Computationally Guided Discovery of a Catalytic Cobalt-Decorated Metal-Organic Framework for Ethylene Dimerization

Varinia Bernales, Aaron B. League, Zhanyong Li, Neil M. Schweitzer, Aaron W. Peters, Rebecca K. Carlson, Joseph T Hupp, Christopher J. Cramer, Omar K. Farha, Laura Gagliardi

Research output: Contribution to journalArticle

30 Citations (Scopus)

Abstract

The catalytic performance of a cobalt(II) single-site catalyst supported on the zirconia-like nodes of the metal organic-framework (MOF) NU-1000 is herein characterized by quantum chemical methods and compared to an iso-structural analogue incorporating nickel(II) as the active transition metal. The mechanisms of atomic layer deposition in MOFs and of catalysis are examined using density functional theory. We compare the catalytic activity of Co and Ni installed on the zirconia-like nodes for ethylene dimerization, considering three plausible pathways. Multiconfigurational wave function theory methods are employed to further characterize the electronic structures of key transition states and intermediates. Finally, we report confirmation of Co catalytic activity for ethylene dimerization from experiments that were prompted by the computational prediction.

Original languageEnglish
Pages (from-to)23576-23583
Number of pages8
JournalJournal of Physical Chemistry C
Volume120
Issue number41
DOIs
Publication statusPublished - Oct 20 2016

Fingerprint

Dimerization
dimerization
Cobalt
Nickel
zirconium oxides
Zirconia
catalytic activity
Catalyst activity
Ethylene
ethylene
cobalt
Metals
nickel
Atomic layer deposition
atomic layer epitaxy
Wave functions
Electron transitions
Catalyst supports
metals
Catalysis

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Surfaces, Coatings and Films
  • Physical and Theoretical Chemistry

Cite this

Bernales, V., League, A. B., Li, Z., Schweitzer, N. M., Peters, A. W., Carlson, R. K., ... Gagliardi, L. (2016). Computationally Guided Discovery of a Catalytic Cobalt-Decorated Metal-Organic Framework for Ethylene Dimerization. Journal of Physical Chemistry C, 120(41), 23576-23583. https://doi.org/10.1021/acs.jpcc.6b07362

Computationally Guided Discovery of a Catalytic Cobalt-Decorated Metal-Organic Framework for Ethylene Dimerization. / Bernales, Varinia; League, Aaron B.; Li, Zhanyong; Schweitzer, Neil M.; Peters, Aaron W.; Carlson, Rebecca K.; Hupp, Joseph T; Cramer, Christopher J.; Farha, Omar K.; Gagliardi, Laura.

In: Journal of Physical Chemistry C, Vol. 120, No. 41, 20.10.2016, p. 23576-23583.

Research output: Contribution to journalArticle

Bernales, V, League, AB, Li, Z, Schweitzer, NM, Peters, AW, Carlson, RK, Hupp, JT, Cramer, CJ, Farha, OK & Gagliardi, L 2016, 'Computationally Guided Discovery of a Catalytic Cobalt-Decorated Metal-Organic Framework for Ethylene Dimerization', Journal of Physical Chemistry C, vol. 120, no. 41, pp. 23576-23583. https://doi.org/10.1021/acs.jpcc.6b07362
Bernales, Varinia ; League, Aaron B. ; Li, Zhanyong ; Schweitzer, Neil M. ; Peters, Aaron W. ; Carlson, Rebecca K. ; Hupp, Joseph T ; Cramer, Christopher J. ; Farha, Omar K. ; Gagliardi, Laura. / Computationally Guided Discovery of a Catalytic Cobalt-Decorated Metal-Organic Framework for Ethylene Dimerization. In: Journal of Physical Chemistry C. 2016 ; Vol. 120, No. 41. pp. 23576-23583.
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