Insights into the Structure–Activity Relationships in Metal–Organic Framework-Supported Nickel Catalysts for Ethylene Hydrogenation

Wang, Xingjie; Zhang, Xuan; Pandharkar, Riddhish; Lyu, Jiafei; Ray, Debmalya; Yang, Ying; Kato, Satoshi; Liu, Jian; Wasson, Megan C.; Islamoglu, Timur; Li, Zhong; Hupp, Joseph T.; Cramer, Christopher J.; Gagliardi, Laura; Farha, Omar K.

doi:10.1021/acscatal.0c01844

Insights into the Structure–Activity Relationships in Metal–Organic Framework-Supported Nickel Catalysts for Ethylene Hydrogenation

Journal Article · Thu Jul 30 00:00:00 EDT 2020 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.0c01844· OSTI ID:1721720

^[1]; ^[2]; Pandharkar, Riddhish ^[3]; ^[2]; ^[3]; Yang, Ying ^[2]; ^[2]; ^[2]; ^[2]; ^[2]; ^[4]; ^[2]; ^[3]; ^[3]; ^[2]

South China Univ. of Technology, Guangzhou (China); Northwestern Univ., Evanston, IL (United States); University of Minnesota
Northwestern Univ., Evanston, IL (United States)
Univ. of Minnesota, Minneapolis, MN (United States)
South China Univ. of Technology, Guangzhou (China)

Solid supports play an indispensable role in heterogeneous catalysis, as they can directly affect the catalytic activity and selectivity of supported catalysts. However, the specific roles of such supports remain to be demystified owing to the difficulties in obtaining precise structural information on supported catalysts. To understand the effects of MOF topology, pore environment, and metal identity of node supports on the catalytic activity, a Ni catalyst was supported on eight Zr- or Hf-MOFs based on 8-connected nodes: namely M-NU-1200, M-NU-1000, M-NU-1008, and M-NU-1010 (M = Zr, Hf). Single-crystal X-ray diffraction (SCXRD), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and X-ray photoelectron spectroscopy (XPS) were employed to characterize the supported catalyst structures. To investigate the support effects on their activities, the supported Ni catalysts were evaluated by using ethylene hydrogenation as a model reaction. The results revealed that all Hf-based-MOF-supported Ni catalysts exhibited higher catalytic reactivity with TOF (turnover frequency) values at least double of those isostructural Zr counterparts. Additionally, MOFs with less congested metal anchoring sites, as a result of the topology and surrounding pore environment, yielded higher TOFs, suggesting the importance of supports in dictating both the catalyst accessibility and activity. Computational analysis complemented the experimental observations and provided insights into reaction barrier differences and their performance variation. Furthermore, this study demonstrates the essential role of the supports and provides a thought for selecting/designing suitable supports in heterogeneous catalysis.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Minnesota, Minneapolis, MN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); NSF

Grant/Contract Number:: SC0012702

OSTI ID:: 1721720

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 16 Vol. 10; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Zr- and Hf-based MOFs
catalysts
chemical calculations
computational analysis
crystal structure
ethylene hydrogenation
hydrocarbons
metal organic frameworks
nickel catalyst
support effect

CCDC 1991614: Experimental Crystal Structure Determination Xingjie, Wang,; Xuan, Zhang,; Riddhish, Pandharkar, https://doi.org/10.5517/ccdc.csd.cc24vfm2 The current record is supplemented by this dataset	dataset	January 2020
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CCDC 1991617: Experimental Crystal Structure Determination Xingjie, Wang,; Xuan, Zhang,; Riddhish, Pandharkar, https://doi.org/10.5517/ccdc.csd.cc24vfq5 The current record is supplemented by this dataset	dataset	January 2020
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Insights into the Structure–Activity Relationships in Metal–Organic Framework-Supported Nickel Catalysts for Ethylene Hydrogenation

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