Authors: Peng Jing, Peixin Liu, Minghao Hu, Xuan Xu, Baocang Liu, Jun Zhang
Published: 2022-05-09
Source: Full article
AbstractElectrochemical nitrogen reduction powered by renewable electricity is a promising strategy to produce ammonia. However, the lack of efficient yet cheap electrocatalysts remains the biggest challenge. Herein, hybrid Cu2O‐CeO2‐C nanorods are prepared on copper mesh through a metal‐organic framework template route. The Cu‐loaded Ce‐MOF is thermally converted to Cu2O‐CeO2 heterojunctions with interfacial Cu‐[OX]‐Ce structures embedded in carbon. Theoretical calculations reveal the lower formation energy of oxygen vacancies in Cu‐[OX]‐Ce structures than in the Cu2O or CeO2 phase. The Cu‐[OX]‐Ce structures with oxygen vacancies enable the formation of interfacial electron‐rich Cu(I) species which show significantly enhanced performance toward electrocatalytic nitrogen reduction with an NH3 yield of 6.37 × 10−3 µg s−1 cm−2 and a Faradaic efficiency of 18.21% in 0.10 m KOH at −0.3 V versus reversible hydrogen electrode. This work highlights the importance of modulation of charge distribution of Cu‐based electrocatalysts to boost the activity toward nitrogen reduction.