The unique physicochemical properties of transition metal carbides (TMCs) have led to their widespread evaluation for catalytic applications such as the conversion of biomass or environmental chemical pollutants (e.g., CO2, CH4) to commodity chemicals and/or fuels. These materials are traditionally synthesized via carburization pathways where a transition metal salt or metal oxide and a carbon source (e.g., graphite, hydrocarbons, CH4/H2) are heated to high temperatures (600-800 °C). However, these methods offer minimal control over the physical properties of the resultant particles, such as size and morphology, which influences their catalytic performance. Regardless of these limitations, recent investigations into improving catalytic activity of TMCs have revealed that modifying the chemical composition, through doping with transition metals, is a promising method toward enhancing the activity, stability, and/or selectivity of these materials. For example, the addition of ionic metal precursors to TMC surfaces to form alloys has led to improved reactivity for a range of noteworthy transformations including methane decomposition, CO hydrogenation, and CO2 reduction. Herein, we expand upon recent synthetic developments from our group that enabled the preparation of phase-pure molybdenum carbide (α-MoC1-x) nanoparticles (NPs) at relatively mild temperatures (i.e., 300 °C) via a solution-phase synthesis route. Decomposition of late first-row transition metal precursors in the presence of in situ generated α-MoC1-x has resulted in the formation of a series of alloyed carbides, MoxMyC (M = Fe, Co, Ni, Cu). This presentation will focus on the synthesis, structural and spectroscopic characterization, and catalytic performance of NP-MoxMyC catalysts. Comparison of the reactivity of NP-MoxMyC to that of the parent α-MoC1-x particles provides insight into the effects of alloying metal carbides on reductive transformations.

Synthesis of ternary metal carbide nanoparticles via a mild solution-based route for the catalytic conversion of renewable carbon sources

ACS Spring Meeting 2021

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