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Development of single solid adsorbents simultaneously combining robust structure, high separation capacity, and easy performance recovery is highly desired but quite a challenge for realizing methane depuration. In the present study, we report an ultramicroporous hydrogen\u2010bonded organic framework compound constructed from a tetracyano bithiophene\u2010functionalized ligand. Similar to the acting principle of enzymes, multisite supramolecular interactions endow the material with not only extraordinary chemical stability in wide pH range including 12\u2005M HCl and 20\u2005M NaOH solutions but also highly selective recognition of acetylene and carbon dioxide over methane. The packing densities and adsorption selectivities toward acetylene and carbon dioxide are the highest reported for the hydrogen\u2010bonded organic framework materials. Dynamic breakthrough experiments demonstrate its highly efficient methane purification ability from binary and even ternary mixed gases, with not only methane productivities up to 2.34\u2005mol\u2009kg\n                    <jats:sup>\u22121<\/jats:sup>\n                    but also moderate regeneration energy. Furthermore, the title compound can be easily regenerated in almost quantitative yield via simple rato\u2010evaporation of its dichloromethane solution once its activity is attenuated or lost.\n                  <\/jats:p>","DOI":"10.1002\/anie.202500970","type":"journal-article","created":{"date-parts":[[2025,2,3]],"date-time":"2025-02-03T07:57:11Z","timestamp":1738569431000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":23,"title":["Efficient Methane Purification Using a Robust and Recoverable Hydrogen\u2010Bonded Organic Framework"],"prefix":"10.1002","volume":"64","author":[{"given":"Shengjie","family":"Lin","sequence":"first","affiliation":[{"name":"Key Laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Materials Science Zhejiang Normal University  Jinhua 321004 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