Xie, Mingyue; Wu, Yong; Gu, Hao; Peng, Yuhao; Zhang, Shan; Wang, Feng Ryan; Xiao, Wei; Xie, Mingyue; Wu, Yong; Gu, Hao; Peng, Yuhao; Zhang, Shan; Wang, Feng Ryan; Xiao, Wei; Gu, Dong; - view fewer (2025) Refining the Distinct Cu–N₄ Coordination in Mesoporous N-Doped Carbon to Boost Selective Deuteration under Mild Conditions. ACS Applied Materials & Interfaces 10.1021/acsami.4c21167. (In press).

Text Wang_2025 ACS AMI Manuscript-revised2.pdf Access restricted to UCL open access staff until 11 January 2026. Download (1MB)

Abstract

Deuterated compounds have broad applications across various fields, with dehalogenative deuteration serving as an efficient method to obtain these molecules. However, the diverse electronic structures of active sites in the heterogeneous system and the limited recyclability in the homogeneous system significantly hinder the advancement of dehalogenative deuteration. In this study, we present a catalyst composed of copper single-atom sites anchored within an ordered mesoporous nitrogen-doped carbon matrix, synthesized via a mesopore confinement method. The Cu1/OMNC-1100 catalyst, characterized by Cu–N₄ sites, demonstrates exceptional performance, high functional group tolerance, and remarkable durability in the deuteration of 2-bromo-6-methoxynaphthalene under relatively mild conditions (80 °C, 2 MPa of CO). Experimental results combined with X-ray absorption fine structure analysis reveal that Cu–N₃ sites can be converted into more stable Cu–N₄ counterparts at higher pyrolysis temperatures, resulting in enhanced catalytic activity. This work demonstrates a strategy for designing single-atom site catalysts with tunable coordination environments, providing a promising approach to improving catalytic performance in selective dehalogenative reactions under relatively mild conditions.

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