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<p>The efficient separation and enrichment of methane (CH<sub>4</sub>) from low-concentration coalbed methane (CBM) are of great significance for enhancing CBM utilization efficiency and promoting the development of low-carbon clean energy. To address this practical need, this study synthesized a tailored chlorinated metal-organic framework (MOF), PCP-IPA-Cl, and systematically evaluated its CH<sub>4</sub>/N<sub>2</sub> separation performance through a combination of static adsorption measurements, density functional theory (DFT) calculations, dynamic breakthrough experiments, and multiple adsorption-desorption cycling tests. Endowed with its optimized pore structure and chlorinated channel environment, PCP-IPA-Cl exhibits excellent CH<sub>4</sub>/N<sub>2</sub> separation performance and regeneration stability: at 298 K and 1 bar, it achieves a high CH<sub>4</sub> adsorption capacity of 21.27 cm<sup>3</sup>/g with a low N<sub>2</sub> uptake of only 5.29 cm<sup>3</sup>/g, and compared with its unchlorinated analog PCP-IPA, the CH<sub>4</sub>/N<sub>2</sub> selectivity is markedly improved from 5.4 to 9.0. DFT calculations reveal that the introduction of–Cl groups creates additional preferential adsorption sites for CH<sub>4</sub> molecules, strengthening host-guest interactions and thus enhancing separation efficiency. Furthermore, breakthrough experiments confirm its excellent dynamic separation ability, and cyclic tests demonstrate that PCP-IPA-Cl can be fully regenerated via helium purging within just 5 min. These findings collectively demonstrate that PCP-IPA-Cl is a promising and regenerable adsorbent for the efficient enrichment and utilization of low-concentration CBM.</p>

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Design of highly efficient, renewable chlorine-modified metal-organic frameworks and investigation of CH4/N2 separation performance

  • 期刊论文

  • 发表日期：

    2026年5月7日

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  • Zhaozhuang Liu,
  • Mingxi Wang,
  • Li Wang,
  • Jiaqi Liu,
  • Jinping Li,
  • Jiangfeng Yang

摘要

The efficient separation and enrichment of methane (CH4) from low-concentration coalbed methane (CBM) are of great significance for enhancing CBM utilization efficiency and promoting the development of low-carbon clean energy. To address this practical need, this study synthesized a tailored chlorinated metal-organic framework (MOF), PCP-IPA-Cl, and systematically evaluated its CH4/N2 separation performance through a combination of static adsorption measurements, density functional theory (DFT) calculations, dynamic breakthrough experiments, and multiple adsorption-desorption cycling tests. Endowed with its optimized pore structure and chlorinated channel environment, PCP-IPA-Cl exhibits excellent CH4/N2 separation performance and regeneration stability: at 298 K and 1 bar, it achieves a high CH4 adsorption capacity of 21.27 cm3/g with a low N2 uptake of only 5.29 cm3/g, and compared with its unchlorinated analog PCP-IPA, the CH4/N2 selectivity is markedly improved from 5.4 to 9.0. DFT calculations reveal that the introduction of–Cl groups creates additional preferential adsorption sites for CH4 molecules, strengthening host-guest interactions and thus enhancing separation efficiency. Furthermore, breakthrough experiments confirm its excellent dynamic separation ability, and cyclic tests demonstrate that PCP-IPA-Cl can be fully regenerated via helium purging within just 5 min. These findings collectively demonstrate that PCP-IPA-Cl is a promising and regenerable adsorbent for the efficient enrichment and utilization of low-concentration CBM.