Simultaneous interlayer and intralayer space control in two-dimensional metal-organic frameworks for acetylene/ethylene separation.
Simultaneous interlayer and intralayer space control in two-dimensional metal-organic frameworks for acetylene/ethylene separation.
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用于乙炔/乙烯分离的二维金属有机框架中同时控制层间和层内空间
DOI：
10.1038/s41467-020-20101-7
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发表时间：
2020-12-07
影响因子：
16.6
通讯作者：
Ren Q
中科院分区：
文献类型：
--
作者：
Shen J;He X;Ke T;Krishna R;van Baten JM;Chen R;Bao Z;Xing H;Dincǎ M;Zhang Z;Yang Q;Ren Q
三维金属有机骨架（MOFs）由于具有丰富的具有特定化学性质的孔而成为吸附去除痕量气体的前沿材料。然而，结合高吸附容量与高选择性和稳定性的理想吸附剂的开发仍然具有挑战性。在这里，我们展示了一种策略来设计吸附剂，利用二维氟化MOFs的层间和层内空间的可调谐性来从乙烯中捕获乙炔。通过X射线衍射和建模验证，连接体原子氧化态的系统变化使得能够精细调节层堆叠图案和连接体构象，这提供了分子的强层间捕获沿着协同层内结合。所得到的坚固材料（ZUL-100和ZUL-200）在0.001-0.05 bar的压力范围内表现出高选择性的基准容量。它们在乙炔/乙烯分离中的效率通过突破性实验得到证实，即使在潮湿条件下循环，也具有优异的乙烯产率（1/99混合物为121 mmol/g，99.9999%）。设计用于去除微量气体的高效吸附剂仍然是一个严峻的挑战。在这里，作者展示了层状2D金属有机框架的前景，这种框架经常被忽视，有利于3D框架，用于从乙烯中分离痕量乙炔，具有增强的性能和高稳定性。
Three-dimensional metal−organic frameworks (MOFs) are cutting-edge materials in the adsorptive removal of trace gases due to the availability of abundant pores with specific chemistry. However, the development of ideal adsorbents combining high adsorption capacity with high selectivity and stability remains challenging. Here we demonstrate a strategy to design adsorbents that utilizes the tunability of interlayer and intralayer space of two-dimensional fluorinated MOFs for capturing acetylene from ethylene. Validated by X-ray diffraction and modeling, a systematic variation of linker atom oxidation state enables fine regulation of layer stacking pattern and linker conformation, which affords a strong interlayer trapping of molecules along with cooperative intralayer binding. The resultant robust materials (ZUL-100 and ZUL-200) exhibit benchmark capacity in the pressure range of 0.001–0.05 bar with high selectivity. Their efficiency in acetylene/ethylene separation is confirmed by breakthrough experiments, giving excellent ethylene productivities (121 mmol/g from 1/99 mixture, 99.9999%), even when cycled under moist conditions. Designing efficient adsorbents for trace gas removal remains a serious challenge. Here, the authors show promise in layered 2D metal−organic frameworks, often overlooked in favor of 3D frameworks, for separating trace acetylene from ethylene with enhanced performance and high stability.
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影响因子：
56.9
作者：
Cadiau, A.;Adil, K.;Eddaoudi, M.
通讯作者：
Eddaoudi, M.
影响因子：
56.9
作者：
Bloch, Eric D.;Queen, Wendy L.;Long, Jeffrey R.
通讯作者：
Long, Jeffrey R.
影响因子：
3.3
作者：
Krishna, R;van Baten, JM
通讯作者：
van Baten, JM
DOI：
10.1002/anie.201808716
发表时间：
2018-12-03
期刊：
Angewandte Chemie (International ed. in English)
影响因子：
--
作者：
Bao Z;Wang J;Zhang Z;Xing H;Yang Q;Yang Y;Wu H;Krishna R;Zhou W;Chen B;Ren Q
通讯作者：
Ren Q
用于从乙烯中捕获乙炔的杂化多孔材料的孔化学和尺寸控制
影响因子：
56.9
作者：
Cui, Xili;Chen, Kaijie;Chen, Banglin
通讯作者：
Chen, Banglin