Rational design, synthesis, and characterization of facilitated transport membranes exhibiting enhanced permeability, selectivity and stability
Rational design, synthesis, and characterization of facilitated transport membranes exhibiting enhanced permeability, selectivity and stability
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DOI：
10.1016/j.memsci.2023.121910
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发表时间：
2023-11
影响因子：
9.5
通讯作者：
Matthew T. Webb;Lucas C. Condes;Harold G. Ly;M. Galizia;Sepideh Razavi
中科院分区：
文献类型：
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作者：
Matthew T. Webb;Lucas C. Condes;Harold G. Ly;M. Galizia;Sepideh Razavi
尽管在短时间内优于常规聚合物膜，但促进传递膜（FTM）易于发生光/化学老化，这导致其性能迅速衰减。此外，当嵌入聚合物材料中以制造混合基质膜时，可能在金属-聚合物界面处形成结构缺陷，导致选择性损失。为了克服这些问题，已经使用不同分子量的4，4 '-氧代二苯二甲酸酐（ODPA）和Jeffamine单体合成了一系列聚酰胺酸（PAA），并用于通过与银离子的螯合反应来制备银纳米颗粒，以尝试成功地i）实现无缺陷的混合基质膜（MMM），ii）靶向CO2选择性传输，以及iii）增强长期稳定性。证实了银和PAA之间发生螯合反应，结果，获得了单个和未聚集的PAA涂覆的银纳米颗粒，并将其掺入商业聚合物Pebax 1657中，以制造无缺陷的混合基质膜。系统地研究了聚丙烯酸长度和醚官能团浓度对所得混合基质膜结构和性能的影响。值得注意的是，相对于纯聚合物，Pebax中仅包含2wt%的纳米颗粒使CO2渗透性提高了50%，CO2选择性提高了100%。的吸附和扩散系数进行了详细的分析，以阐明所观察到的膜性能的分子起源。最后，初步数据表明，新合成的材料在暴露于纯H2时表现出高的化学稳定性。
Despite outperforming conventional polymer membranes in the short time frame, facilitated transport membranes (FTMs) are prone to photo/chemical aging, which causes a rapid decay of their performance. Moreover, when embedded in polymer materials to fabricate mixed matrix membranes, structural defects may form at the metal-polymer interface, causing a selectivity loss. To overcome these issues, a series of poly(amic acid)s (PAAs) have been synthesized using 4,4’-oxydiphathalic anhydride (ODPA) and Jeffamine monomers of varying molecular weight, and used to fabricate silver nanoparticles via the chelating reaction with silver ions, in attempts to simultaneouslyi)achieve defect-free mixed matrix membranes (MMMs),ii)target CO2selective transport, andiii)enhance long-term stability. The occurrence of the chelating reaction between silver and the PAA was confirmed, and as a result, individual and un-aggregated PAA-coated silver nanoparticles were obtained and incorporated into a commercial polymer, Pebax 1657, to fabricate defect-free mixed matrix membranes. The effect of the PAA length and ether functional group concentration on the structure and performance of the resulting mixed matrix membranes was systematically investigated. Remarkably, inclusion of only 2 wt% nanoparticles in Pebax enhances the CO2permeability by 50% and CO2selectivity by 100% relative to neat polymer. A detailed analysis of the sorption and diffusion coefficients was performed to elucidate the molecular origin of the observed membrane performance. Finally, preliminary data show that the newly synthesized materials exhibit high chemical stability upon exposure to pure H2.