Palladium-Modified MoS₂ with Accelerated Water Hydrolysis for Highly Efficient Electrocatalytic Ammonia Production

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Electrocatalytic nitrogen reduction reaction (NRR) under environmental conditions is an environmentally friendly way. However, the first hydrogenation step in the reaction process limits the kinetic process. Herein, we report the synthesis of MS–Pd x ( x = 0.5, 1.0, 1.5) catalysts for electrocatalytic nitrogen reduction by rapid Joule heating preparation of S vacancy-containing MoS 2 with vacancy-induced anchoring of Pd in an Ar/H 2 atmosphere. MS–Pd 1 nanosheets exhibit high activity and selectivity at room temperature, with an NH 3 yield of ∼96.41 μg h –1 mg –1 cat. at −0.50 V vs RHE and a Faradaic efficiency of 39.38% at −0.40 V vs RHE. Density-functional theory (DFT) calculations manifested that the unique activity of MS–Pd 1 stemmed from the effective enhancement of nitrogen adsorption by Mo near its S vacancies and the effective promotion of H 2 O dissociation by MoS 2 after the introduction of Pd, that the generated *H combined with *N 2 instead of generating H 2, and that the effective combination of the two reduced the free-energy barriers for the hydrotropic conversion of *N 2 to *NNH. This study provides new ideas for the design of N 2 electroreduction catalysts and strengthens the understanding of N 2 activation over MoS 2 -based catalysts.