Volume 10 Issue 3
Mar.  2025
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Article Navigation >  Green Energy&Environment  > 2025  >  10(3): 560-572
Ping Zhang, Xingyun Ma, Zhuoheng Tu, Xiaomin Zhang, Xingbang Hu, Youting Wu. Constructing ether-rich and carboxylate hydrogen bonding sites in protic ionic liquids for efficient and simultaneous membrane separation of H2S and CO2 from CH4. Green Energy&Environment, 2025, 10(3): 560-572. doi: 10.1016/j.gee.2024.05.009
Citation: Ping Zhang, Xingyun Ma, Zhuoheng Tu, Xiaomin Zhang, Xingbang Hu, Youting Wu. Constructing ether-rich and carboxylate hydrogen bonding sites in protic ionic liquids for efficient and simultaneous membrane separation of H2S and CO2 from CH4. Green Energy&Environment, 2025, 10(3): 560-572. doi: 10.1016/j.gee.2024.05.009
shu

Constructing ether-rich and carboxylate hydrogen bonding sites in protic ionic liquids for efficient and simultaneous membrane separation of H2S and CO2 from CH4

doi: 10.1016/j.gee.2024.05.009

  • a. Separation Engineering Research Center, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210023, China;

  • b. Institute of Green Chemistry and Engineering, Nanjing University, Suzhou, 215163, China

Funds:

This work was sponsored by the National Natural Science Foundation of China (Nos. 22308145, 22208140, 22178159, 22078145), Natural Science Foundation of Jiangsu Province (BK20230791) and Postgraduate Research Innovation Program of Jiangsu Province (KYCX24_0165).

  • Received date 17 January 2024, Accepted date 17 May 2024, RevRecd date 19 April 2024, Available online 07 April 2025, Publish date 20 May 2024,
    Abstract
  • Removing H2S and CO2 is of great significance for natural gas purification. With excellent gas affinity and tunable structure, ionic liquids (ILs) have been regarded as nontrivial candidates for fabricating polymer-based membranes. Herein, we firstly reported the incorporation of protic ILs (PILs) having ether-rich and carboxylate sites (ECPILs) into poly(ether-block-amide) (Pebax) matrix for efficient separation H2S and CO2 from CH4. Notably, the optimal permeability of H2S reaches up to 4310 Barrer (40 °C, 0.50 bar) in Pebax/ECPIL membranes, along with H2S/CH4 and (H2S + CO2)/CH4 selectivity of 97.7 and 112.3, respectively. These values are increased by 1125%, 160.8% and 145.9% compared to those in neat Pebax membrane. Additionally, the solubility and diffusion coefficients of the gases were measured, demonstrating that ECPIL can simultaneously strengthen the dissolution and diffusion of H2S and CO2, thus elevating the permeability and permselectivity. By using quantum chemical calculations and FT-IR spectroscopy, the highly reversible multi-site hydrogen bonding interaction between ECPILs and H2S was revealed, which is responsible for the fast permeation of H2S and good selectivity. Furthermore, H2S/CO2/CH4 (3/3/94 mol/mol) ternary mixed gas can be efficiently and stably separated by Pebax/ECPIL membrane for at least 100 h. Overall, this work not only illustrates that PILs with ether-rich and carboxylate hydrogen bonding sites are outstanding materials for simultaneous removal of H2S and CO2, but may also provide a novel insight into the design of membrane materials for natural gas upgrading.

     

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