文献类型：期刊文献

英文题名：A dynamic reaction density functional theory for interfacial reaction-diffusion coupling at nanoscale

作者：Tang, Weiqiang[1,2];Yu, Hongping[1,2];Zhao, Teng[1,2];Qing, Leying[1,2];Xu, Xiaofei[1,2];Zhao, Shuangliang[1,2,3]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200237, Peoples R China;[3]Guangxi Univ, Sch Chem & Chem Engn, Guangxi Key Lab Petrochem Resource Proc & Proc In, Nanning 530004, Peoples R China

年份：2021

卷号：236

外文期刊名：CHEMICAL ENGINEERING SCIENCE

收录：;EI(收录号：20210909988482);WOS:【SCI-EXPANDED(收录号:WOS:000632967400008)】；

基金：This work is supported by National Natural Science Foundation of China (Nos. 21878078, 91934302, and 21978079) , and the Dean Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology.

语种：英文

外文关键词：Classical density functional theory; Reaction-diffusion; Interfacial reaction; Nanoscale

摘要：Reaction-diffusion (RD) coupling lies in the heart of chemical engineering. Due to the inherent density inhomogeneity of interfacial systems, the existing continuum approaches for quantifying the coupling between reaction and diffusion do not translate into interfacial systems, which highlights the urgent need for developing new methods to describe the RD coupling at nanoscale. In this work, a dynamic reaction density functional theory (DRxDFT) is proposed by combining the classical dynamic DFT for describing reactant/product diffusion with the reaction collision theory for addressing chemical reaction. For demonstrating its applicability to interfacial systems, the DRxDFT is hereafter applied to investigate an irreversible model reaction A + 2B ? 2C on a catalytic substrate, and the effects of temperature, substrate adsorption strength, reactant concentration, diffusion coefficient, and reaction activation energy on reaction efficiency are examined. The calculated results show that the enhancement of reaction efficiency weakly depends on the unilateral increase of reaction or diffusion rate, but is strongly determined by the incensement of the coupled degree of reaction and diffusion. The proposed theory provides a promising tool for guiding the optimization and intensification of interfacial RD processes. (c) 2021 Elsevier Ltd. All rights reserved.