文献类型：期刊文献

英文题名：Separation of SO2and NO2with the Zeolite Membrane: Molecular Simulation Insights into the Advantageous NO2Dimerization Effect

作者：Liu, Yingshu[1]; Zuo, Jiayu[1]; Li, Ziyi[1]; Li, Jun[1]; Zou, Xiaoqin[2]; Yang, Xiong[1]; Yang, Bentao[3]; Zhang, Chuanzhao[4]; Wang, Haoyu[4]; Pui, David Y. H.[5]; Yang, Ralph T.[6]

第一作者：Liu, Yingshu

机构：[1] School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing, 100083, China; [2] Faculty of Chemistry, Northeast Normal University, Changchun, 130024, China; [3] Zhongye Changtian International Engineering Co., Ltd., Changsha, 410205, China; [4] College of Biochemical Engineering, Beijing Union University, Beijing, 100023, China; [5] Mechanical Engineering, University of Minnesota, 111 Church Street, S.E., Minneapolis, MN, 55455, United States; [6] Department of Chemical Engineering, University of Michigan, Ann Arbor, MI, 48109-2136, United States

第一机构：School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing, 100083, China

通讯机构：[1]School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing, 100083, China

年份：2022

卷号：38

期号：9

起止页码：2751-2762

外文期刊名：Langmuir

收录：EI(收录号：20221011761676);Scopus(收录号：2-s2.0-85125815744)

语种：英文

外文关键词：Molecular structure - Nitrogen oxides - Adsorption - Temperature distribution - Zeolites - Molecular dynamics - Separation

摘要：NO2and SO2, as valuable chemical feedstock, are worth being recycled from flue gases. The separation of NO2and SO2is a key process step to enable practical deployment. This work proposes SO2separation from NO2using chabazite zeolite (SSZ-13) membranes and provides insights into the feasibility and advantages of this process using molecular simulation. Grand canonical ensemble Monte Carlo and equilibrium molecular dynamics methods were respectively adopted to simulate the adsorption equilibria and diffusion of SO2, NO2, and N2O4on SSZ-13 at varying Si/Al (1, 5, 11, 71, +∞), temperatures (248-348 K), and pressures (0-100 kPa). The adsorption capacity and affinity (SO2> N2O4> NO2) demonstrated strong competitive adsorption of SO2based on dual-site interactions and significant reduction in NO2adsorption due to dimerization in the ternary gas mixture. The simulated order of diffusivity (NO2> SO2> N2O4) on SSZ-13 demonstrated rapid transport of NO2, strong temperature dependence of SO2diffusion, and the impermeability of SSZ-13 to N2O4. The membrane permeability of each component was simulated, rendering a SO2/NO2membrane separation factor of 26.34 which is much higher than adsorption equilibrium (6.9) and kinetic (2.2) counterparts. The key role of NO2-N2O4dimerization in molecular sieving of SO2from NO2was addressed, providing a facile membrane separation strategy at room temperature. ? 2022 American Chemical Society. All rights reserved.