Overcoming humidity-induced swelling of graphene oxide-based hydrogen membranes using charge-compensating nanodiamonds

Guoji Huang, Behnam Ghalei (), Ali Pournaghshband Isfahani, H. Enis Karahan, Daiki Terada, Detao Qin, Conger Li, Masahiko Tsujimoto, Daisuke Yamaguchi, Kunihisa Sugimoto, Ryuji Igarashi, Bor Kae Chang, Tao Li, Masahiro Shirakawa and Easan Sivaniah ()
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Guoji Huang: Kyoto University
Behnam Ghalei: Kyoto University
Ali Pournaghshband Isfahani: Kyoto University
H. Enis Karahan: Kyoto University
Daiki Terada: Kyoto University
Detao Qin: Kyoto University
Conger Li: ShanghaiTech University
Masahiko Tsujimoto: Kyoto University
Daisuke Yamaguchi: Kyoto University
Kunihisa Sugimoto: Kyoto University
Ryuji Igarashi: National Institutes for Quantum Science and Technology
Bor Kae Chang: National Central University
Tao Li: ShanghaiTech University
Masahiro Shirakawa: Kyoto University
Easan Sivaniah: Kyoto University

Nature Energy, 2021, vol. 6, issue 12, 1176-1187

Abstract: Abstract Graphene oxide (GO) can form ultrapermeable and ultraselective membranes that are promising for various gas separation applications, including hydrogen purification. However, GO films lose their attractive separation properties in humid conditions. Here we show that incorporating positively charged nanodiamonds (ND+s) into GO nanolaminates leads to humidity-resistant, yet high-performing, membranes. While native GO membranes fail at a single run, the GO/ND+ composite retains up to roughly 90% of GO’s H2 selectivity against CO2 after several cycles under an aggressive humidity test. The addition of negatively charged ND to GO brought no such stabilization, suggesting that charge compensation acts as the main mechanism conferring humidity resistance, where ND+s neutralize the negative charge GO sheets. We observed a similar but inferior stabilization effect when positively charged polyhedral oligomeric silsesquioxane replaces ND+. The demonstrated material platform offers a solution for separating H2 gas from its usually humid mixtures generated from fossil fuel sources or water splitting.

Date: 2021
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DOI: 10.1038/s41560-021-00946-y

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