SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2021, Vol. 36 ›› Issue (8): 67-75.DOI: 10.1016/j.cjche.2020.09.003

• Separation Science and Engineering • 上一篇    下一篇

Fabrication of Pd-Nb bimetallic doped organosilica membranes by different metal doping routes for H2/CO2 separation

Hengfei Zhang1, Yibin Wei1, Shufeng Niu2, Hong Qi1   

  1. 1 State Key Laboratory of Material-Oriented Chemical Engineering, Membrane Science and Technology Research Center, Nanjing Tech University, Nanjing 210009, China;
    2 Hongyi Ceramic Membranes Research Institute, Nanjing Hongyi Ceramic Nanofiltration Membranes Co., Ltd., Nanjing 210009, China
  • 收稿日期:2020-06-08 修回日期:2020-08-16 出版日期:2021-08-28 发布日期:2021-09-30
  • 通讯作者: Hong Qi
  • 基金资助:
    This work is supported by the National Natural Science Foundation of China (21490581), China Petroleum & Chemical Corporation (317008-6) and Guangxi Innovation Driven Development Foundation (AA17204092).

Fabrication of Pd-Nb bimetallic doped organosilica membranes by different metal doping routes for H2/CO2 separation

Hengfei Zhang1, Yibin Wei1, Shufeng Niu2, Hong Qi1   

  1. 1 State Key Laboratory of Material-Oriented Chemical Engineering, Membrane Science and Technology Research Center, Nanjing Tech University, Nanjing 210009, China;
    2 Hongyi Ceramic Membranes Research Institute, Nanjing Hongyi Ceramic Nanofiltration Membranes Co., Ltd., Nanjing 210009, China
  • Received:2020-06-08 Revised:2020-08-16 Online:2021-08-28 Published:2021-09-30
  • Contact: Hong Qi
  • Supported by:
    This work is supported by the National Natural Science Foundation of China (21490581), China Petroleum & Chemical Corporation (317008-6) and Guangxi Innovation Driven Development Foundation (AA17204092).

摘要: Monometallic doping has proved its superiority in improving either permselectivity or H2 permeability of organosilica membranes for H2/CO2 separation, but it is still challenging to break the trade-off effect. Herein, we report a series of Pd-Nb bimetallic doped 1,2-bis(triethoxysilyl)ethane (Pd-Nb-BTESE, PNB) membranes with different metal doping routes for simultaneously improving H2 permeance and H2/CO2 permselectivity by the synergetic effects of Pd and Nb. The doped Pd can exist in the BTESE network as nanoparticles while the doped Nb is incorporated into BTESE network forming Nb-O-Si covalent bonds. The metal doping routes significantly influence the microstructure of PNB networks and gas separation performance of the PNB membranes. We found that the PNB membrane with Pd doping priority (PNB-Pd) exhibited the highest surface area and pore volume, comparing with Nb doping priority (PNB-Nb) or Pd-Nb simultaneous doping (PNB-PdNb). The PNB-Pd membrane could not only exhibit an excellent H2 permeance of ~10-6 mol·m-2·s-1·Pa-1 but also a high H2/CO2 permselectivity of 17.2. Our findings may provide novel insights into preparation of bimetallic doped organosilica membranes with excellent H2/CO2 separation performance.

关键词: Hydrogen, Separation, Membranes, Bimetallic doping, Organosilica

Abstract: Monometallic doping has proved its superiority in improving either permselectivity or H2 permeability of organosilica membranes for H2/CO2 separation, but it is still challenging to break the trade-off effect. Herein, we report a series of Pd-Nb bimetallic doped 1,2-bis(triethoxysilyl)ethane (Pd-Nb-BTESE, PNB) membranes with different metal doping routes for simultaneously improving H2 permeance and H2/CO2 permselectivity by the synergetic effects of Pd and Nb. The doped Pd can exist in the BTESE network as nanoparticles while the doped Nb is incorporated into BTESE network forming Nb-O-Si covalent bonds. The metal doping routes significantly influence the microstructure of PNB networks and gas separation performance of the PNB membranes. We found that the PNB membrane with Pd doping priority (PNB-Pd) exhibited the highest surface area and pore volume, comparing with Nb doping priority (PNB-Nb) or Pd-Nb simultaneous doping (PNB-PdNb). The PNB-Pd membrane could not only exhibit an excellent H2 permeance of ~10-6 mol·m-2·s-1·Pa-1 but also a high H2/CO2 permselectivity of 17.2. Our findings may provide novel insights into preparation of bimetallic doped organosilica membranes with excellent H2/CO2 separation performance.

Key words: Hydrogen, Separation, Membranes, Bimetallic doping, Organosilica