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2026年2期
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Hydrogen Spillover-Enabled Pd/CeO2 Interface Catalysis for Highly Efficient Electrochemical Nitrate-to-Ammonia Conversion
Hydrogen Spillover-Enabled Pd/CeO2 Interface Catalysis for Highly Efficient Electrochemical Nitrate-to-Ammonia Conversion
摘要
The electrocatalytic nitrate reduction reaction(NO3RR)provides a sustainable route for nitrogen pollution remediation and ammonia production under ambient conditions.However,the process involves sluggish multi-electron/proton transfer and suffers from competing hydrogen evolution(HER)which severely limits efficiency and selectivity.Herein,we construct a Pdx-CeO2/C composite catalyst,in which strong interactions between Pd and CeO2 induce interfacial electronic redistribution,thereby effectively modulating the Pd electronic structure.This interfacial coupling enhances water dissociation,accelerates the generation of reactive*H,and promotes its spillover from Pd to CeO2.In-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)confirms that hydrogen spillovers facilitate stepwise hydrogenation of inter-mediates while suppressing HER.Density functional theory calculations further reveal that Pd-Ce interactions inhibit HER and enable N-O side-on adsorption,shifting the potential-determining step and lowering the reaction barrier,thus boosting electrocatalytic activity.As a result,the optimized 5 wt％Pd-CeO2/C delivers a Faradaic efficiency of 98.0％for ammonia at-0.4 V(vs.RHE),and achieves an ammonia yield rate of 4.17 mmol/(mgPd•h)at-0.6 V.This work offers new insights into the application of interfacial engineering for efficient electrocatalytic ammonia synthesis.
年，卷(期)：
2026, 7(2)
机标分类号：
O643
TP311
R741.02
在线出版日期：
2026年7月27日
