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In situ X-ray diffraction monitoring of a mechanochemical reaction reveals a unique topology metal-organic framework

Katsenis, Athanassios D.; Puškarić, Andreas; Štrukil, Vjekoslav; Mottillo, Cristina; Julien, Patrick A.; Užarević, Krunoslav; Pham, Minh-Hao; Do, Trong-On; Kimber, Simon A.J.; Lazić, Predrag; Magdysyuk, Oxana; Dinnebier, Robert E.; Halasz, Ivan; Friščić, Tomislav (2015) In situ X-ray diffraction monitoring of a mechanochemical reaction reveals a unique topology metal-organic framework. Nature Communications, 6 . pp. 6662-1. ISSN 2041-1723

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Abstract

Chemical and physical transformations by milling are attracting enormous interest for their ability to access new materials and clean reactivity, and are central to a number of core industries, from mineral processing to pharmaceutical manufacturing. While continuous mechanical stress during milling is thought to create an environment supporting non- conventional reactivity and exotic intermediates, such speculations have remained without proof. Here we use in situ, real-time powder X-ray diffraction monitoring to discover and capture a metastable, novel-topology intermediate of a mechanochemical transformation. Monitoring the mechanochemical synthesis of an archetypal metal-organic framework ZIF-8 by in situ powder X-ray diffraction reveals unexpected amorphization, and on further milling recrystallization into a non-porous material via a metastable intermediate based on a previously unreported topology, herein named katsenite (kat). The discovery of this phase and topology provides direct evidence that milling transformations can involve short-lived, structurally unusual phases not yet accessed by conventional chemistry.

Item Type: Article
Uncontrolled Keywords: mechanochemistry; in situ powder diffraction; metal-organic framework; topology; katsenite
Subjects: NATURAL SCIENCES > Chemistry
NATURAL SCIENCES > Chemistry > Physical Chemistry
NATURAL SCIENCES > Chemistry > Inorganic Chemistry
Divisions: Division of Materials Chemistry
Division of Organic Chemistry and Biochemistry
Division of Physical Chemistry
Theoretical Physics Division
Depositing User: Krunoslav Užarević
Date Deposited: 01 Dec 2016 12:49
Last Modified: 01 Dec 2016 12:49
URI: http://fulir.irb.hr/id/eprint/3158
DOI: 10.1038/ncomms7662

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