Controlling Dissolution and Transformation of Zeolitic Imidazolate Frameworks by using Electron-Beam-Induced Amorphization

Controlling Dissolution and Transformation of Zeolitic Imidazolate Frameworks by using Electron-Beam-Induced Amorphization
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DOI:
10.1002/anie.201809921
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发表时间:
2018-10-08
影响因子:
16.6
通讯作者:
Tsapatsis, Michael
Tsapatsis, Michael
中科院分区:
化学1区
文献类型:
--
作者:
Conrad, Sabrina;Kumar, Prashant;Tsapatsis, Michael

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无定形沸石咪唑酯框架(ZIF)作为新型功能材料具有广阔的应用前景。在此,基于各个ZIF-L晶体的非晶化,证明了通过扫描电子束曝光的ZIF-L的非晶化。非晶化ZIF产品具有显著增加的抗水中溶解的稳定性。建立了允许在浸入水中之后完全保存无定形颗粒的电子剂量,从而产生具有亚微米长度尺度的空间控制的无定形ZIF-L的新形状。对于三种另外的金属有机框架(ZIF-8、Zn(BeIm)0Ac、MIL-101),证明了由于扫描电子束曝光而改变的水稳定性,突出了电子束用于自上而下的MOF图案化的潜在用途。最后,研究了ZIF-L在连接剂存在下的重结晶,并且显示出结晶和非晶化材料的明显差异。
Amorphous zeolitic imidazolate frameworks (ZIFs) offer promising applications as novel functional materials. Herein, amorphization of ZIF-L through scanning-electron-beam exposure is demonstrated, based on amorphization of individual ZIF-L crystals. The amorphized ZIF product has drastically increased stability against dissolution in water. An electron dose that allows for complete preservation of amorphous particles after immersion in water is established, resulting in new shapes of amorphous ZIF-L with spatial control at the sub-micrometer length scale. Changed water stability as a consequence of scanning-electron-beam exposure is demonstrated for three additional metal-organic frameworks (ZIF-8, Zn(BeIm)OAc, MIL-101), highlighting the potential use of an electron beam for top-down MOF patterning. Lastly, recrystallization of ZIF-L in the presence of linker is studied and shows distinct differences for crystalline and amorphized material.