Entropy-Driven Mechanochemical Synthesis of Polymetallic Zeolitic Imidazolate Frameworks for CO2 Fixation

Angew Chem Int Ed Engl. 2019 Apr 1;58(15):5018-5022. doi: 10.1002/anie.201900787. Epub 2019 Mar 6.

Abstract

High-entropy materials refer to a kind of materials in which five or more metal species were incorporated deliberately into a single lattice with random occupancy. Up to now, such a concept has been only restricted to hard materials, such as high-entropy alloys and ceramics. Herein we report the synthesis of hybrid high-entropy materials, polymetallic zeolitic imidazolate framework (also named as high-entropy zeolitic imidazolate framework, HE-ZIF), via entropy-driven room-temperature mechanochemistry. HE-ZIF contains five metals including ZnII , CoII , CdII , NiII , and CuII which are dispersed in the ZIF structure randomly. Moreover, HE-ZIF shows enhanced catalytic conversion of CO2 into carbonate compared with ZIF-8 presumably a result of the synergistic effect of the five metal ions as Lewis acid in epoxide activation.

Keywords: carbon dioxide fixation; high-entropy materials; mechanochemistry; metal-organic frameworks; zeolitic imidazolate frameworks.