College of Environmental Science and Engineering, Nankai University, No. 38, Tongyan Road, Jinnan District, Tianjin 300350, China.
Graduate School of Environmental Studies, Tohoku University, Aramaki Aza Aoba 6-6-11, Aoba-ku, Sendai 980-8579, Japan.
Sci Total Environ. 2022 Aug 25;836:155640. doi: 10.1016/j.scitotenv.2022.155640. Epub 2022 May 2.
In electrocatalytic reduction of nitrates to nitrogen, key issues are electrode activity, sustainable materials, preparation methods and cost. Herein, lignin, Fe ion, and non-ionic surfactant were combined with evaporation-induced self-assembly (EISA) to prepare zero-valent Fe-dispersed ordered mesoporous carbon (OMC) electrode materials denoted as Fe#OMC. The method developed for preparing Fe-coordinated OMC material avoids the use of toxic phenols, aldehyde reagents and metal doping compounds. When synthesized Fe#OMC samples were applied as electrode materials for the electrocatalytic reduction of nitrate in aqueous solutions, maximum nitrate nitrogen removal was as high as 5373 mg N·g Fe from aqueous solutions containing 400 mg·L NO-N, while nitrogen selectivity was close to 100%, exceeding catalytic performance of comparable materials. Active hydrogen produced by electrolysis of water during the reaction re-reduced Fe ions formed in the OMC material and stabilized Fe#OMC electrode performance and recycle. The Fe#OMC electrode is self-renewing with respect to its Fe zero-valent state, is simple to prepare from sustainable materials and is effective for electrocatalytic reduction of nitrate or nitrogen-containing compounds in water.
在硝酸盐电催化还原为氮气的过程中,关键问题是电极活性、可持续材料、制备方法和成本。本文将木质素、Fe 离子和非离子表面活性剂与蒸发诱导自组装(EISA)相结合,制备了零价 Fe 分散的有序介孔碳(OMC)电极材料,记为 Fe#OMC。所开发的用于制备 Fe 配位 OMC 材料的方法避免了使用有毒的酚类、醛试剂和金属掺杂化合物。当合成的 Fe#OMC 样品用作水溶液中硝酸盐电催化还原的电极材料时,从含有 400 mg·L 的 NO-N 的水溶液中,最大硝酸盐氮去除率高达 5373 mg N·g Fe,而氮的选择性接近 100%,超过了可比材料的催化性能。反应过程中水电解产生的活性氢将 OMC 材料中形成的 Fe 离子重新还原,并稳定了 Fe#OMC 电极的性能和循环使用。Fe#OMC 电极的 Fe 零价状态可以自我更新,且其制备方法简单,可有效用于水中硝酸盐或含氮化合物的电催化还原。