Metal-Organic Framework Supported Single Site Chromium(III) Catalyst for Ethylene Oligomerization at Low Pressure and Temperature

Timothy A. Goetjen, Xuan Zhang, Jian Liu, Joseph T Hupp, Omar K. Farha

Research output: Contribution to journalArticle

5 Citations (Scopus)

Abstract

A chemically and thermally stable, mesoporous, crystalline metal-organic framework, NU-1000, serves as a structurally well-defined support for catalytic reactions. Depositing chromium(III), a metal widely used in homogeneous ethylene oligomerization catalysts, onto the Zr6 node of NU-1000 allows for the atomically precise determination of the structure of the Cr3+ catalyst through single-crystal X-ray diffraction studies. Chromium modification of NU-1000 was accomplished via solvothermal deposition in MOFs (SIM); termed Cr-SIM-NU-1000, the elaborated material features individual Cr atoms directed in single-site fashion into the mesopore of NU-1000. It was found that NU-1000 serves to stabilize the catalyst against both the typical chemical deactivation of homogeneous systems and leaching from heterogeneous systems. Cr-SIM-NU-1000 exhibits superior catalytic activity, as compared to Cr2O3, for ethylene oligomerization, with 20% conversion at a turnover frequency of about 60 h-1 and products ranging from C8-C28. Given that this catalysis occurs at low temperature (ambient) and low pressure (1 bar C2H4), along with minimal quantity of cocatalyst, the high activity shown by Cr-SIM-NU-1000 enables significant reduction in materials usage and waste. Postcatalytic characterization reveals Cr-SIM-NU-1000 remains intact with no leaching under the reaction conditions.

Original languageEnglish
Pages (from-to)2553-2557
Number of pages5
JournalACS Sustainable Chemistry and Engineering
Volume7
Issue number2
DOIs
Publication statusPublished - Jan 22 2019

Fingerprint

Oligomerization
Chromium
ethylene
chromium
low pressure
Ethylene
Metals
catalyst
Catalysts
metal
Leaching
Temperature
leaching
catalysis
Catalysis
Catalyst activity
turnover
X-ray diffraction
Single crystals
crystal

Keywords

  • Ethylene oligomerization
  • Heterogeneous catalysis
  • Metal-organic frameworks
  • Single-crystal

ASJC Scopus subject areas

  • Chemistry(all)
  • Environmental Chemistry
  • Chemical Engineering(all)
  • Renewable Energy, Sustainability and the Environment

Cite this

Metal-Organic Framework Supported Single Site Chromium(III) Catalyst for Ethylene Oligomerization at Low Pressure and Temperature. / Goetjen, Timothy A.; Zhang, Xuan; Liu, Jian; Hupp, Joseph T; Farha, Omar K.

In: ACS Sustainable Chemistry and Engineering, Vol. 7, No. 2, 22.01.2019, p. 2553-2557.

Research output: Contribution to journalArticle

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