Abstract

Developing highly active and selective electrocatalysts for electrochemical nitrate reduction reaction (NITRR) is very important for synthesizing recyclable ammonia (NH3 ) in an economic and environmentally friendly manner. Despite some encouraging progress, their activity and selectivity have been remarkably slower than expected. In this manuscript, mesoporous palladium-nonmetal (meso-PdX) nanocubes (NCs) are reported as a new series of highly efficient electrocatalysts for selective nitrate reduction reaction (NITRR) electrocatalysis to NH3 . The samples feature uniformly alloyed compositions and highly penetrated mesopores with abundant highly active sites and optimized electronic structures. The best meso-PdN NCs hold an outstanding NITRR activity and selectivity with a remarkable NH3 Faradaic efficiency of 96.1% and a yield rate of 3760µg h-1 mg-1 , suppressing the state-of-the-art electrocatalysts. Meanwhile, meso-PdN NCs are electrocatalytically stable, retaining well the activity and selectivity of NO3 - -to-NH3 electrocatalysis for more than 20 cycles. Detailed mechanism studies ascribe the superior performance to combined compositional and structural synergies of meso-PdN NCs that not only promote the adsorption (reactivity) of NO3 - and the desorption of NH3 but also increase the retention time of key intermediates for the deeper NITRR electrocatalysis to NH3 through an eight-electron pathway.

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