文献类型：期刊文献

英文题名：Separation of SO2 and NO2 with the Zeolite Membrane: Molecular Simulation Insights into the Advantageous NO2 Dimerization 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

通讯作者：Li, ZY[1]

机构：[1]Univ Sci & Technol Beijing, Sch Energy & Environm Engn, Beijing 100083, Peoples R China;[2]Northeast Normal Univ, Fac Chem, Changchun 130024, Peoples R China;[3]Zhongye Changtian Int Engn Co Ltd, Changsha 410205, Peoples R China;[4]Beijing Union Univ, Coll Biochem Engn, Beijing 100023, Peoples R China;[5]Univ Minnesota, Mech Engn, Minneapolis, MN 55455 USA;[6]Univ Michigan, Dept Chem Engn, Ann Arbor, MI 48109 USA

第一机构：Univ Sci & Technol Beijing, Sch Energy & Environm Engn, Beijing 100083, Peoples R China

通讯机构：[1]corresponding author), Univ Sci & Technol Beijing, Sch Energy & Environm Engn, Beijing 100083, Peoples R China.

年份：2022

卷号：38

期号：9

起止页码：2751-2762

外文期刊名：LANGMUIR

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000771993300001)】；

基金：The authors would like to express the gratitude to the National Natural Science Foundation of China (no. 21808012), the Fundamental Research Funds for the Central Universities (nos. FRF-IDRY-19-025 and FRF-TP-20-011A2), and the Scientific Research Project of Beijing Educational Committee (no. KM202011417007). The computation is completed using Shenzhen supercomputer in the National Supercomputing Center.

语种：英文

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

摘要：NO2 and SO2, as valuable chemical feedstock, are worth being recycled from flue gases. The separation of NO2 and SO2 is a key process step to enable practical deployment. This work proposes SO2 separation from NO2 using 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 N2O4 on SSZ-13 at varying Si/Al (1, 5, 11, 71, +infinity), temperatures (248-348 K), and pressures (0-100 kPa). The adsorption capacity and affinity (SO2 > N2O4 > NO2) demonstrated strong competitive adsorption of SO2 based on dual-site interactions and significant reduction in NO2 adsorption 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 SO2 diffusion, and the impermeability of SSZ-13 to N2O4. The membrane permeability of each component was simulated, rendering a SO2/NO2 membrane separation factor of 26.34 which is much higher than adsorption equilibrium (6.9) and kinetic (2.2) counterparts. The key role of NO2-N2O4 dimerization in molecular sieving of SO2 from NO2 was addressed, providing a facile membrane separation strategy at room temperature.