数字农科院2.0

Mechanically treated natural mineral-modified biochar for triggering peroxymonosulfate oxidation of micropollutants: Unveiling the critical role of non-radical pathways and vacancy-mediated electron transfer

文献类型： 外文期刊

作者： Huanhuan Wang;Geng Chen;Quanbin Zhang;Zhenhua Wang;Bo Fu;Huifu Ji;Yifan Liu;Yunjie Wu;Jingshang Xiao;Binqiang Tian

作者机构：

关键词： Activation;Ball-mill;Pyrite;Sulfur vacancy

期刊名称： Chemical Engineering Journal

ISSN： 1385-8947

年卷期： 2025 年 520 卷

页码：

收录情况： SCIE（2025版） ; ; EI（2025版）

摘要： Pyrite (FeS2) is a green and natural mineral with inherent catalytic potential; however, its cluster effect hinders sustained catalysis. In this study, highly dispersed FeS2 anchored on tobacco straw biochar (FeS2@TSBC) was prepared via a mechanically treated and used for peroxymonosulfate (PMS) activation to degrade sulfonamides (SAs). The characterizations demonstrated that mechanical energy successfully dispersed FeS2 nanoparticles on TSBC surface, effectively suppressing particle agglomeration and surface passivation. The FeS2@TSBC/PMS system achieved 93.84 % SMX degradation within 30 min under optimized conditions. In addition, this system showed anti-interference ability and strong pH tolerance (3.0–11.0) with less efficiency variation. However, the removal efficiency of the system was worsened in presence of HCO₃− and CO₃2−, as these ions elevated the pH of reaction system. Experiments and calculations showed that PMS adsorbed onto FeS2@TSBC, which then decomposed to generate SO4•−, •OH, O2•− and 1O2 via O[sbnd]O bond cleavage. Meanwhile, the reductive sulfur species in FeS2@TSBC facilitated Fe (III)/Fe (II) cycling. The variable valence states of Fe sites could enhance the multi-electron transfer pathways in system, driving the formation of high-valent iron species (Fe (IV)/Fe (V)). Among these reactive species, 1O2 was identified as a major contributor to SMX removal in FeS2@TSBC/PMS system, and its cumulative concentration was 84.11 μM. The electron-rich sulfur vacancies (SVs) acted as catalytic sites, driving oxygen activation and subsequent 1O2 generation through vacancy-mediated electron transfer. Finally, FeS2@TSBC/PMS system showed excellent reusability and stability after cycles and sustainable degradation. DFT calculations showed that non-radical pathways mainly attacked the amine group sulfonamide bond, causing less toxic products or mineralization. This study provides valuable insights into developing stable natural mineral-modified biochar, broadening its potential applications in wastewater antibiotic treatment.

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