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

doi:10.1021/jacs.6b08711

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

Northwestern University

Research output: Contribution to journal › Article

42 Citations (Scopus)

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 language	English
Pages (from-to)	13513-13516
Number of pages	4
Journal	Journal of the American Chemical Society
Volume	138
Issue number	41
DOIs	https://doi.org/10.1021/jacs.6b08711
Publication status	Published - Oct 19 2016

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ASJC Scopus subject areas

Catalysis
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry

Cite this

Gallington, L. C., Kim, I. S., Liu, W. G., Yakovenko, A. A., Platero-Prats, A. E., Li, Z., Wang, T. C., Hupp, J. T., Farha, O. K., Truhlar, D. G., Martinson, A. B. F., & Chapman, K. W. (2016). Regioselective Atomic Layer Deposition in Metal-Organic Frameworks Directed by Dispersion Interactions. Journal of the American Chemical Society, 138(41), 13513-13516. https://doi.org/10.1021/jacs.6b08711

Regioselective Atomic Layer Deposition in Metal-Organic Frameworks Directed by Dispersion Interactions. / Gallington, Leighanne C.; Kim, In Soo; Liu, Wei Guang; Yakovenko, Andrey A.; Platero-Prats, Ana E.; Li, Zhanyong; Wang, Timothy C.; Hupp, Joseph T; Farha, Omar K.; Truhlar, Donald G.; Martinson, Alex B F; Chapman, Karena W.

In: Journal of the American Chemical Society, Vol. 138, No. 41, 19.10.2016, p. 13513-13516.

Research output: Contribution to journal › Article

Gallington, LC, Kim, IS, Liu, WG, Yakovenko, AA, Platero-Prats, AE, Li, Z, Wang, TC, Hupp, JT, Farha, OK, Truhlar, DG, Martinson, ABF & Chapman, KW 2016, 'Regioselective Atomic Layer Deposition in Metal-Organic Frameworks Directed by Dispersion Interactions', Journal of the American Chemical Society, vol. 138, no. 41, pp. 13513-13516. https://doi.org/10.1021/jacs.6b08711

Gallington, Leighanne C. ; Kim, In Soo ; Liu, Wei Guang ; Yakovenko, Andrey A. ; Platero-Prats, Ana E. ; Li, Zhanyong ; Wang, Timothy C. ; Hupp, Joseph T ; Farha, Omar K. ; Truhlar, Donald G. ; Martinson, Alex B F ; Chapman, Karena W. / Regioselective Atomic Layer Deposition in Metal-Organic Frameworks Directed by Dispersion Interactions. In: Journal of the American Chemical Society. 2016 ; Vol. 138, No. 41. pp. 13513-13516.

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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.",

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AB - 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.

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10.1021/jacs.6b08711