电催化剂
法拉第效率
催化作用
氨生产
电化学
化学
无机化学
尖晶石
X射线光电子能谱
化学工程
氨
可逆氢电极
材料科学
电极
物理化学
工作电极
有机化学
工程类
冶金
作者
Dohun Kim,Subramani Surendran,Yoongu Lim,Hyeonuk Choi,Jaehyoung Lim,Joon‐Young Kim,Mi‐Kyung Han,Uk Sim
摘要
The electrochemical nitrogen reduction reaction (ENRR) is considered an environmentally-friendly process for ammonia production under ambient conditions, compared to the conventional Haber-Bosch method. However, the electrochemical synthesis of ammonia suffers from poor selectivity and low efficiency owing to constrained catalytic activity and the competitive hydrogen evolution reaction (HER). Spinel-type solid materials have received considerable interest owing to their various applications in catalysis, energy storage, and optical devices. Particularly, mixed transition-metal oxides with a formula of A2BO4 exhibit improved catalytic activity owing to the presence of multiple balance sites for cations (A2+/3+ and B2+/3+/4+) in their structure. In this study, Ni2GeO4 nanoparticles synthesized via a facile hydrothermal method were investigated as a novel electrocatalyst for the ENRR. X-ray photoelectron spectroscopy confirmed the presence of octahedrally-coordinated Ni2+ and tetrahedrally-coordinated Ge4+ in the prepared spinel-type Ni2GeO4 material. Notably, the Ni2GeO4 electrocatalyst achieved an excellent Faradaic efficiency of 3.57% and an ammonia yield rate of 3.06 μg h−1 cm−2 at −0.1 V vs RHE, owing to the enhanced charge transfer and chemical activity caused by charge polarization between the polyhedral units. The results of this primary investigation can inspire the development of Ni2GeO4-based electrocatalysts using innovative approaches to realize superior ENRR activity.
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