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Nanoporous Palladium Hydride for Electrocatalytic N 2 Reduction under Ambient Conditions
Author(s) -
Xu Wence,
Fan Guilan,
Chen Jialiang,
Li Jinhan,
Zhang Le,
Zhu Shengli,
Su Xuncheng,
Cheng Fangyi,
Chen Jun
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201914335
Subject(s) - overpotential , hydride , palladium hydride , palladium , faraday efficiency , chemistry , electrocatalyst , inorganic chemistry , electrochemistry , hydrogen , density functional theory , nanoporous , hydrogen storage , rate determining step , catalysis , electrode , computational chemistry , organic chemistry
The electrocatalytic nitrogen reduction reaction (NRR) is an alternative eco‐friendly strategy for sustainable N 2 fixation with renewable energy. However, NRR suffers from sluggish kinetics owing to difficult N 2 adsorption and N≡N cleavage. Now, nanoporous palladium hydride is reported as electrocatalyst for electrochemical N 2 reduction under ambient conditions, achieving a high ammonia yield rate of 20.4 μg h −1 mg −1 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 2 H formation step. The unique protonation mode of palladium hydride would provide a new insight on designing efficient and robust electrocatalysts for nitrogen fixation.