Lei Fengcai, Wang Ying, Hou Yuhan, Huai Ruixue, Zhang Menghan, Xie Junfeng, Hao Pin, Song Yuzhi, Yu Jing
College of Chemistry, Chemical Engineering and Materials Science, Key Laboratory of Molecular and Nano Probes (Ministry of Education), Collaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of Shandong, Institute of Molecular and Nano Science, Shandong Normal University, Jinan, Shandong 250014, PR China.
College of Chemistry, Chemical Engineering and Materials Science, Key Laboratory of Molecular and Nano Probes (Ministry of Education), Collaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of Shandong, Institute of Molecular and Nano Science, Shandong Normal University, Jinan, Shandong 250014, PR China.
J Colloid Interface Sci. 2025 Dec 15;700(Pt 1):138378. doi: 10.1016/j.jcis.2025.138378. Epub 2025 Jul 8.
The development of efficient catalysts for nitrate reduction to ammonia is crucial for sustainable nitrogen cycle management. In this study, we introduce an amorphous multimetal borides (CoFeNiB) catalyst that demonstrates exceptional performance in the electrochemical reduction of nitrate to ammonia. X-ray photoelectron spectroscopy (XPS) and in-situ Raman spectroscopy reveal that the catalyst exhibits a unique surface reconstruction during the reaction, leading to the formation of CoOOH, where Co ions can serve as active sites, significantly enhancing the adsorption of nitrate ions and atomic hydrogen, thereby promoting the reduction reaction. Specially, besides the activity enhancement of CoFeNiB compared with CoFeB and CoB, the stability of it can be markedly improved by the synergistic effect of Ni and Fe in the catalyst. Consequently, the CoFeNiB catalyst achieves a stable Faradaic efficiency above 90 % across a broad voltage range of 0 ∼ -0.6 V vs reversible hydrogen electrode (RHE) and an ammonia yield peaked of 3961.4 mmol g h at -0.6 V vs RHE. The CoFeNiB catalyst offers a promising avenue for the efficient and stable synthesis of ammonia from nitrate, addressing key challenges in environmental sustainability and nitrogen management.
开发用于将硝酸盐还原为氨的高效催化剂对于可持续氮循环管理至关重要。在本研究中，我们引入了一种非晶态多金属硼化物（CoFeNiB）催化剂，该催化剂在将硝酸盐电化学还原为氨的过程中表现出卓越的性能。X射线光电子能谱（XPS）和原位拉曼光谱表明，该催化剂在反应过程中呈现独特的表面重构，导致形成CoOOH，其中Co离子可作为活性位点，显著增强硝酸根离子和原子氢的吸附，从而促进还原反应。特别地，除了与CoFeB和CoB相比CoFeNiB的活性增强外，催化剂中Ni和Fe的协同作用可显著提高其稳定性。因此，CoFeNiB催化剂在相对于可逆氢电极（RHE）为0 ∼ -0.6 V的宽电压范围内实现了高于90%的稳定法拉第效率，并且在相对于RHE为-0.6 V时氨产率峰值达到3961.4 mmol g⁻¹ h⁻¹。CoFeNiB催化剂为从硝酸盐高效稳定合成氨提供了一条有前景的途径，解决了环境可持续性和氮管理方面的关键挑战。
