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Zeolitic Imidazolate Framework Membrane with Marked Thermochemical Stability for High-Temperature Catalytic Processes
Chemistry of Materials ( IF 7.2 ) Pub Date : 2018-01-03 00:00:00 , DOI: 10.1021/acs.chemmater.7b04409
Seungju Lee 1 , Jaesung Kim 1 , Jieun Kim 1 , Doohwan Lee 1
Affiliation  

The thermochemical stability of metal organic framework (MOF) membranes is vital for the application in chemical-reaction and -separation processes, but understanding the stability of MOF membranes and structure–property relationships under antagonistic chemical atmosphere is still required. In this work, a supported zeolitic imidazolate framework (ZIF) membrane, ZIF-7/MgO-Al2O3, of unprecedented hydrothermal stability is obtained by a modulation of the acid–base chemistry at the membrane/support interface. The solid/solid interface acidity that has been overlooked in the fields turns out to have paramount inducing effects on the thermochemical stability of ZIF membranes, resulting in the catastrophic acid-catalyzed decomposition of ZIF frameworks at atomic level. The ZIF-7/MgO-Al2O3 of marked thermochemical stability permits the first significant application of MOF membranes for catalytic membrane reactor (MR) in severe and practical process conditions, performing water–gas shift reaction (CO + H2O ↔ CO2 + H2) at considerably high temperatures (473–673 K) and steam concentrations (20–40%). The findings and results provide significant new insights on the property and stability of ZIF membranes with extensive opportunities for thermochemical processes that have been permitted only for the inorganic membranes such as zeolites, palladium, and metal oxides.

中文翻译:

具有明显热化学稳定性的沸石咪唑酸酯骨架膜,适用于高温催化过程

金属有机骨架(MOF)膜的热化学稳定性对于在化学反应和分离过程中的应用至关重要,但是仍然需要了解在不利的化学气氛下MOF膜的稳定性和结构-性质之间的关系。在这项工作中,通过调节膜/载体界面的酸碱化学性质,获得了具有前所未有的水热稳定性的负载的沸石咪唑酸盐骨架(ZIF)膜ZIF-7 / MgO-Al 2 O 3。在该领域中被忽视的固体/固体界面酸度被证明对ZIF膜的热化学稳定性具有最重要的诱导作用,从而导致在原子水平上灾难性酸催化的ZIF骨架分解。ZIF-7 / MgO-Al2 O 3具有显着的热化学稳定性,使得MOF膜首次在苛刻和实际的工艺条件下显着应用于催化膜反应器(MR),可在相当高的温度下进行水煤气变换反应(CO + H 2 O↔CO 2 + H 2)高温(473–673 K)和蒸汽浓度(20–40%)。这些发现和结果为ZIF膜的性能和稳定性提供了重要的新见识,并为热化学过程提供了广阔的机会,而热化学过程仅适用于诸如沸石,钯和金属氧化物的无机膜。
更新日期:2018-01-03
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