Abstract

<h2>Summary</h2> Modulating the oxygen-metal interface that enables efficient and selective C–H activation remains challenging. Herein, we present a novel MoC<sub>x</sub>O<sub>y</sub> oxygen carrier for syngas production via the chemical looping CH<sub>4</sub>–CO<sub>2</sub> reforming (CL-DRM) reaction. Molybdenum carbide additive induces the re-dispersion of Ni particles from Al<sub>2</sub>O<sub>3</sub> surface to α-MoC driven by the strong interaction between Ni and α-MoC. A dynamic structure transformation between MoC<sub>x</sub> and MoC<sub>x</sub>O<sub>y</sub> occurs and new Ni–MoC<sub>x</sub>O<sub>y</sub> interfaces form during the redox cycling, which is discovered to be crucial for the low-temperature CH<sub>4</sub> activation using surface construction experiments and <i>in-situ</i> spectroscopic methods. As a result, Ni–(α-MoC)/Al<sub>2</sub>O<sub>3</sub> exhibits near 100% selectivity to syngas with a H<sub>2</sub>/CO ratio of 2:1 at 500°C, which is a significantly lower temperature than that of conventional systems. This study first employs molybdenum carbide as an oxygen storage material (OSM) in CL-DRM reaction, paving the way of utilizing transition metal carbides as OSMs in chemical looping processes.

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