文献类型：期刊文献

英文题名：Chloride activation driven by Mn3O4-activated peracetic acid enables selective ammonia-to-nitrogen conversion at ambient conditions

作者：Zhao, Tao[1];Ma, Lijuan[1];Zhang, Pengkang[1];Liu, Changbo[1];Zhao, Jiuli[1];Zhang, Meixue[1];Yang, Shenglong[1];Chen, Xiurong[1,2]

机构：[1]East China Univ Sci & Technol, Key Lab Environm Risk Assessment & Control Chem Pr, Minist Ecol & Environm, Shanghai 200237, Peoples R China;[2]Shihezi Univ, Sch Chem & Chem Engn, Key Lab Environm Monitoring & Pollutant Control Xi, Shihezi 832003, Xinjiang, Peoples R China

年份：2026

卷号：14

期号：3

外文期刊名：JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING

收录：;EI(收录号：20262821098221);Scopus(收录号：2-s2.0-105044401655);WOS:【SCI-EXPANDED(收录号:WOS:001758819800001)】；

基金：The authors are incredibly grateful to the National Key Technology and Development Program of Corps (2025AA001) for financial support.

语种：英文

外文关键词：Ammonia; Peracetic acid; Manganese oxide; Chloride ion activation; Hypochlorous acid; Aerosol spraying

摘要：A ternary manganese oxide (Mn3O4)/peracetic acid (PAA)/chloride (Cl-) catalytic oxidation system was developed for efficient ammonia (NH3) abatement under ambient conditions, with low byproduct formation and high N-2 selectivity. Micro-/nano-aerosol spraying was integrated with in situ catalytic oxidation at near-neutral pH. Mn3O4 served as a low-cost heterogeneous catalyst, PAA as the oxidant, and Cl-, commonly regarded as a radical scavenger, as an activatable catalytic substrate. PAA activation was driven by Mn(II)/Mn(III)/Mn(IV) redox cycling, establishing a hybrid oxidative environment dominated by hypochlorous acid (HOCl), with radicals as secondary contributors. In aqueous solution, 96.6% NH3 was removed within 30 min, with an apparent N-2 selectivity of 99.15% based on nitrogen mass-balance analysis. NO2-, NO3-, ClO2-, and ClO3- remained at low levels; NO2- was below the analytical limit of detection, and chlorine oxyanions remained below the corresponding analytical limits or regulatory thresholds. In the gas-phase reactor, 10-15 s of reagent spraying reduced the NH3 residual fraction to similar to 1% within 20 min, while total nitrogen did not accumulate in the recovery solution, indicating reaction-enhanced absorption coupled with rapid liquid-phase conversion. Mechanistic analyses suggested an HOCl-mediated chloramination-denitrogenation pathway promoted by oxygen vacancies and multivalent Mn species on Mn3O4. More than 90% removal efficiency was retained after five cycles, with Mn leaching below 0.5 mg/L. These results demonstrate a byproduct-controllable and potentially scalable strategy for near-field NH3 mitigation, with promising engineering and economic potential due to its ambient-condition operation, low-cost catalyst, and spray-based implementation.