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Controllable inverse C2H2/CO2 separation in ultra-stable Zn-organic frameworks for efficient removal of trace CO2 from acetylene
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2022-10-24 , DOI: 10.1039/d2ta07473g
Jia Yu 1 , Jing Zhang 1 , Peng Zhang 1 , Ying Wang 1 , Shu-Ni Li 1 , Quan-Guo Zhai 1
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2022-10-24 , DOI: 10.1039/d2ta07473g
Jia Yu 1 , Jing Zhang 1 , Peng Zhang 1 , Ying Wang 1 , Shu-Ni Li 1 , Quan-Guo Zhai 1
Affiliation
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It is of great challenge to produce highly pure C2H2 from the CO2/C2H2 mixture because of their similar physical properties. Metal–organic frameworks (MOFs) have shown great potential in purifying C2H2 by virtue of their versatile pore environment with excellent tunability. However, the rational exploration of ideal MOF adsorbents with CO2-preferred CO2/C2H2 separation performance (also called inverse C2H2/CO2 separation) is extremely difficult. In this work, we demonstrate a new Zn-MOF family (SNNU-334–336) with special CO2-preferred CO2/C2H2 separation performance, which can be rationally controlled by functional groups as well as temperature. Notably, SNNU-334–336 MOFs show extremely high stability, and SNNU-336 can maintain a stable structure even after 7 days in boiling water and 30 days in air, which is unprecedented for all Zn-based MOF materials. Different to common MOF adsorbents, the adsorption isotherms of SNNU-334–336 MOFs for C2H2 and CO2 under the same temperature all have an intersection point (we called the inverse point), which gradually moves to the high-pressure region with the increase of temperature and changes with the pore environment variation. So, SNNU-334–336 MOFs can be rationally controlled from C2H2-selective to CO2-selective CO2/C2H2 adsorption separation adsorbents. IAST selectivity calculation indicates that a very high CO2 over C2H2 selectivity (3595.4) can be achieved, which nearly surpasses those of all reported MOFs with CO2-preferred CO2/C2H2 separation performance. Fixed-bed column breakthrough experiments further prove that SNNU-334–336 MOFs all have controllable inverse CO2/C2H2 separation ability and can produce C2H2 with extra-high purity (>99.9%) from the CO2/C2H2 (1/99) mixture.
中文翻译:
超稳定锌有机框架中可控的逆 C2H2/CO2 分离,用于有效去除乙炔中的痕量 CO2
由CO 2 /C 2 H 2混合物生产高纯度C 2 H 2具有很大的挑战,因为它们具有相似的物理性质。金属有机框架(MOFs)凭借其多功能的孔环境和出色的可调性在纯化C 2 H 2方面显示出巨大的潜力。然而,合理探索具有CO 2优先CO 2 /C 2 H 2分离性能的理想MOF吸附剂(也称为逆C 2 H 2 /CO 2分离)非常困难。在这项工作中,我们展示了一个新的 Zn-MOF 家族 (SNNU-334-336),它具有特殊的 CO 2优先 CO 2 /C 2 H 2分离性能,可以通过官能团和温度进行合理控制。值得注意的是,SNNU-334-336 MOFs表现出极高的稳定性,SNNU-336即使在沸水7天和空气中30天后仍能保持稳定的结构,这在所有锌基MOF材料中是前所未有的。与普通 MOF 吸附剂不同,SNNU-334-336 MOF 对 C 2 H 2和 CO 2的吸附等温线在相同温度下都有一个交点(我们称为反点),随着温度的升高逐渐向高压区移动,并随着孔隙环境的变化而变化。因此,SNNU-334-336 MOFs可以从C 2 H 2选择性到CO 2选择性CO 2 /C 2 H 2吸附分离吸附剂进行合理控制。IAST 选择性计算表明,可以实现比 C 2 H 2非常高的 CO 2选择性 (3595.4),这几乎超过了所有报道的具有 CO 2优先 CO 2 /C 2的 MOFH 2分离性能。固定床柱突破实验进一步证明,SNNU-334-336 MOFs均具有可控的逆CO 2 /C 2 H 2分离能力,可从CO 2 /中产生超高纯度(>99.9%)的C 2 H 2 / C 2 H 2 (1/99) 混合物。
更新日期:2022-10-24
中文翻译:

超稳定锌有机框架中可控的逆 C2H2/CO2 分离,用于有效去除乙炔中的痕量 CO2
由CO 2 /C 2 H 2混合物生产高纯度C 2 H 2具有很大的挑战,因为它们具有相似的物理性质。金属有机框架(MOFs)凭借其多功能的孔环境和出色的可调性在纯化C 2 H 2方面显示出巨大的潜力。然而,合理探索具有CO 2优先CO 2 /C 2 H 2分离性能的理想MOF吸附剂(也称为逆C 2 H 2 /CO 2分离)非常困难。在这项工作中,我们展示了一个新的 Zn-MOF 家族 (SNNU-334-336),它具有特殊的 CO 2优先 CO 2 /C 2 H 2分离性能,可以通过官能团和温度进行合理控制。值得注意的是,SNNU-334-336 MOFs表现出极高的稳定性,SNNU-336即使在沸水7天和空气中30天后仍能保持稳定的结构,这在所有锌基MOF材料中是前所未有的。与普通 MOF 吸附剂不同,SNNU-334-336 MOF 对 C 2 H 2和 CO 2的吸附等温线在相同温度下都有一个交点(我们称为反点),随着温度的升高逐渐向高压区移动,并随着孔隙环境的变化而变化。因此,SNNU-334-336 MOFs可以从C 2 H 2选择性到CO 2选择性CO 2 /C 2 H 2吸附分离吸附剂进行合理控制。IAST 选择性计算表明,可以实现比 C 2 H 2非常高的 CO 2选择性 (3595.4),这几乎超过了所有报道的具有 CO 2优先 CO 2 /C 2的 MOFH 2分离性能。固定床柱突破实验进一步证明,SNNU-334-336 MOFs均具有可控的逆CO 2 /C 2 H 2分离能力,可从CO 2 /中产生超高纯度(>99.9%)的C 2 H 2 / C 2 H 2 (1/99) 混合物。
