Integration of mesopores and crystal defects in metal-organic frameworks via templated electrosynthesis

Xinchen Kang, Kai Lyu, Lili Li, Jiangnan Li, Louis Kimberley, Bin Wang, Lifei Liu, Yongqiang Cheng, Mark D. Frogley, Svemir Rudić, Anibal J. Ramirez-Cuesta, Robert A.W. Dryfe, Buxing Han, Sihai Yang, Martin Schröder

Research output: Contribution to journalArticlepeer-review

95 Scopus citations

Abstract

Incorporation of mesopores and active sites into metal-organic framework (MOF) materials to uncover new efficient catalysts is a highly desirable but challenging task. We report the first example of a mesoporous MOF obtained by templated electrosynthesis using an ionic liquid as both electrolyte and template. The mesoporous Cu(II)-MOF MFM-100 has been synthesised in 100 seconds at room temperature, and this material incorporates crystal defects with uncoupled Cu(II) centres as evidenced by confocal fluorescence microscopy and electron paramagnetic resonance spectroscopy. MFM-100 prepared in this way shows exceptional catalytic activity for the aerobic oxidation of alcohols to produce aldehydes in near quantitative yield and selectivity under mild conditions, as well as having excellent stability and reusability over repeated cycles. The catalyst-substrate binding interactions have been probed by inelastic neutron scattering. This study offers a simple strategy to create mesopores and active sites simultaneously via electrochemical formation of crystal defects to promote efficient catalysis using MOFs.

Original languageEnglish
Article number4466
JournalNature Communications
Volume10
Issue number1
DOIs
StatePublished - Dec 1 2019

Funding

We thank EPSRC (EP/I011870), ERC (AdG 742041), the Royal Society, University of Manchester and Institute of Chemistry, Chinese Academy of Science for funding. X.K. is supported by a Royal Society Newton International Fellowship. We are especially grateful to Diamond Light Source and STFC/ISIS Facility for access to the Beamlines B22 and TOSCA, respectively. The computing resources were made available through the VirtuES and the ICE-MAN projects, funded by Laboratory Directed Research and Development programme at ORNL. KL and JL acknowledge the China Scholarship Council for support of PhD studentships.

Fingerprint

Dive into the research topics of 'Integration of mesopores and crystal defects in metal-organic frameworks via templated electrosynthesis'. Together they form a unique fingerprint.

Cite this