Nanoporous Palladium Hydride for Electrocatalytic N Reduction under Ambient Conditions.

Angew Chem Int Ed Engl

Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Engineering Research Center of High-efficiency Energy Storage (Ministry of Education), Renewable Energy Conversion and Storage Center, College of Chemistry, Nankai University, Tianjin, 300071, China.

Published: February 2020

The electrocatalytic nitrogen reduction reaction (NRR) is an alternative eco-friendly strategy for sustainable N fixation with renewable energy. However, NRR suffers from sluggish kinetics owing to difficult N adsorption and N≡N cleavage. Now, nanoporous palladium hydride is reported as electrocatalyst for electrochemical N reduction under ambient conditions, achieving a high ammonia yield rate of 20.4 μg h  mg with a Faradaic efficiency of 43.6 % at low overpotential of 150 mV. Isotopic hydrogen labeling studies suggest the involvement of lattice hydrogen atoms in the hydride as active hydrogen source. In situ Raman analysis and density functional theory (DFT) calculations further reveal the reduction of energy barrier for the rate-limiting *N H formation step. The unique protonation mode of palladium hydride would provide a new insight on designing efficient and robust electrocatalysts for nitrogen fixation.

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http://dx.doi.org/10.1002/anie.201914335DOI Listing

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