文献类型：期刊文献

英文题名：Product-feedback in the molecular interaction-based reaction–diffusion coupling system

作者：Shen, Xucheng[1]; Shen, Yueqiu[2]; Tang, Weiqiang[1]; Xu, Xiaofei[1]; Zhao, Shuangliang[2]

机构：[1] State Key Laboratory of Chemical Engineering and School of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China; [2] State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, and School of Chemistry and Chemical Engineering, Guangxi University, Nanning, 530004, China

年份：2025

卷号：422

外文期刊名：Journal of Molecular Liquids

收录：EI(收录号：20250417724450)

语种：英文

摘要：This work presents an extension of the dynamic reaction density functional theory (DRxDFT) to explore the impact of adsorbate interactions, particularly excluded volume and electrostatic effects, on a unimolecular catalytic reaction (A → B) at a catalytic substrate. The limitations of traditional reaction–diffusion models are addressed by incorporating both steric and electrostatic effects into DRxDFT, in contrast to the models which often ignore structural inhomogeneity and diffusivity variations. The DRxDFT model is validated against the Poisson-Nernst-Planck model with reaction source term and is used to explore the impacts of ion valence, bulk density, surface adsorption affinity, and external electric fields on reaction efficiency. The results demonstrate that reaction efficiency is significantly influenced by adsorbate interactions, and that the ion valence of reactants and products, bulk fluid density, and surface affinity alter the coupling between reaction and diffusion. Furthermore, external electric fields have been shown to modulate reaction dynamics by affecting reactant adsorption. The findings of this work suggest that a nuanced consideration of steric and electrostatic interactions is crucial for accurately modeling reaction–diffusion systems and optimizing catalytic performance. ? 2025 Elsevier B.V.