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

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71 Scopus citations


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 (US)
Pages (from-to)23576-23583
Number of pages8
JournalJournal of Physical Chemistry C
Issue number41
StatePublished - Oct 20 2016

Bibliographical note

Funding Information:
We thank Dr. Konstantino, D. Vogiatzis, and Dr. Manuel A. Ortu?o for helpful discussions. This work was supported as part of the Inorganometallic Catalyst Design Center, an EFRC funded by the DOE, Office of Basic Energy Sciences (DESC0012702).

Publisher Copyright:
© 2016 American Chemical Society.


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