Reversible Solid-State Isomerism of Azobenzene-Loaded Large-Pore Isoreticular Mg-CUK-1,Journal of the American Chemical Society

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Reversible Solid-State Isomerism of Azobenzene-Loaded Large-Pore Isoreticular Mg-CUK-1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-03-18 , DOI: 10.1021/jacs.9b13793
Junpeng He ₁ , Kanchan Aggarwal ₁ , Naman Katyal ₁ , Shichao He ₁ , Edward Chiang ₁ , Samuel G. Dunning ₁ , Joseph E. Reynolds ₁ , Alexander Steiner ₂ , Graeme Henkelman ₁ , Emily L. Que ₁ , Simon M. Humphrey ₁

Affiliation

A large-pore version of Mg-CUK-1, a water-stable MOF with 1-D channels, was synthesized in basic water. Mg-CUK-1L has a BET surface area of 2,896 m2 g-1 and shows a stark selectivity for CO2 sorption over N2, O2, H2, and CH4. It displays reversible, multi-step gated sorption of CO2 below 0.33 atm. The dehydrated single crystal structure of Mg-CUK-1L confirms retention of the open channel structure. The MOF is thermally stable up to 450 °C and can be loaded with organic molecules by direct immersion in hot melts, providing single crystals suitable for X-ray diffraction. Trans-azobenzene fills the channels in a 2×2 end-to-end fashion. Solid-state UV-Vis spectroscopy of the composite reveals that azobenzene molecules undergo fully reversible trans-cis isomerization, despite being close-packed; this surprising result is confirmed by DFT-simulated UV-vis spectra.

中文翻译：

载有偶氮苯的大孔等网状Mg-CUK-1的可逆固态异构

在碱性水中合成了大孔版本的 Mg-CUK-1，一种具有一维通道的水稳定 MOF。Mg-CUK-1L 的 BET 表面积为 2,896 m2 g-1，对 CO2 吸附比 N2、O2、H2 和 CH4 显示出明显的选择性。它显示了 0.33 atm 以下的 CO2 的可逆、多步门控吸附。Mg-CUK-1L 的脱水单晶结构证实了开放通道结构的保留。MOF 在高达 450 °C 的温度下具有热稳定性，并且可以通过直接浸入热熔体中来装载有机分子，从而提供适用于 X 射线衍射的单晶。反式偶氮苯以 2×2 端到端方式填充通道。复合材料的固态 UV-Vis 光谱显示偶氮苯分子尽管是密堆积的，但仍会发生完全可逆的反式-顺式异构化；

更新日期：2020-03-18

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