Visible light-mediated supramolecular framework for tunable CO2 adsorption

Tao Yang, Chunyi Yu, Chen Gu, Yang Liu, Hui Wen, Xiao Qin Liu, Guoliang Liu, Lifeng Ding, Lin Bing Sun

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3 引用 (Scopus)

摘要

In the pursuit of creating azobenzene-functionalized photo-responsive supramolecular frameworks (PSMFs) activated by the visible spectrum, an endeavor traditionally relied on ultraviolet activation, we report the successful fabrication of a visible light-mediated metal–organic cage-based PSMF, designated as NUT-104. This achievement was realized by the hierarchical self-assembly process of Zr-metal–organic cages featuring ortho-fluoroazobenzene functional terephthalic acid and tri-nuclear Zr-clusters. NUT-104 displays permanent porosity coupled with reversible responsiveness to visible light. This remarkable behavior emerges as a consequence of the σ-electron-withdrawing effect induced by the presence of fluorine substituents. Visible light-regulated CO2 adsorption capacity can be achieved and the change value can reach 61 %, while the change for CH4 and N2 is only 7 % and 3 %, respectively. In response to irradiation at wavelengths of 520 and 420 nm, respectively, the azobenzene moieties within the NUT-104 structure exhibit a remarkable capacity for visible light-controlled reversible conformational changes. Grand Canonical Monte Carlo simulations unveiled that the dynamic reorganization of the NUT-104 proficiently governs the accessibility of CO2 adsorption sites positioned within the interstitial regions of proximate cages. The advent of NUT-104, underpinned by its visible light responsiveness and versatile tunability, paves the way for avenues of exploration in controlled gas separation and storage applications.

源语言英语
文章编号150254
期刊Chemical Engineering Journal
486
DOI
出版状态已出版 - 15 4月 2024

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