| 王赫,王铭,刘艺伟,段春迎.具有烯/炔烃分离性能的钴金属有机笼功能化石墨烯[J].,2023,63(4):331-337 |
| 具有烯/炔烃分离性能的钴金属有机笼功能化石墨烯 |
| Cobalt metal organic cage functionalized graphene with alkene/alkyne separation performance |
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| DOI：10.7511/dllgxb202304001 |
| 中文关键词: 钴 金属有机笼 石墨烯 烯/炔烃分离 |
| 英文关键词: cobalt metal organic cage graphene alkene/alkyne separation |
| 基金项目:国家自然科学基金资助项目(2217103521901135)；中央高校基本科研业务费专项资金资助项目(DUT21LK18)；催化基础国家重点实验室(中国科学院大连化学物理研究所)开放课题(N-21-08). |
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| 中文摘要: |
| 为实现乙烯/乙炔高效分离，以联苯胺-吡啶-2-甲醛形成的双臂二齿有机配体与钴离子配位自组装合成了四面体金属有机笼(MOCs)：Co4(LBA)6(ClO4)8(Co-LBA，LBA= \-4，4′-二胺，N4，N4′-二(2-吡啶亚甲基))．结构分析表明Co-LBA的窗口尺寸(0.4 nm)恰好处于乙炔动力学直径(0.334 nm)和乙烯动力学直径(0.418 nm)之间．为避免Co-LBA微孔结构对乙炔吸附动力学的限制，进一步通过浸渍法将其分散到氧化石墨烯(GO)基底上，煅烧得到稳定的多级结构Co-LBA功能化石墨烯材料(Co-LBA@rGO)．透射电子显微镜(TEM)、傅里叶变换红外光谱(FTIR)和N2吸附结果表明，在 Co-LBA@rGO复合材料中，Co-LBA保持笼状结构且高度分散在石墨烯层间，从而使材料同时具有微孔和介孔两种分子扩散通道．在室温条件下，Co-LBA@rGO展示出显著的选择性吸附乙炔能力，p/p0为0.5时乙炔与乙烯吸附量比达到12.5，具有潜在的烯/炔烃分离应用前景． |
| 英文摘要: |
| To realize the efficient separation of ethylene/acetylene, tetrahedral metal organic cages (MOCs)：Co4(LBA)6(ClO4)8 (Co-LBA, LBA=\-4, 4′-diamine, N4, N4′-bis(2-pyridinylmethylene)) are synthesized by self-assembly of double arm bidentate organic ligand formed by benzidine, pyridine-2-formaldehyde and cobalt ion. The structural analysis shows that the window size (0.4 nm) of Co-LBA is just between the kinetic diameters of acetylene (0.334 nm) and ethylene (0.418 nm). In order to avoid the limitation of adsorption kinetics of acetylene by Co-LBA microporous structure, it is further dispersed on graphene oxide (GO) substrate by impregnation method, and a stable Co-LBA functionalized graphene material with hierarchical structure (Co-LBA@rGO) is obtained by calcination. The results of transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR) and N2 adsorption show that Co-LBA keeps a cage structure and is highly dispersed in the interlayer of graphene in Co-LBA@rGO composites, so that the materials have both microporous and mesoporous molecular diffusion channels. At room temperature, Co-LBA@rGO shows remarkable selective adsorption of acetylene, when p/p0 is 0.5, the adsorption ratio of acetylene to ethylene reaches 12.5, which has a potential application prospect for alkene/alkyne separation. |
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