改性生物炭活化过硫酸盐降解盐酸四环素

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Abstract Tetracycline hydrochloride (TC) degradation was investigated utilizing hydrogen peroxide modified magnetic biochar (H₂O₂modified biochar, HMB) as an activator of peroxydisulfate (PDS), with a focus on assessing the impact of initial pH on TC degradation kinetics. The underlying reaction mechanisms and degradation pathways of HMB-activated PDS for TC degradation were elucidated through a series of experimental techniques, including quenching tests, electron paramagnetic resonance (EPR) spectroscopy for identifying active species, X-ray photoelectron spectroscopy (XPS) analysis, density functional theory (DFT) calculations, and liquid-liquid mass spectrometry (LC-MS) detection. Hydrogen peroxide modification significantly enhanced TC removal, achieving a removal rate of 83.9% under the specified conditions of TC concentration (20mg/L), PDS concentration (1mmol/L), and HMB dosage (0.5g/L). This efficacy surpassed that of PDS alone or the unmodified biochar system, albeit exhibiting a decrease in removal efficiency with rising pH levels. Quenching tests and EPR analyses unveiled both radical and non-radical pathways contributing to TC degradation, the active species mainly includes: SO₄^.-、·OH、O₂^.-and ¹O₂. XPS analysis identified carbonyl (C=O) functionalities as the primary active sites responsible for TC degradation within the HMB/PDS system. Complementary DFT calculations were employed to quantitatively assess the contribution of C=O moieties to the HMB/PDS-mediated degradation process. Furthermore, LC-MS analyses coupled with DFT calculations delineated two distinct degradation pathways for TC, involving mechanisms such as deamidation, hydroxylation, demethylation, and dehydration ring opening.

Key words： tetracycline hydrochloride magnetic biochar oxidative modification density functional theory mechanism of reaction

Received: 20 March 2024

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X703

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	WANG Shi-sheng
	YANG Yu
	SHENG Guang-hong
	LIU Yi-yun
	LI Shen-bo

Cite this article:

WANG Shi-sheng,YANG Yu,SHENG Guang-hong等. Modified biochar activated persulfate for degradation of tetracycline[J]. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(11): 6122-6131.

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http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2024/V44/I11/6122

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