Gamma Irradiation of Cellulose Acetate-Polyethylene Glycol 400 Composite Membrane and Its Performance Test for Gas Separation

Gas separation processes through membrane permeation have attracted the attention of researchers recently due to their promising applications. In this study, we modified the cellulose acetate (CA) membrane to improve the membrane performance of CO₂/CH₄ gas separation. The CA membrane was modified by adding polyethylene glycol (PEG) 400 as the carrier and N, N’-methylenebisacrylamide (MBA) as the cross-linking agent. Gamma-ray from cobalt 60 was used as a reaction initiator with variation in irradiation doses. The membrane characterization tests were conducted using scanning electron micrograph (SEM), Fourier transforms infrared (FTIR), and instron tensile strength tester. The permeability and selectivity of the membranes were tested against the single gases CO₂ and CH₄. The SEM analysis showed the morphology change in the membrane surface by gamma irradiation and a crosslinking agent. The spectra of FTIR showed a change in peak intensity on several polymer functional groups in the presence of gamma-ray irradiation. The tensile strength test showed that membranes with MBA have a higher mechanical strength than those without MBA. Based on the membrane permeability and selectivity tests, CO₂ gas permeability was affected by pressure. The ideal selectivity of CO₂/CH₄ shows that the irradiated membrane has a higher selectivity than that of the non-irradiated membrane.

Cellulose acetate membrane; Fixed carrier membrane; Gamma irradiation; Gas separation; Polyethylene glycol

    Various types of technologies that can be applied for CO₂ gas separation have been investigated by many researchers, one of which is membrane technology (Kartohardjono et al, 2017; Kusrini et al., 2018; Yulia et al., 2019). Membrane separation technology was reported to have advantages, such as being environmentally friendly, having relatively low operating costs and low mobility, only requiring a compact space, and ease of maintenance and operation (Bandehali et al., 2020). The cellulose acetate (CA) membrane is one of the most widely used polymeric membranes for gas separation, including CO₂ and CH₄ gases. Pak et al. (2016) have investigated the use of the hollow fiber CA membrane to separate CO₂ and CH₄.

However, unmodified CA membranes tend to have a lower permeability to CO₂. Some researchers have reported that modified CA membranes could enhance CO₂ permeability (Sanaeepur et al., 2019). One of the compounds that can help increase the permeability of the CA membrane to CO₂ is polyethylene glycol (PEG) (Wu et al., 2015). CO₂ has a good solubility in PEG, so the addition of PEG can increase CO₂ permeability (Hu et al., 2006).

In this study, the modification of CA with PEG was carried out by adding N,N'-methylenebisacrylamide (MBA) as a cross-linking agent and performing gamma-ray irradiation (Suhartini et al., 2020). The aim of using the crosslinking agent was to improve the mechanical stability of the membrane at the time of application (Zhang et al., 2017; Pryhazhayeva et al., 2021).

The aim of this study was to examine the characteristics of the irradiated polymer membrane used for CO₂ gas separation. Gamma-ray irradiation increases the bond between CA, MBA, and PEG to form a copolymer that functions as a fixed carrier membrane (FCM) with the PEG molecule as the carrier. Ghobashy (2018) reported that the advantages of copolymerization irradiation are simple and safe methods. This method can accelerate the formation of polymer radicals so that it is easier for the copolymerization reaction to occur and to form a copolymer chain (Rahmawati et al., 2015). The aim of this study is to improve the performance of CA membranes with modifications using PEG as a carrier, MBA as a cross-linking agent, and gamma-ray irradiation as an accelerator for the bonding between CA, MBA, and PEG. Membrane casting was performed using the phase inversion method (Febriasari et al., 2021). The formed membrane was then characterized based on the Fourier transform infrared (FTIR) analysis, scanning electron micrograph (SEM), and tensile strength. The permeability and selectivity tests were conducted using single gases CO₂ and CH₄ to observe the membrane’s performance.

    The copolymerization of CA-PEG and CA-MBA-PEG has been carried out using gamma-ray irradiation to form FCM. The Fourier transforms infrared (FTIR) results indicate that the irradiation process opened the carbonyl bonds in the CA molecule and changed the intensity of some peaks. The SEM analysis showed that gamma ray irradiation has the potential to widen the membrane pores due to the increase in molecular density caused by the intermolecular bonding process. The mechanical test results with tensile strength show that the CA-MBA-PEG membrane has a higher tensile strength value than that of the CA-PEG membrane. The membrane performance test on single gas CO₂ and CH₄ showed that the ideal selectivity of the CA-PEG and CA-MBA-PEG irradiated membranes was higher than that of the non-irradiated membranes. Ultimately, it can be concluded that this experiment produces a membrane that is quite selective for CO₂ with good stability against pressure. For further research, it is necessary to test the efficiency of the membrane against mixed gases and the stability of the membrane against changes in temperature.

    The authors would like to thank the International Atomic Energy Agency (IAEA) for funding this research. Also, thanks to Mr. Mujiono and Mr. Tavip Sugeng Sugiono from Radiation and Isotopes Application Technology Research Center - Research Organization of Nuclear Power (BATAN)-BRIN for their practical help in this work

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