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Silicon Nitride Surface Enabled Propane Dehydrogenation Catalyzed by Supported Organozirconium

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.4c02776· OSTI ID:2367356
 [1];  [1];  [1];  [2];  [1];  [3];  [1];  [1];  [1];  [1];  [1]
  1. Argonne National Laboratory (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  2. Argonne National Laboratory (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; Northwestern University, Evanston, IL (United States)
  3. Ames Laboratory (AMES), Ames, IA (United States). Chemical and Biological Sciences Division; Iowa State University, Ames, IA (United States)
+ Show Author Affiliations
Mesoporous silicon nitride (Si3N4) is a nontraditional support for the chemisorption of organometallic complexes with the potential for enhancing catalytic activity through features such as the increased Lewis basicity of nitrogen for heterolytic bond activation, increased ligand donor strength, and metal–ligand orbital overlap. In this report tetrabenzyl zirconium (ZrBn4) was chemisorbed on Si3N4, and the resulting supported organometallic species was characterized by Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS), Dynamic Nuclear Polarization-enhanced Solid State Nuclear Magnetic Resonance (DNP-SSNMR), and X-ray Absorption Spectroscopy (XAS). Based on the hypothesis that the nitride might enable facile heterolytic C–H bond activation along the Zr–N bond, this material was found to be a highly active (1.53 molpropene molZr–1 h–1 at 450 °C) and selective (99% to propylene) catalyst for propane dehydrogenation. In contrast, the homologous silica supported complex exhibited negligible activity under these conditions.
Research Organization:
Ames Laboratory (AMES), Ames, IA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
Grant/Contract Number:
AC02-06CH11357; AC02-07CH11358
OSTI ID:
2367356
Alternate ID(s):
OSTI ID: 2500809
Report Number(s):
IS-J--11,340
Journal Information:
Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 21 Vol. 146; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
heterogeneous catalysis
propane dehydrogenation
surface organometallic chemistry
zirconium