Sequential single-crystal-to-single-crystal vapochromic inclusion in a nonporous coordination polymer: unravelling dynamic rearrangement for selective pyridine sensing

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Abstract

Unprecedent selective and reversible pyridine solid–vapor sequential inclusion in a nonporous Fe( ii) coordination polymer accompanied by a color change is presented. Although the internal reorganization is significant, the process remains SCSC.

Abstract

Beyond zeolites, alternative porous materials such as metal–organic frameworks (MOF) and covalent organic frameworks (COF) have provided a variety of materials with potential applications ranging from sensing to catalysis. However, less attention has been paid to nonporous materials acting in a porous fashion, probably because of the lack of structural data. Herein, we present the unprecedented selective solid–vapour sequential inclusion of pyridine in a nonporous Fe( ii) coordination polymer. Even though this reorganization leads to a dramatic transformation of the initial 2D structure, through a 1D intermediate structure, to a 0D compound, these transformations remain single-crystal to single-crystal. Remarkably, pyrazine substitution is accompanied by a naked-eye colour change, and the process is reversible. In addition, this molecular process also takes place when the coordination polymer is embedded in a polymeric matrix.

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The chemistry and applications of metal-organic frameworks.

Hiroyasu Furukawa, Kyle E. Cordova, Michael O'Keeffe … (2013)

Crystalline metal-organic frameworks (MOFs) are formed by reticular synthesis, which creates strong bonds between inorganic and organic units. Careful selection of MOF constituents can yield crystals of ultrahigh porosity and high thermal and chemical stability. These characteristics allow the interior of MOFs to be chemically altered for use in gas separation, gas storage, and catalysis, among other applications. The precision commonly exercised in their chemical modification and the ability to expand their metrics without changing the underlying topology have not been achieved with other solids. MOFs whose chemical composition and shape of building units can be multiply varied within a particular structure already exist and may lead to materials that offer a synergistic combination of properties.

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De novo synthesis of a metal-organic framework material featuring ultrahigh surface area and gas storage capacities.

Omar K. Farha, A. Özgür Yazaydın, Ibrahim Eryazici … (2010)

Metal-organic frameworks--a class of porous hybrid materials built from metal ions and organic bridges--have recently shown great promise for a wide variety of applications. The large choice of building blocks means that the structures and pore characteristics of the metal-organic frameworks can be tuned relatively easily. However, despite much research, it remains challenging to prepare frameworks specifically tailored for particular applications. Here, we have used computational modelling to design and predictively characterize a metal-organic framework (NU-100) with a particularly high surface area. Subsequent experimental synthesis yielded a material, matching the calculated structure, with a high BET surface area (6,143 m(2) g(-1)). Furthermore, sorption measurements revealed that the material had high storage capacities for hydrogen (164 mg g(-1)) and carbon dioxide (2,315 mg g(-1))--gases of high importance in the contexts of clean energy and climate alteration, respectively--in excellent agreement with predictions from modelling.