Sintering-Resistant Single-Site Nickel Catalyst Supported by Metal-Organic Framework

Zhanyong Li, Neil M. Schweitzer, Aaron B. League, Varinia Bernales, Aaron W. Peters, Andrew Bean Getsoian, Timothy C. Wang, Jeffrey T. Miller, Aleksei Vjunov, John L. Fulton, Johannes A. Lercher, Christopher J. Cramer, Laura Gagliardi, Joseph T Hupp, Omar K. Farha

Research output: Contribution to journalArticle

144 Citations (Scopus)

Abstract

Developing supported single-site catalysts is an important goal in heterogeneous catalysis since the well-defined active sites afford opportunities for detailed mechanistic studies, thereby facilitating the design of improved catalysts. We present herein a method for installing Ni ions uniformly and precisely on the node of a Zr-based metal-organic framework (MOF), NU-1000, in high density and large quantity (denoted as Ni-AIM) using atomic layer deposition (ALD) in a MOF (AIM). Ni-AIM is demonstrated to be an efficient gas-phase hydrogenation catalyst upon activation. The structure of the active sites in Ni-AIM is proposed, revealing its single-site nature. More importantly, due to the organic linker used to construct the MOF support, the Ni ions stay isolated throughout the hydrogenation catalysis, in accord with its long-term stability. A quantum chemical characterization of the catalyst and the catalytic process complements the experimental results. With validation of computational modeling protocols, we further targeted ethylene oligomerization catalysis by Ni-AIM guided by theoretical prediction. Given the generality of the AIM methodology, this emerging class of materials should prove ripe for the discovery of new catalysts for the transformation of volatile substrates.

Original languageEnglish
Pages (from-to)1977-1982
Number of pages6
JournalJournal of the American Chemical Society
Volume138
Issue number6
DOIs
Publication statusPublished - Feb 17 2016

Fingerprint

Nickel
Catalysis
Catalyst supports
Sintering
Hydrogenation
Metals
Catalysts
Catalytic Domain
Ions
Gases
Oligomerization
Atomic layer deposition
Ethylene
Chemical activation
Substrates

ASJC Scopus subject areas

  • Chemistry(all)
  • Catalysis
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Li, Z., Schweitzer, N. M., League, A. B., Bernales, V., Peters, A. W., Getsoian, A. B., ... Farha, O. K. (2016). Sintering-Resistant Single-Site Nickel Catalyst Supported by Metal-Organic Framework. Journal of the American Chemical Society, 138(6), 1977-1982. https://doi.org/10.1021/jacs.5b12515

Sintering-Resistant Single-Site Nickel Catalyst Supported by Metal-Organic Framework. / Li, Zhanyong; Schweitzer, Neil M.; League, Aaron B.; Bernales, Varinia; Peters, Aaron W.; Getsoian, Andrew Bean; Wang, Timothy C.; Miller, Jeffrey T.; Vjunov, Aleksei; Fulton, John L.; Lercher, Johannes A.; Cramer, Christopher J.; Gagliardi, Laura; Hupp, Joseph T; Farha, Omar K.

In: Journal of the American Chemical Society, Vol. 138, No. 6, 17.02.2016, p. 1977-1982.

Research output: Contribution to journalArticle

Li, Z, Schweitzer, NM, League, AB, Bernales, V, Peters, AW, Getsoian, AB, Wang, TC, Miller, JT, Vjunov, A, Fulton, JL, Lercher, JA, Cramer, CJ, Gagliardi, L, Hupp, JT & Farha, OK 2016, 'Sintering-Resistant Single-Site Nickel Catalyst Supported by Metal-Organic Framework', Journal of the American Chemical Society, vol. 138, no. 6, pp. 1977-1982. https://doi.org/10.1021/jacs.5b12515
Li Z, Schweitzer NM, League AB, Bernales V, Peters AW, Getsoian AB et al. Sintering-Resistant Single-Site Nickel Catalyst Supported by Metal-Organic Framework. Journal of the American Chemical Society. 2016 Feb 17;138(6):1977-1982. https://doi.org/10.1021/jacs.5b12515
Li, Zhanyong ; Schweitzer, Neil M. ; League, Aaron B. ; Bernales, Varinia ; Peters, Aaron W. ; Getsoian, Andrew Bean ; Wang, Timothy C. ; Miller, Jeffrey T. ; Vjunov, Aleksei ; Fulton, John L. ; Lercher, Johannes A. ; Cramer, Christopher J. ; Gagliardi, Laura ; Hupp, Joseph T ; Farha, Omar K. / Sintering-Resistant Single-Site Nickel Catalyst Supported by Metal-Organic Framework. In: Journal of the American Chemical Society. 2016 ; Vol. 138, No. 6. pp. 1977-1982.
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