Volume 79
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Ding, X., Tan, F., Zhao, H., Xin, Q., & Zhang, Y. (2023). Ultrapermeable membranes based on connected cluster of hollow polydimethylsiloxane nanoparticles for gas separation. Particuology, 79, 45-53. https://doi.org/10.1016/j.partic.2022.10.015
Ultrapermeable membranes based on connected cluster of hollow polydimethylsiloxane nanoparticles for gas separation
Xiaoli Ding a b, Fangfang Tan a b, Hongyong Zhao a b *, Qingping Xin a b, Yuzhong Zhang a b
a State Key Laboratory of Separation Membranes and Membrane Processes, National Center for International Joint Research on Separation Membranes, Tiangong University, Tianjin, 300387, China
b Tianjin Key Laboratory of Hollow Fiber Membrane Materials and Processes (Tiangong University), Tianjin, 300387, China
10.1016/j.partic.2022.10.015
Volume 79, August 2023, Pages 45-53
Received 29 August 2022, Revised 30 October 2022, Accepted 31 October 2022, Available online 19 November 2022, Version of Record 24 January 2023.
E-mail: zhaohongyong@tiangong.edu.cn

Highlights

• Hollow PDMS nanoparticles were synthesized as fillers to fabricate MMMs.

• High-concentrated soft PDMS nanoparticles formed continuous phase of MMMs.

• Connected cluster of hollow PDMS nanoparticles dominated gas transport in MMMs.

• Permeability increases significantly, more than ten times higher than that of PDMS.


Abstract

Mixed matrix membranes (MMMs) with the performance between the matrix and the filler is a promising strategy for membranes with excellent gas permeability-selectivity. In this study, the hollow polydimethylsiloxane nanoparticles were synthesized and then incorporated with the poly(oxide ethylene) monomer and tri-functional cross-linker to form mixed matrix membranes by in situ polymerization. The hollow nanoparticles formed the independent closed nanocavities in membranes, which enhanced the gas permeability contributed by both the improved diffusivity and solubility. At high loading, the hollow polydimethylsiloxane nanoparticle was converted into the continuous phase with the cross-linked poly(oxide ethylene) as the dispersed phase. Gases preferred to permeate through the connected cluster of hollow polydimethylsiloxane nanoparticles, finally leading to ultrahigh gas permeabilities far going beyond the instinct values of polydimethylsiloxane and the cross-linked poly(oxide ethylene). The optimized membrane with 34 wt% hollow nanoparticles loadings exhibited ultrahigh permeabilities with the values of 44186 Barrer for CO2 and 11506 Barrer for O2, accompanied with a CO2/N2 selectivity of 9.9 and an O2/N2 selectivity of 2.6, which exceeded the 2008 Robeson upper bound for O2/N2 and located at the 2008 Robeson upper bound for CO2/N2.

Graphical abstract
Keywords
Hollow nanoparticles; Polydimethylsiloxane nanoparticles; Mixed matrix membranes; Nanocavity; Gas separation