青岛科技大学张永超团队报道了缺硒FeSe₂/F₃O₄电催化剂还原硝酸盐制氨研究。相关研究成果发表在2024年12月24日出版的《德国应用化学》。

NO₃^-的电催化还原是一种绿色可持续的方法，不仅有助于处理废水中的工业污染物，而且可以生产有价值的化学品。然而，质子耦合电子转移过程的缓慢动力学，导致高势垒和低转换效率。

该文中，研究人员合成了缺硒FeSe₂/F₃O₄异质结，该异质结在0.1 M硝酸盐还原反应中表现出优异的电化学性能，优于目前报道的大多数催化剂。缺硒FeSe₂/F₃O₄的高活性是由于FeSe₂和Fe₃O₄之间的协同作用，实现了NO₃^-的中继催化还原。

其中，缺硒FeSe₂有助于NO₃^-脱氧和随后的氢化，Fe₃O₄促进H₂O分解提供H质子，共同促进NO₃RR。最后，在线微分电化学质谱（DEMS）、原位拉曼和DFT计算，证实了缺硒FeSe₂/F₃O₄（100）上NO₃RR转化为NH₃的最佳途径。

该中继催化策略为处理高浓度硝酸盐废水，提供了一种潜在的方法。

附：英文原文

Title: Selenium-Deficient FeSe2/Fe3O4 Electrocatalyst for Nitrate Reduction to Ammonia

Author: Yue Du, Haijiao Lu, Jinting Wu, Yalong Zou, Zhen-Feng Huang, Ji-Jun Zou, Tiansheng Mu, Jian Gao, Xiao-Dong Zhu, Yong-Chao Zhang

Issue&Volume: 2024-12-24

Abstract: Electrocatalytic reduction of NO3- is a green and sustainable method that not only helps to treat industrial pollutants in wastewater, but also produces valuable chemicals. However, the slow dynamics of the proton-coupled electron transfer process results in a high barrier and low conversion efficiency. In this work, the Se-deficient FeSe2/Fe3O4 heterojunction was synthesized, which showed excellent electrochemical performance in 0.1 M nitrate reduction reaction, superior to most currently reported catalysts. The high activity of Se-deficient FeSe2/Fe3O4 is due to the synergistic effect between FeSe2 and Fe3O4 to achieve relay catalytic NO3- reduction. Among them, the Se-deficient FeSe2 contributes to NO3- deoxygenation and subsequent hydrogenation, and Fe3O4 promotes H2O decomposition to provide H proton, jointly promote NO3RR. Finally, the online differential electrochemical mass spectra (DEMS), in-situ Raman and DFT calculation confirmed the optimal pathway for NO3RR to NH3 on Se-deficient FeSe2/Fe3O4(100). This strategy of relay catalysis provides a potential way to treat wastewater with high concentration nitrate.

DOI: 10.1002/anie.202420903

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202420903