Exfoliated metal oxide ultrathin nanosheets with supported Pd nanoparticles enabling the one-pot reaction of phenol into caprolactam

作     者：Xiaomeng Cheng Bingfeng Chen Lei Zhang Tianjiao Wang Sen Luan Yang Sun Huizhen Liu Buxing Han 

作者机构：Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences School of Chemistry and Chemical Engineering University of Chinese Academy of Sciences Shanghai Key Laboratory of Green Chemistry and Chemical Processes State Key Laboratory of Petroleum Molecular & Process EngineeringSchool of Chemistry and Molecular Engineering East China Normal University 

出 版 物：《Science China Chemistry》 (中国科学:化学(英文版))

年 卷 期：2025年第68卷第6期

页      面：2636-2643页

核心收录：

学科分类：081702[工学-化学工艺] 081705[工学-工业催化] 07[理学] 070205[理学-凝聚态物理] 08[工学] 0817[工学-化学工程与技术] 080501[工学-材料物理与化学] 0805[工学-材料科学与工程（可授工学、理学学位）] 0702[理学-物理学] 

基　　金：supported by the National Key Research and Development Program of China (2022YFA1504901, 2023YFA1508103) the National Natural Science Foundation of China (22293012, 22179132, 22293015, 22121002) 

主　　题：two-dimensional oxides ultrathin nanosheets bifunctional catalysts tandem reaction caprolactam 

摘      要：Two-dimensional（2D） oxide nanomaterials have great potential for various applications but face challenges due to strong interlayer interactions. In this work, we propose a novel and facile method to exfoliate layered transition metal oxides into ultrathin nanosheets functionalized with phosphate species by the combination of ball-milling and liquid-exfoliation with phosphoric acid. The resulting HNb Mo O6nanosheets with supported Pd nanoparticles displayed excellent catalytic performance in the one-pot conversion of phenol into caprolactam（CPL）, achieving a yield of up to 71.9%. This one-pot route avoids the energy-intensive intermediate separation process in conventional multi-step approaches to CPL. The superior catalytic performance of the catalysts is attributed to the tunable Br?nsted acid/Lewis acid ratio and readily accessible active sites on the ultrathin nanosheets. This research demonstrates a new methodology for constructing ultrathin nanosheets and preparing bifunctional catalysts for tandem reactions, which opens the way for one-pot production of CPL.