Fu Chengyu, Du Jiehao, Shi Na, Yang Limeng, Che Qiuling, Zhang Pengfei
School of Textile Science and Engineering, Xi'an Polytechnic University, 19 Jinhua Road, Xi'an, 710048, Shaanxi, China.
Key Laboratory of Functional Textile Material and Product (Xi'an Polytechnic University), Ministry of Education, Xi'an, 710048, Shaanxi, China.
Sci Rep. 2024 Aug 2;14(1):17947. doi: 10.1038/s41598-024-68319-5.
C-H bond activation under mild conditions remains a great challenge in the chemical industry, while catalytic cyclohexane oxidation is inefficient and often requires organic solvents and strong oxidants. This study constructed a CN/WO Z-type heterojunction catalyst to efficiently convert cyclohexane into cyclohexanone and cyclohexanol (KA oil) through aqueous phase oxidation by O under visible light irradiation. With strong redox performance and high photogenerated carrier separation ability, the proposed composite catalyst can produce the key active species for cyclohexane oxidation in the HO-O system. The reaction mechanism was clarified through experiment and DFT theory calculation. Cyclohexane was converted into cyclohexyl radical under the action of ·OH, and ·O converted most products into cyclohexanone. The catalyst can be recycled under optimized process conditions while reaching a KA oil yield of 139.73 μmol g h and a selectivity of 93.1%.
在温和条件下实现C-H键活化在化学工业中仍然是一个巨大的挑战，而催化环己烷氧化效率低下，且通常需要有机溶剂和强氧化剂。本研究构建了一种CN/WO Z型异质结催化剂，通过在可见光照射下利用O进行水相氧化，将环己烷高效转化为环己酮和环己醇（KA油）。所提出的复合催化剂具有很强的氧化还原性能和高光生载流子分离能力，能够在HO-O体系中产生用于环己烷氧化的关键活性物种。通过实验和DFT理论计算阐明了反应机理。环己烷在·OH的作用下转化为环己基自由基，而·O将大部分产物转化为环己酮。该催化剂在优化的工艺条件下可以循环使用，同时KA油产率达到139.73 μmol g h，选择性为93.1%。
