Functionalized GO Membranes for Efficient Separation of Acid Gases from Natural Gas: A Computational Mechanistic Understanding
Membrane separation technology is applied in natural gas processing, while a high-performance membrane is highly in demand. This paper considers the bright future of functionalized graphene oxide (GO) membranes in acid gas removal from natural gas. By molecular simulations, the adsorption and diffus...
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| Format: | Article |
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MDPI AG
2022-11-01
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| Series: | Membranes |
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| Online Access: | https://www.mdpi.com/2077-0375/12/11/1155 |
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| author | Quan Liu Zhonglian Yang Gongping Liu Longlong Sun Rong Xu Jing Zhong |
| author_facet | Quan Liu Zhonglian Yang Gongping Liu Longlong Sun Rong Xu Jing Zhong |
| author_sort | Quan Liu |
| collection | DOAJ |
| description | Membrane separation technology is applied in natural gas processing, while a high-performance membrane is highly in demand. This paper considers the bright future of functionalized graphene oxide (GO) membranes in acid gas removal from natural gas. By molecular simulations, the adsorption and diffusion behaviors of several unary gases (N<sub>2</sub>, CH<sub>4</sub>, CO<sub>2</sub>, H<sub>2</sub>S, and SO<sub>2</sub>) are explored in the 1,4-phenylenediamine-2-sulfonate (PDASA)-doped GO channels. Molecular insights show that the multilayer adsorption of acid gases evaluates well by the Redlich-Peterson model. A tiny amount of PDASA promotes the solubility coefficient of CO<sub>2</sub> and H<sub>2</sub>S, respectively, up to 4.5 and 5.3 mmol·g<sup>−1</sup>·kPa<sup>−1</sup>, nearly 2.5 times higher than those of a pure GO membrane, which is due to the improved binding affinity, great isosteric heat, and hydrogen bonds, while N<sub>2</sub> and CH<sub>4</sub> only show single-layer adsorption with solubility coefficients lower than 0.002 mmol·g<sup>−1</sup>·kPa<sup>−1</sup>, and their weak adsorption is insusceptible to PDASA. Although acid gas diffusivity in GO channels is inhibited below 20 × 10<sup>−6</sup> cm<sup>2</sup>·s<sup>−1</sup> by PDASA, the solubility coefficient of acid gases is certainly high enough to ensure their separation efficiency. As a result, the permeabilities (<i>P</i>) of acid gases and their selectivities (<i>α</i>) over CH<sub>4</sub> are simultaneously improved (<i>P</i><sub>CO2</sub> = 7265.5 Barrer, <i>α<sub>CO2/CH4</sub> =</i> 95.7; <i>P<sub>(</sub></i><sub>H2S+CO2)</sub> = 42075.1 Barrer, <i>α<sub>H2S/CH4</sub></i> = 243.8), which outperforms most of the ever-reported membranes. This theoretical study gives a mechanistic understanding of acid gas separation and provides a unique design strategy to develop high-performance GO membranes toward efficient natural gas processing. |
| first_indexed | 2024-03-09T18:08:35Z |
| format | Article |
| id | doaj.art-115a5271b969446dbfa89f2be44d1903 |
| institution | Directory Open Access Journal |
| issn | 2077-0375 |
| language | English |
| last_indexed | 2024-03-09T18:08:35Z |
| publishDate | 2022-11-01 |
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| series | Membranes |
| spelling | doaj.art-115a5271b969446dbfa89f2be44d19032023-11-24T09:12:41ZengMDPI AGMembranes2077-03752022-11-011211115510.3390/membranes12111155Functionalized GO Membranes for Efficient Separation of Acid Gases from Natural Gas: A Computational Mechanistic UnderstandingQuan Liu0Zhonglian Yang1Gongping Liu2Longlong Sun3Rong Xu4Jing Zhong5Analytical and Testing Center, School of Chemical Engineering, Anhui University of Science and Technology, Huainan 232001, ChinaAnalytical and Testing Center, School of Chemical Engineering, Anhui University of Science and Technology, Huainan 232001, ChinaState Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, 30 Puzhu Road (S), Nanjing 211816, ChinaAnalytical and Testing Center, School of Chemical Engineering, Anhui University of Science and Technology, Huainan 232001, ChinaKey Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, Gehu Road, Changzhou 213164, ChinaKey Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, Gehu Road, Changzhou 213164, ChinaMembrane separation technology is applied in natural gas processing, while a high-performance membrane is highly in demand. This paper considers the bright future of functionalized graphene oxide (GO) membranes in acid gas removal from natural gas. By molecular simulations, the adsorption and diffusion behaviors of several unary gases (N<sub>2</sub>, CH<sub>4</sub>, CO<sub>2</sub>, H<sub>2</sub>S, and SO<sub>2</sub>) are explored in the 1,4-phenylenediamine-2-sulfonate (PDASA)-doped GO channels. Molecular insights show that the multilayer adsorption of acid gases evaluates well by the Redlich-Peterson model. A tiny amount of PDASA promotes the solubility coefficient of CO<sub>2</sub> and H<sub>2</sub>S, respectively, up to 4.5 and 5.3 mmol·g<sup>−1</sup>·kPa<sup>−1</sup>, nearly 2.5 times higher than those of a pure GO membrane, which is due to the improved binding affinity, great isosteric heat, and hydrogen bonds, while N<sub>2</sub> and CH<sub>4</sub> only show single-layer adsorption with solubility coefficients lower than 0.002 mmol·g<sup>−1</sup>·kPa<sup>−1</sup>, and their weak adsorption is insusceptible to PDASA. Although acid gas diffusivity in GO channels is inhibited below 20 × 10<sup>−6</sup> cm<sup>2</sup>·s<sup>−1</sup> by PDASA, the solubility coefficient of acid gases is certainly high enough to ensure their separation efficiency. As a result, the permeabilities (<i>P</i>) of acid gases and their selectivities (<i>α</i>) over CH<sub>4</sub> are simultaneously improved (<i>P</i><sub>CO2</sub> = 7265.5 Barrer, <i>α<sub>CO2/CH4</sub> =</i> 95.7; <i>P<sub>(</sub></i><sub>H2S+CO2)</sub> = 42075.1 Barrer, <i>α<sub>H2S/CH4</sub></i> = 243.8), which outperforms most of the ever-reported membranes. This theoretical study gives a mechanistic understanding of acid gas separation and provides a unique design strategy to develop high-performance GO membranes toward efficient natural gas processing.https://www.mdpi.com/2077-0375/12/11/1155acid gas removalgraphene oxidemembrane separationmolecular simulationnatural gas |
| spellingShingle | Quan Liu Zhonglian Yang Gongping Liu Longlong Sun Rong Xu Jing Zhong Functionalized GO Membranes for Efficient Separation of Acid Gases from Natural Gas: A Computational Mechanistic Understanding Membranes acid gas removal graphene oxide membrane separation molecular simulation natural gas |
| title | Functionalized GO Membranes for Efficient Separation of Acid Gases from Natural Gas: A Computational Mechanistic Understanding |
| title_full | Functionalized GO Membranes for Efficient Separation of Acid Gases from Natural Gas: A Computational Mechanistic Understanding |
| title_fullStr | Functionalized GO Membranes for Efficient Separation of Acid Gases from Natural Gas: A Computational Mechanistic Understanding |
| title_full_unstemmed | Functionalized GO Membranes for Efficient Separation of Acid Gases from Natural Gas: A Computational Mechanistic Understanding |
| title_short | Functionalized GO Membranes for Efficient Separation of Acid Gases from Natural Gas: A Computational Mechanistic Understanding |
| title_sort | functionalized go membranes for efficient separation of acid gases from natural gas a computational mechanistic understanding |
| topic | acid gas removal graphene oxide membrane separation molecular simulation natural gas |
| url | https://www.mdpi.com/2077-0375/12/11/1155 |
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