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An Exceptionally Mild and Scalable Solution-Phase Synthesis of Molybdenum Carbide Nanoparticles for Thermocatalytic CO2 Hydrogenation

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.9b11238· OSTI ID:1592083
 [1];  [2];  [1];  [2];  [1];  [1];  [3];  [4];  [1];  [1];  [2];  [2]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States). National Bioenergy Center
  2. Univ. of Southern California, Los Angeles, CA (United States)
  3. Univ. of New South Wales, Sydney, NSW (Australia)
  4. Illinois Inst. of Technology, Chicago, IL (United States)
+ Show Author Affiliations
Transition metal carbides (TMCs) have demonstrated outstanding potential for utilization in a wide range of catalytic applications because of their inherent multifunctionality and tunable composition. However, the harsh conditions required to prepare these materials have limited the scope of synthetic control over their physical properties. The development of low-temperature, carburization-free routes to prepare TMCs would unlock the versatility of this class of materials, enhance our understanding of their physical properties, and enable their cost-effective production at industrial scales. Here in this paper, we report an exceptionally mild and scalable solution-phase synthesis route to phase-pure molybdenum carbide (α-MoC1-x) nanoparticles (NPs) in a continuous flow millifluidic reactor. We exploit the thermolytic decomposition of Mo(CO)6 in the presence of a surface-stabilizing ligand and a high boiling point solvent to yield MoC1-x NPs that are colloidally stable and resistant to bulk oxidation in air. To demonstrate the utility of this synthetic route to prepare catalytically active TMC NPs, we evaluated the thermochemical CO2 hydrogenation performance of α-MoC1-x NPs dispersed on an inert carbon support. The α-MoC1-x/C catalyst exhibited a 2-fold increase in both activity on a per-site basis and selectivity to C2+ products as compared to the bulk α-MoC1-x analogue.
Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Bioenergy Technologies Office (EE-3B)
Grant/Contract Number:
AC02-06CH11357; AC36-08GO28308
OSTI ID:
1592083
Alternate ID(s):
OSTI ID: 1598023
Report Number(s):
NREL/JA-5100-75569
Journal Information:
Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 2 Vol. 142; 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
CCTPL
catalysis
nanoparticles
transition metal carbides