Reductive modification of electrolytic manganese residue unlocks multifunctional active sites for enhanced peroxymonosulfate activation and aniline aerofloat removal

IF 7.8 2区环境科学与生态学 Q1 ENGINEERING, CHEMICAL

Process Safety and Environmental Protection Pub Date : 2025-09-05 DOI:10.1016/j.psep.2025.107839

Jieyi Wang , Mengke Li , Chenquan Ni , Yuting Liang , Zhiguo He

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引用次数: 0

Abstract

The preparation of catalysts for peroxymonosulfate (PMS) activation usually entails substantial costs and intricate steps. In this study, a novel catalyst (2FA-EMR) was successfully obtained from electrolytic manganese residue (EMR) through reduction modification. 2FA-EMR exhibited a loose and porous surface morphology, removing 95.88 % aniline aerofloat (AAF, 100 mg/L) within 120 min. The reaction rate constant (k_o_bs) of 2FA-EMR reached 17.5 times that of unmodified EMR. Mechanism analysis revealed that oxygen vacancies (O_V) and low-velent Fe/Mn in diverse Fe and Mn phases were the key active sites for AAF degradation. The synergistic effect among them enhanced the electron transfer efficiency between 2FA-EMR and PMS, thereby promoting the generation of reactive oxygen species (ROS). ¹O₂ was identified as the dominant ROS responsible for AAF degradation in the 2FA-EMR/PMS system, originating from the conversion of Ov and O₂^•− and preferentially attacking the P-N bond of AAF. Additionally, the mild and continuous reaction process achieved a mineralization degree of over 75 %. The study furnished a meaningful reference for the development of cost-effective and easy-to-prepare catalysts for PMS activation.

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电解锰渣的还原改性解锁了多功能活性位点，增强了过氧单硫酸盐活化和苯胺的去除

制备过氧单硫酸盐（PMS）活化催化剂通常需要大量的成本和复杂的步骤。本研究以电解锰渣（EMR）为原料，通过还原改性制备了一种新型催化剂（2FA-EMR）。2FA-EMR表现出松散多孔的表面形貌，在120 min内去除95.88 %苯胺浮粒（AAF, 100 mg/L）。2FA-EMR的反应速率常数（kobs）达到未改性EMR的17.5倍。机理分析表明，不同Fe和Mn相中的氧空位（OV）和低电位Fe/Mn是AAF降解的关键活性位点。它们之间的协同作用提高了2FA-EMR和PMS之间的电子传递效率，从而促进活性氧（ROS）的生成。在2FA-EMR/PMS系统中，O2被认为是主要的降解AAF的活性氧，起源于Ov和O2•−的转化，并优先攻击AAF的P-N键。反应过程温和连续，矿化度达75% %以上。该研究为开发成本低、制备简单的PMS活化催化剂提供了有意义的参考。

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来源期刊

Process Safety and Environmental Protection 环境科学-工程：化工

CiteScore

11.40

自引率

15.40%

发文量

929

审稿时长

8.0 months

期刊介绍： The Process Safety and Environmental Protection (PSEP) journal is a leading international publication that focuses on the publication of high-quality, original research papers in the field of engineering, specifically those related to the safety of industrial processes and environmental protection. The journal encourages submissions that present new developments in safety and environmental aspects, particularly those that show how research findings can be applied in process engineering design and practice. PSEP is particularly interested in research that brings fresh perspectives to established engineering principles, identifies unsolved problems, or suggests directions for future research. The journal also values contributions that push the boundaries of traditional engineering and welcomes multidisciplinary papers. PSEP's articles are abstracted and indexed by a range of databases and services, which helps to ensure that the journal's research is accessible and recognized in the academic and professional communities. These databases include ANTE, Chemical Abstracts, Chemical Hazards in Industry, Current Contents, Elsevier Engineering Information database, Pascal Francis, Web of Science, Scopus, Engineering Information Database EnCompass LIT (Elsevier), and INSPEC. This wide coverage facilitates the dissemination of the journal's content to a global audience interested in process safety and environmental engineering.