期刊
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
卷 34, 期 15, 页码 6492-6504出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2009.05.137
关键词
Hydrogen purification; Reverse-selective membrane; Cross-linked network; PEO; Silica
资金
- Singapore National Research Foundation (NRF) [R-279-000-261-281, R-398-000-058-305]
- Specialized Research Fund for the Doctoral Program of Higher Education [20070213004]
- Harbin Science and Technology Innovation Talent Funds [2006RFLXG015]
- The Scientific Research Foundation for the Returned Oversea Chinese Scholars, State Education Ministry
Targeting at hydrogen purification, cross-linked organic-inorganic reverse-selective membranes containing poly(ethylene oxide) (PEO) are fabricated in situ by using functional oligomers (O,O'-bis(2-aminopropyl) polypropylene glycol-block-polyethylene glycol-block-polypropylene glycol: Jeffamine (R) ED-2003) with a high content of PEO and epoxy-functional silanes (3-glycidyloxypropyltrimethoxysilane: GOTMS). Changes in physicochemical properties due to varying silica content have been characterized; including a great decline in melting temperature; an improvement in glassy and degradation temperature, and the suppression of PEO crystallinity. The strong affinity between quadrupolar CO2 and polar ethylene oxide (EO) groups enhances the CO2/H-2 separation performance of hybrid membranes, which can be further tuned by controlling the organic/inorganic ratio. The organic-inorganic hybrid membrane with 90 wt% of ED-2003 demonstrates an appealing CO2 permeability of 367 Barrer with an attractive CO2/H-2 selectivity of 8.95 at 3.5 atm and 35 degrees C. The transport performance trend with composition variations is explained by analyzing the calculated solubility and diffusivity based on the solution-diffusion mechanism. Moreover, CO2 permeability increases with applied pressure in pure gas tests because Of CO2 plasticization phenomena, which is beneficial for CO2/H-2 separation. Attributing to CO2 plasticization and CO2 dominant sorption, the mixed gas test results of the membrane containing only 25 wt% ED-2003 show greatly improved CO2/H-2 selectivity of 13.2 with CO2 permeability of 148 Barrer at 35 degrees C compared to pure gas results. Interestingly, at a stipulated CO2 pressure, the inherent tension in cross-linked networks maintains the CO2 permeability stable with the time. The cross-linked organic-inorganic membranes with enhancements in mechanical and thermal proper-ties are promising for industrial-scale hydrogen purification. (C) 2009 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved.
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