Insight into the mechanism of peracetic acid activation by corn straw-derived biochar as efficient green activator mediating electron transfer: Crucial role of carbonyl functional group

IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Linjie Li , Jiale Zhao , Xiaodan Zhao , Zuoming Zhou , Guohua Jing
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Abstract

Efficient and economical activator for enhancing peracetic acid (PAA) to generate reactive species is greatly critical for elevating the removal efficiency of the recalcitrant organic compounds in the water and wastewater treatment. Corn straw-derived biochar (CBC) is prepared by pyrolysis method with ample oxygen-containing functional group and defective structures working as an efficient electron transfer medium, which can promote PAA activation for the tetracycline (TC) degradation. In the CBC/PAA system, the TC degradation rate can reach 97.7 % within 30 min of reaction. The high performance of the CBC/PAA system is mainly attributed to the combined process of the free radical and the non-free radical pathway. According to the electrochemical experiments and density functional theory (DFT) calculation, carbonyl functional group (C=O) plays a crucial role for PAA activation. The electron-rich group C=O can not only transfer electrons from carbon networks and TC to PAA, but also provide electrons to directly activate PAA due to the presence of lone pair electrons. Moreover, the TC degradation pathways guided by radical and non-radical mechanisms are elucidated, and the toxicity changes of intermediate products are evaluated. In this study, a low-cost and efficient process combining PAA and biochar based on electron transfer mechanisms is proposed, guaranteeing the rapid TC degradation.

Abstract Image

玉米秸秆生物炭作为介导电子传递的高效绿色活化剂对过氧乙酸活化机理的深入研究:羰基官能团的关键作用
高效、经济的活化剂可促进过乙酸(PAA)生成活性物种,这对于提高水和废水处理中难降解有机化合物的去除效率至关重要。玉米秸秆衍生生物炭(CBC)是通过热解方法制备的,具有丰富的含氧官能团和缺陷结构,可作为高效的电子传递介质,促进过乙酸(PAA)的活化,从而降解四环素(TC)。在 CBC/PAA 系统中,反应 30 分钟内 TC 降解率可达 97.7%。CBC/PAA 系统的高性能主要归功于自由基和非自由基途径的结合过程。根据电化学实验和密度泛函理论(DFT)计算,羰基官能团(C=O)对 PAA 的活化起着至关重要的作用。富电子基团 C=O 不仅能将电子从碳网络和 TC 转移到 PAA,而且由于存在孤对电子,还能提供电子直接活化 PAA。此外,还阐明了自由基和非自由基机制引导的 TC 降解途径,并评估了中间产物的毒性变化。本研究提出了一种基于电子传递机制的低成本、高效率的 PAA 与生物炭结合工艺,保证了 TC 的快速降解。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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