Regioselective Atomic Layer Deposition in Metal-Organic Frameworks Directed by Dispersion Interactions

Leighanne C. Gallington, In Soo Kim, Wei Guang Liu, Andrey A. Yakovenko, Ana E. Platero-Prats, Zhanyong Li, Timothy C. Wang, Joseph T. Hupp, Omar K. Farha, Donald G. Truhlar, Alex B.F. Martinson, Karena W. Chapman

Research output: Contribution to journalArticlepeer-review

52 Scopus citations

Abstract

The application of atomic layer deposition (ALD) to metal-organic frameworks (MOFs) offers a promising new approach to synthesize designer functional materials with atomic precision. While ALD on flat substrates is well established, the complexity of the pore architecture and surface chemistry in MOFs present new challenges. Through in situ synchrotron X-ray powder diffraction, we visualize how the deposited atoms are localized and redistribute within the MOF during ALD. We demonstrate that the ALD is regioselective, with preferential deposition of oxy-Zn(II) species within the small pores of NU-1000. Complementary density functional calculations indicate that this startling regioselectivity is driven by dispersion interactions associated with the preferential adsorption sites for the organometallic precursors prior to reaction.

Original languageEnglish (US)
Pages (from-to)13513-13516
Number of pages4
JournalJournal of the American Chemical Society
Volume138
Issue number41
DOIs
StatePublished - Oct 19 2016

Bibliographical note

Funding Information:
This work was supported as part of the Inorganometallic Catalysis Design Center, an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, under Award No. DESC0012702. It used resources of the Advanced Photon Source, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. A.E.P.-P. acknowledges

Publisher Copyright:
© 2016 American Chemical Society.

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