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<p>Zn-based metal–organic frameworks (Zn MOFs) synthesized under ambient conditions offer a scalable and energy-efficient route to porous materials, but their poorer moisture stability compared to conventionally prepared MOFs limits their use in gas adsorption. To overcome this limitation, thermal pyrolysis has emerged as an effective strategy to enhance structural durability and tailor the pore structure of MOF-derived materials. In this study, a Zn-based pillared-layer MOF, [Zn<sub>2</sub>(BDC)<sub>2</sub>DABCO]<sub><i>n</i></sub> (ZnBD), was synthesized under ambient conditions and subsequently subjected to thermal pyrolysis under an inert atmosphere at 500–700&#xa0;°C. The resulting materials, denoted as ZnBD-T (T = pyrolysis temperature), were systematically characterized in terms of morphology, pore structure, surface functionality, and CO<sub>2</sub> adsorption performance. Among them, ZnBD-600 exhibited the highest CO<sub>2</sub> uptake and CO<sub>2</sub>/N<sub>2</sub> selectivity at 298&#xa0;K. This superior performance is attributed to the combined effects of abundant ultramicropores and high pyridinic nitrogen content, both of which enhance CO<sub>2</sub> affinity. Furthermore, ZnBD-600 not only demonstrated excellent stability but also outperformed the unpyrolyzed parent ZnBD in CO<sub>2</sub> adsorption capacity and selectivity. These results highlight that moderate-temperature pyrolysis offers a simple and scalable route to transform unstable Zn MOFs into durable and high-performance CO<sub>2</sub> adsorbents suitable for practical applications.</p>

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Controlled Thermal Pyrolysis for Optimizing the Stability and CO2 Adsorption Performance of Metal–Organic Frameworks Synthesized under Ambient Conditions

  • 期刊论文

  • 发表日期：

    2025年9月15日

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  • Giwook Lee,
  • Jongkook Hwang

摘要

Zn-based metal–organic frameworks (Zn MOFs) synthesized under ambient conditions offer a scalable and energy-efficient route to porous materials, but their poorer moisture stability compared to conventionally prepared MOFs limits their use in gas adsorption. To overcome this limitation, thermal pyrolysis has emerged as an effective strategy to enhance structural durability and tailor the pore structure of MOF-derived materials. In this study, a Zn-based pillared-layer MOF, [Zn2(BDC)2DABCO]n (ZnBD), was synthesized under ambient conditions and subsequently subjected to thermal pyrolysis under an inert atmosphere at 500–700 °C. The resulting materials, denoted as ZnBD-T (T = pyrolysis temperature), were systematically characterized in terms of morphology, pore structure, surface functionality, and CO2 adsorption performance. Among them, ZnBD-600 exhibited the highest CO2 uptake and CO2/N2 selectivity at 298 K. This superior performance is attributed to the combined effects of abundant ultramicropores and high pyridinic nitrogen content, both of which enhance CO2 affinity. Furthermore, ZnBD-600 not only demonstrated excellent stability but also outperformed the unpyrolyzed parent ZnBD in CO2 adsorption capacity and selectivity. These results highlight that moderate-temperature pyrolysis offers a simple and scalable route to transform unstable Zn MOFs into durable and high-performance CO2 adsorbents suitable for practical applications.