 (OH) 2 nanosheets (u-CoCH) in NIR light (λ > 780 nm) driven carbonylation reaction by using the reacting substrates (diamines) as the ligands. The coordination of diamines with surface Co 2+ ions form a binuclear complex at the crystallographic planes of u-CoCH. The as-formed complexes can reduce the energy barrier of carbonylation reaction by weaking the N-H bond of the substrate on u-CoCH, and afford enhanced light response as well as the prolonged photogenerated electron lifetime. Together with the successful synthesis of a series of important structural motifs in pharmaceuticals and bioactive agents, the promoted photosynthesis reaction mode via in-situ formed surface complexes offers a model toward full-spectrum-solar-energy conversion in the field of chemical synthesis. • Diamines act as substrate and ligand to tailor the surficial chemical environment of CoCO 3 (OH) 2 nanosheets. • The surface adjacent Co 2+ ions binding to diamine molecules form a binuclear complex. • The complexes enhanced light absorption ability and reduced the energy barrier of carbonylation by weaking the N-H bonds. • A protocol for accessing cyclic ureas through NIR light driven carbonylation of diamine with CO over CoCO 3 (OH) 2 .
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