Enhanced retention of arsenite and arsenate through heterogeneous interactions between Fe(III) (Hydr)Oxides and black carbon: a multi-mechanistic study

文献类型： 外文期刊

第一作者： Li, Bingyu

作者： Li, Bingyu;Liu, Saihua;Xie, Yunhe;Ji, Xionghui;Li, Bingyu;Liu, Saihua;Xie, Yunhe;Ji, Xionghui;Li, Bingyu;Liu, Saihua;Xie, Yunhe;Ji, Xionghui;Li, Bingyu;Jing, Miaomiao;Li, Jingru;Li, Zhuoqing;Zhou, Yimin;Lei, Ming;Cui, Haojie;Wei, Dongning

作者机构：

关键词： Black carbon; Ferrihydrite; Pore diffusion; Free radical; Arsenic; Sorption

期刊名称：CHEMICAL ENGINEERING JOURNAL （ 影响因子：13.2； 五年影响因子：13.5 ）

ISSN： 1385-8947

年卷期： 2025 年 515 卷

页码：

收录情况： SCI

摘要： Amorphous Fe(III) (hydr)oxides ubiquitously interact with organic matter, forming organic-inorganic assemblages in natural environments. Yet, how their hetero-aggregation with pyrogenic organic matter influences coexisting pollutants remains unclear. Herein, we simulated two associations of rice straw-derived black carbon (RBC) with Fe(III) oxide, by employing different formation scenarios (sorption and coprecipitation) across various Fe/C ratios. Batch experiments and microscopic characterization techniques (e.g. XRD, XPS, FTIR, BET) were used to evaluate the effects of hetero-aggregation between RBC and Fe(III) oxides on the fate of the co-presence of As(III) and As(V). We showed that iron minerals and RBC mainly through-COOH and Si-O bonds formed different Fe/C associations, and RBC greatly modified the surface properties of iron minerals (e.g. zeta potential, pore structure). Batch experiments demonstrated that RBC significantly improved the retention of As (III) and As(V) on iron minerals, with a pronounced effect on As(V). Our multi-mechanistic study, utilizing non-local density functional theory, radical quenching, and electrostatic interactions, demonstrated that the heteroaggregation of RBC/Fe(III) oxides resulted in the formation of more characteristic pores across various mineral systems, significantly enhancing the pore diffusion of As(III) and As(V) within the bulk mineral matrix. We identified distinct electrostatic interactions between As(III)/As(V) and various mineral end-members, with As(V) promoting the aggregation of iron oxides and decreasing pore width, whereas As(III) exhibited minimal impact on the pore structures of iron oxides. Interestingly, RBC enhanced the resistibility of the pore structure against negative potential, thereby facilitating the extensive diffusion of As(III) and As(V). Furthermore, we identified that RBC-mediated radical reaction also contributed to the immobilization of As(III). Our findings help better understand how arsenic behaves under black carbon-rich geological settings where iron-carbon coupled reactions prevail.

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