Xie Hui-Qi, Zheng Xuan, Feng Qing-Yun, Chen Xiao-Ping, Zou Ze-Hua, Wang Qing-Xiang, Tang Jing, Li Yi, Ling Yun
Fujian Provincial Key Laboratory of Modern Analytical Science and Separation Technology, Fujian Provincial Key Laboratory of Pollution Monitoring and Control, College of Chemistry, Chemical Engineering and Environment, Minnan Normal University, 363000, Zhangzhou, P. R. China.
College of Chemistry, Fuzhou University, 350116, Fuzhou, P. R. China.
ChemSusChem. 2022 Nov 8;15(21):e202200919. doi: 10.1002/cssc.202200919. Epub 2022 Aug 23.
Nitrogen reduction electrocatalysts are highly attractive for catalytic science. However, most electrocatalysts are limited by their low faradaic efficiency, poor ammonia yield, and tedious and costly catalyst synthesis process. In this work, Fe-based oxide composite nanoparticles with steady chemical states are prepared by a single-step green procedure under ambient conditions. The resulting Fe-Fe O demonstrates remarkable activity and selectivity for nitrogen reduction reaction (NRR) with the highest faradaic efficiency of 53.2±1.8 % and NH yield rate of 24.6±0.8 μg h mg at -0.4 V (vs. RHE) in 0.1 m Na SO electrolyte. Characterization experiments and theoretical calculation reveal that Fe-Fe O exhibits significantly enhanced charge transfer capability and suppresses the competitive HER process.
氮还原电催化剂对催化科学极具吸引力。然而，大多数电催化剂受到其低法拉第效率、低氨产率以及繁琐且昂贵的催化剂合成过程的限制。在这项工作中，通过在环境条件下的一步绿色程序制备了具有稳定化学状态的铁基氧化物复合纳米颗粒。所得的Fe-Fe₂O₃在0.1 m Na₂SO₄电解质中，在-0.4 V（相对于可逆氢电极）下对氮还原反应（NRR）表现出显著的活性和选择性，最高法拉第效率为53.2±1.8 %，NH₃产率为24.6±0.8 μg h⁻¹ mg⁻¹。表征实验和理论计算表明，Fe-Fe₂O₃表现出显著增强的电荷转移能力，并抑制了竞争性析氢反应过程。
