文献类型：期刊文献

英文题名：Molecular interaction-based reaction-diffusion coupling within catalytic nanochannels

作者：Yu, Hongping[1];Tang, Weiqiang[1];Xu, Xiaofei[1];Zhao, Shuangliang[1,2]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Guangxi Univ, Sch Chem & Chem Engn, Guangxi Key Lab Petrochem Resource Proc & Proc Int, Nanning 530004, Peoples R China

年份：2023

卷号：386

外文期刊名：JOURNAL OF MOLECULAR LIQUIDS

收录：;EI(收录号：20232914401606);WOS:【SCI-EXPANDED(收录号:WOS:001046487100001)】；

基金：This work is supported by the National Natural Science Foundation of China (Nos. 21878078, 21978079, and 22108070) , the Guangxi Science and Technology Base and Talent Special Project (No. AD21220017) , the China Postdoctoral Science Foundation (No. 2021M691008) , and the Young Elite Scientists Sponsorship Program by CAST (No. 2022QNRC001) .

语种：英文

外文关键词：Reaction-diffusion coupling; Catalytic nanochannel; Dynamic reaction density functional theory; Local diffusion coefficient

摘要：The nanoconfinement effect on the inner reaction-diffusion coupling is significant, while the underlying common principle remains ambiguous, which is mainly attributed to the lack of a feasible model. Herein, the dynamic reaction density functional theory (DRxDFT) is extended, by involving the position-dependent local diffusion coefficient, to investigate the reaction-diffusion coupling of an irreversible unimolecular isothermal reaction within catalytic nanochannels. The local diffusion coefficient is jointly determined by the pore size and local density. For demonstration, the reaction-diffusion in a rectangle nanochannel is studied by means of DRxDFT, and the predicted steady-state productivities are in excellent agreement with reactive molecular dynamics simulations. The DRxDFT is further applied to analyze the RD coupling within generic catalytic nanochannels. Towards this end, a microscopic effectiveness factor is introduced to identify the dominant role in the competition between reaction and diffusion, with which it is found that the effect of nanochannel size on productivity exhibits a generic opposite trend under reaction-dominated and diffusion-dominated conditions. This work provides a microscopic insight into the coupling of reaction and diffusion in nanoconfinement.