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Active Hydrogen Enrichment on Cu6Sn5-type High Entropy Intermetallics for Efficient Nitrate Reduction Reaction
Ziwei Xiang1, Ying-Rui Lu2, Linghu Meng1
1College of Materials Science and Engineering, State Key Laboratory of Advanced Design and Manufacturing Technology for Vehicle, Hunan University, Changsha, Hunan, 410082, China.
None:
Electrocatalytic nitrate reduction reaction (NO3RR) provides a feasible strategy for green ammonia production and the treatment of nitrate pollution in wastewater. The generation of active hydrogen (H*) plays an important role in improving the selectivity, yield rate, and Faradaic efficiency of ammonia products. Here, structurally ordered nanoporous Cu6Sn5-type high entropy intermetallics (HEI) with extremely superior performance toward NO3RR is demonstrated. The optimal nanoporous (Cu0.25Ni0.25Fe0.25Co0.25)6Sn5 HEI delivers a high NH3 Faradaic efficiency of 97.09 ± 1.15% and excellent stability of 120 h at the industrial level current density of 1 A cm-2, accordingly directly converting NO3 ‒ to high-purity (NH4)2HPO4 with near-unity efficiency. Theoretical calculations combined with experimental results reveal that the ordered multi-site nature of the nanoporous HEI can simultaneously promote water dissociation, reduce the reaction-free energy of the hydrogenation process, and suppress hydrogen evolution. This work provides the design of the precious-metal-free HEI for sustainable NH3 synthesis and paves insights into the H* enrichment mechanism.
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