Metal–Organic Frameworks Derived from Zero-Valent Metal Substrates: Mechanisms of Formation and Modulation of Properties

Jieun Kim, Seungju Lee, Jaesung Kim, Doohwan Lee

Research output: Contribution to journalArticlepeer-review

21 Scopus citations

Abstract

The replicative construction of metal–organic frameworks (MOFs) templated with solvent-insoluble solid substrates is of marked importance, as it allows for the assembly of 2D and 3D macro- and mesoscopic architectures with properties that are challenging to attain by the conventional solution-based synthesis approach. This work reports an in situ and direct construction of MOFs from zero-valent metal substrates via a green hydrothermal oxidation–MOF construction chemistry without the use of any additional metal source, chemical reagents, or acidification of solvent, and elucidates the zero-valent metal derived formation mechanisms of MOFs and their structure modulation to 1D nanofibers (NFs), 2D film, and 3D core–shell microstructures. Through modulation of the competing surface oxidation-dissolution and MOF crystallization kinetics, Al@MIL-53 core–shell microstructures and MIL-53 (Al) NFs are obtained that exhibit unique morphologies and marked properties superior to the conventional MIL-53 (Al) powders. The generality of zero-valent metal-templated synthesis of MOFs is demonstrated with formation of MIL-53 (Al), HKUST-1, and ZIF-7 polycrystalline films on Al, Cu, and Zn metal meshes, elucidating the significance of the approach utilizing solid metal substrate that can be easily processed into various shapes, architectures, and compositions.

Original languageEnglish
Article number1808466
JournalAdvanced Functional Materials
Volume29
Issue number8
DOIs
StatePublished - 21 Feb 2019

Keywords

  • MOF nanofibers
  • core–shell structure
  • formation mechanism
  • metal–organic framework
  • templated synthesis

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