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<p>The efficient discrimination of industrially relevant gases, particularly those with closely analogous physicochemical properties, remains a formidable challenge within the realm of adsorptive separation technologies. Achieving satisfactory separation efficiency poses stringent requirements on the precise control over the pore structures of adsorbents. Here we introduce a strategy for the precise modulation of pore structures in a carbonate-pillared Zn-triazolate framework, Zn<sub>2</sub>(datrz)<sub>2</sub>CO<sub>3</sub> (datrz = 3,5-diamino-1,2,4-triazolate), through the straightforward adjustment of the solvothermal synthesis temperature. Utilizing this approach, we have successfully fabricated a series of Zn<sub>2</sub>(datrz)<sub>2</sub>CO<sub>3</sub> materials with tunable pore structures while maintaining the framework composition and overall connectivity. These materials demonstrate selective recognition for challenging gas mixtures, including C<sub>3</sub>H<sub>6</sub>/C<sub>3</sub>H<sub>8</sub>, CO<sub>2</sub>/CH<sub>4</sub>, and CO<sub>2</sub>/N<sub>2</sub>. Density functional theory (DFT) calculations confirm that the precisely engineered pore environment plays a decisive role on selective gas adsorption. Further, the high reproducibility and scalability of this temperature-controlled synthesis method underscore its immense potential for industrial-scale applications in gas purification and separation processes.</p>

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Temperature-regulated synthesis of carbonate-pillared zinc-triazolate frameworks for precise molecular recognition

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月11日

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  • Jiaqi Liu,
  • Tong Li,
  • Qiyi Bu,
  • Xiaowei Bai,
  • Li Wang,
  • Jiafeng Miao,
  • Hao Wang,
  • Jinping Li

摘要

The efficient discrimination of industrially relevant gases, particularly those with closely analogous physicochemical properties, remains a formidable challenge within the realm of adsorptive separation technologies. Achieving satisfactory separation efficiency poses stringent requirements on the precise control over the pore structures of adsorbents. Here we introduce a strategy for the precise modulation of pore structures in a carbonate-pillared Zn-triazolate framework, Zn2(datrz)2CO3 (datrz = 3,5-diamino-1,2,4-triazolate), through the straightforward adjustment of the solvothermal synthesis temperature. Utilizing this approach, we have successfully fabricated a series of Zn2(datrz)2CO3 materials with tunable pore structures while maintaining the framework composition and overall connectivity. These materials demonstrate selective recognition for challenging gas mixtures, including C3H6/C3H8, CO2/CH4, and CO2/N2. Density functional theory (DFT) calculations confirm that the precisely engineered pore environment plays a decisive role on selective gas adsorption. Further, the high reproducibility and scalability of this temperature-controlled synthesis method underscore its immense potential for industrial-scale applications in gas purification and separation processes.