Active surface area determines the activity of biochar in Fenton-like oxidation processes

IF 11.3 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL
Ziqian Wang, Chunyu Du, Shengjiong Yang, Xiaoping Li, Rongzhi Chen, Dahu Ding
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Abstract

Biochar (BC) possesses diverse active sites (e.g., oxygen-containing groups OCGs, defects, and electronegative heteroatom) responsible for the catalytic reactions. As an ordinary indicator, specific surface area (SSA) can not accurately reflect the activity of biochar. Herein, we proposed active surface area (ASA), which referred to the surface containing active sites to characterize the activity of biochar in advanced oxidation processes (AOPs). We developed a simple and non-destructive etching method to realize the regulation of OCGs and SSA in silicon-abundant biochar. Intriguingly, peroxydisulfate (PDS) activation was improved whilst periodate (PI) activation was inhibited in HFBC-AOPs. Mechanistic study and theoretical calculations revealed that the electron-transfer between tetracycline (TC) and metastable high-potential complexes BC-PDS⁎ dominated the TC oxidation in HFBC-PDS system. Meanwhile, the oxidation of TC was driven by the singlet oxygen (1O2) in PI system, where the surface –OH played a crucial role. The depletion of surface −OH well explained the inhibited TC oxidation in HFBC-PI system though the SSA was increased. Eventually, the established BC-AOPs performed excellent adaptability in complex scenarios and low eco-environmental risks through multi-level toxicity analysis. Overall, this study systematically scrutinized the critical role of ASA in BC-AOPs and enlightened the rational design of biochar for wastewater treatment.

Abstract Image

活性表面积决定了生物炭在类芬顿氧化过程中的活性
生物炭(BC)具有多种催化反应的活性位点(如含氧基团OCGs、缺陷和电负性杂原子)。比表面积(SSA)作为一种常用的指标,并不能准确反映生物炭的活性。在此,我们提出了活性表面积(ASA),它是指含有活性位点的表面,用于表征生物炭在高级氧化过程(AOPs)中的活性。我们开发了一种简单且无损的蚀刻方法来实现富硅生物炭中OCGs和SSA的调控。有趣的是,在HFBC-AOPs中,过氧二硫酸盐(PDS)活化得到改善,而高碘酸盐(PI)活化受到抑制。机制研究和理论计算表明,在HFBC-PDS体系中,四环素(TC)和亚稳高电位配合物BC-PDS之间的电子转移主导了TC氧化过程。同时,在PI体系中,TC的氧化是由单线态氧(1O2)驱动的,其中表面-OH起着至关重要的作用。表面- OH的耗尽很好地解释了hbc - pi体系中TC氧化被抑制的原因,尽管SSA增加了。最终,通过多级毒性分析,所建立的BC-AOPs对复杂场景具有良好的适应性,生态环境风险低。总的来说,本研究系统地探讨了ASA在BC-AOPs中的关键作用,并为废水处理生物炭的合理设计提供了启示。
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来源期刊
Journal of Hazardous Materials
Journal of Hazardous Materials 工程技术-工程:环境
CiteScore
25.40
自引率
5.90%
发文量
3059
审稿时长
58 days
期刊介绍: The Journal of Hazardous Materials serves as a global platform for promoting cutting-edge research in the field of Environmental Science and Engineering. Our publication features a wide range of articles, including full-length research papers, review articles, and perspectives, with the aim of enhancing our understanding of the dangers and risks associated with various materials concerning public health and the environment. It is important to note that the term "environmental contaminants" refers specifically to substances that pose hazardous effects through contamination, while excluding those that do not have such impacts on the environment or human health. Moreover, we emphasize the distinction between wastes and hazardous materials in order to provide further clarity on the scope of the journal. We have a keen interest in exploring specific compounds and microbial agents that have adverse effects on the environment.
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