Understanding the mechanism of hydrogen transport in imidazolyl polymers doped Nafion membranes via molecular dynamics simulations: Case of PVMZ/Nafion

被引:2
|
作者
Han, Zhiyue [1 ]
Pei, Supeng [1 ]
Yu, Chunyang [2 ,3 ]
Zhou, Yongfeng [2 ,3 ]
机构
[1] Shanghai Inst Technol, Sch Chem & Environm Engn, Shanghai 201418, Peoples R China
[2] Shanghai Jiao Tong Univ, Frontiers Sci Ctr Transformat Mol, Sch Chem & Chem Engn, Shanghai Key Lab Elect Insulat & Thermal Aging, Shanghai 200240, Peoples R China
[3] Chinese Acad Sci, Key Lab Green & High End Utilizat Salt Lake Resour, Xining 810008, Peoples R China
关键词
Nafion composite membranes; Hydrogen transport; Molecular dynamics simulations; PERFLUOROSULFONIC ACID POLYMER; PROTON-EXCHANGE MEMBRANES; SIDE-CHAIN LENGTH; HIGH-TEMPERATURE; ATOMISTIC SIMULATION; OXYGEN-TRANSPORT; PROGRAM PACKAGE; WATER-SORPTION; GAS-CROSSOVER; PERMEATION;
D O I
10.1016/j.ijhydene.2024.05.398
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Decreasing gas penetration has noticeable effects on the durability and performance of Nafion based proton exchange membranes (PEMs). Experimental studies showed that adding imidazolyl groups into Nafion could reduce the hydrogen permeation in the membrane, while causing the substantial increase in power density. Nonetheless, the microscopic mechanism of doping on the reduction of hydrogen permeation is remain unclear. In this work, molecular dynamics simulation was performed to understand the transport behaviors of hydrogen in polyvinylimidazole (PVMZ)/Nafion composite membranes at the molecular level. The simulation results indicate that there are different degrees of effects about the polymer phase and aqueous domain on the diffusion kinetics of hydrogen in Nafion and PVMZ/Nafion at low and high hydration levels. With the increase of water content, the hydrogen molecules will migrate from the polymer phase to the polymer/water interface in Nafion and PVMZ/Nafion membranes. At low water content, the more free volume and the more pores in Nafion membrane are conducive to the diffusion of hydrogen than that in PVMZ/Nafion membrane to a greater extent. For the aqueous domain, the smaller and the rougher surface of water clusters in PVMZ/Nafion membranes have a certain limiting effect on the diffusion of hydrogen molecules than that in Nafion membranes at high water content. Consequently, at low water contents (lambda <= 9), the self-diffusion coefficient of hydrogen (DH2) increases slowly from 0.55 to 1.01 ( x 10-5 cm2/s) in Nafion membrane and from 0.26 to 0.53 ( x 10-5 cm2/s) in PVMZ/ Nafion membrane. In contrast, at high water contents (lambda >= 9), the DH2 increases rapidly from 1.01 to 2.35 ( x 10-5 cm2/s) in Nafion membranes and from 0.53 to 1.74 ( x 10-5 cm2/s) in PVMZ/Nafion membranes. The current work can provide a fundamental understanding for experimentally designing new type Nafion based PEMs for hydrogen fuel cells.
引用
收藏
页码:437 / 448
页数:12
相关论文
共 38 条
  • [21] Dynamics of water and solute transport in polymeric reverse osmosis membranes via molecular dynamics simulations
    Shen, Meng
    Keten, Sinan
    Lueptow, Richard M.
    JOURNAL OF MEMBRANE SCIENCE, 2016, 506 : 95 - 108
  • [22] Study on the transport performance degradation of Nafion membrane due to the presence of Na+ and Ca2+ using molecular dynamics simulations
    Zhang, Guoling
    Yang, Guogang
    Shen, Qiuwan
    Li, Shian
    Li, Zheng
    Liao, Jiadong
    Jiang, Ziheng
    Wang, Hao
    Zhang, Hongpeng
    Ye, Weiqiang
    JOURNAL OF POWER SOURCES, 2022, 542
  • [23] Virtually imprinted polymers (VIPs): understanding molecularly templated materials via molecular dynamics simulations
    Zink, S.
    Moura, F. A.
    Alves da Silva Autreto, P.
    Galvao, D. S.
    Mizaikoff, B.
    PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2018, 20 (19) : 13145 - 13152
  • [24] Nature of water transport and electro-osmosis in nafion: Insights from first-principles molecular dynamics simulations under an electric field
    Choe, Yoong-Kee
    Tsuchida, Eiji
    Ikeshoji, Tamio
    Yamakawa, Shunsuke
    Hyodo, Shi-aki
    JOURNAL OF PHYSICAL CHEMISTRY B, 2008, 112 (37): : 11586 - 11594
  • [25] Understanding the temperature effect on transport dynamics and structures in polyamide reverse osmosis system via molecular dynamics simulations
    Li, Ke
    Liu, Lifen
    Wu, Hao
    Li, Shanlong
    Yu, Chunyang
    Zhou, Yongfeng
    Huang, Wei
    Yan, Deyue
    PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2018, 20 (47) : 29996 - 30005
  • [26] Dynamic Mechanism of Fatty Acid Transport across Cellular Membranes through FadL: Molecular Dynamics Simulations
    Zou, Hanjun
    Zheng, Mingyue
    Luo, Xiaomin
    Zhu, Weiliang
    Chen, Kaixian
    Shen, Jianhua
    Jiang, Hualiang
    JOURNAL OF PHYSICAL CHEMISTRY B, 2008, 112 (41): : 13070 - 13078
  • [27] Mixed Grotthuss and Vehicle Transport Mechanism in Proton Conducting Polymers from Ab initio Molecular Dynamics Simulations
    Luduena, Guillermo A.
    Kuehne, Thomas D.
    Sebastiani, Daniel
    CHEMISTRY OF MATERIALS, 2011, 23 (06) : 1424 - 1429
  • [28] Hop, Skip, and Jump: Hydrogen Molecular Transport through Amorphous Polyethylene Matrices Studied via Molecular Dynamics Simulations
    Divine-Ayela, Candice
    Perez, Felipe
    Striolo, Alberto
    INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2023, 62 (46) : 19893 - 19906
  • [29] Comment on "Mixed Grotthuss and Vehicle Transport Mechanism in Proton Conducting Polymers from Ab initio Molecular Dynamics Simulations"
    Vilciauskas, Linas
    Kreuer, Klaus-Dieter
    CHEMISTRY OF MATERIALS, 2011, 23 (14) : 3377 - 3378
  • [30] Understanding the transport mechanism of seawater through FMOF-1 and its derivative via molecular dynamics simulation
    Chen, Eryu
    Jia, Lingjie
    Chen, Chen
    Huang, Fang
    Zhang, Li
    JOURNAL OF MOLECULAR LIQUIDS, 2021, 325