Study on the performance and mechanism of MnFe2O4@hydrothermal carbon activated persulfate for tetracycline degradation

doi:10.19965/j.cnki.iwt.2025-0048

Abstract

Abstract:

The catalyst of manganese ferrite loaded on corn stover powder hydrochar was synthesized through a one-step hydrothermal treatment method, and then activated peroxydisulfate(PDS) to degrade tetracycline hydrochloride(TC).The catalyst was characterized by SEM, XRD, FTIR and XPS to analyze the composition and properties of the catalyst. The reaction parameters were determined by batch tests. After repetitive experiments and metal ion precipitation experiments, the repetitive utilization performance and stability of the catalyst were studied. Active species in the reaction process were analyzed by quenching texts, and the degradation pathways were studied by LC-MS. The results showed that when the TC was 25 mg/L, the catalyst dosage was 0.3 g/L, and the PDS was 4 mmol/L, the TC degradation rate could reach 85% after 90 min of reaction. The solution had a high degradation rate at initial pH range of 3-9. The reaction rate and degradation rate increased with increasing temperature. Additionally, CO₃ ^2-, HCO₃ ^- and H₂PO₄ ^- all had strong inhibitory effect on the catalytic reaction, while Cl^-, SO₄ ^2- and HA had slight inhibitory effect, and NO₃ ^- had a weak promoting effect. It was also found that SO₄ ^·-, ·OH, ¹O₂ and O₂ ^·- all played roles, among which ¹O₂ was the main active species in the reaction system. The degradation paths mainly included demethylation, deamidation and hydroxylation.

Key words: hydrothermal carbon supported manganese ferrite, persulfate, tetracycline hydrochloride, catalytic oxidation

摘要：

利用一步水热法制备玉米秸秆粉水热炭负载铁酸锰催化剂，活化过二硫酸盐（PDS）去除四环素（TC），采用SEM、XRD、FTIR、XPS对催化剂进行表征以分析催化剂的成分与性质。通过批次实验确定反应参数，经过重复性实验和金属离子析出实验研究催化剂的重复利用性能和稳定性能，通过猝灭实验分析反应过程中的活性物种，结合LC-MS测试研究降解路径。结果表明，当TC为25 mg/L，催化剂投加量为0.3 g/L，PDS为4 mmol/L时，经反应90 min，TC降解率可达到85%，溶液初始pH在3~9均具有较高的降解率，反应速率、降解率随着温度的升高而升高，CO₃ ^2-、HCO₃ ^-、H₂PO₄ ^-对催化反应均有较强的抑制作用，Cl^-、SO₄ ^2-、腐殖酸（HA）有轻微的抑制作用，NO₃ ^-有微弱的促进作用。反应体系中SO₄ ^·-、·OH、¹O₂、O₂ ^·-均起到作用，其中¹O₂为主要活性物种，降解路径主要有去甲基、脱酰胺、羟基化等。

关键词: 水热炭负载铁酸锰, 过硫酸盐, 四环素, 催化氧化

CLC Number:

X703.1

Yixing ZHANG, Yun LI, Huixiang HU. Study on the performance and mechanism of MnFe₂O₄@hydrothermal carbon activated persulfate for tetracycline degradation[J]. Industrial Water Treatment, 2025, 45(12): 88-99.

张一星, 李芸, 胡慧翔. MnFe₂O₄@水热炭活化过硫酸盐降解四环素的性能与机理研究[J]. 工业水处理, 2025, 45(12): 88-99.

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URL: https://www.iwt.cn/EN/10.19965/j.cnki.iwt.2025-0048

https://www.iwt.cn/EN/Y2025/V45/I12/88

Figures/Tables 15

Fig.1 Effects of tetracycline removal by different metal ratio materials（a） and manganese ion precipitation during the reaction（b）

Fig.2 Catalytic（a） and adsorption（b） performance of materials with different m（MF）∶m（HTC） ratios

Fig.3 SEM images of catalyst materials

Fig.4 XRD pattern of catalyst materials

Fig.5 FTIR spectrum of catalyst materials

Fig.6 XPS fine spectrum of catalyst materials

Fig.7 Effects of different systems on catalytic reactions

Fig.8 Effects of different PDS concentrations（a） and the dosage of MF@HTC （b）on the catalytic reaction

Fig.9 Effects of different TC concentrations（a）， initial pH（b），reaction temperatures（c），anions and HA（d） on catalytic reactions

Fig.10 Mn precipitation in the reaction process

Fig.11 Contribution of manganese ions precipitated in the reaction system

Fig.12 Reusability of MF@HTC

Fig.13 Free radical quenching experiment

Fig.14 Schematic diagram of activation mechanism in the reaction system

Fig.15 TC degradation paths

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Study on the performance and mechanism of MnFe₂O₄@hydrothermal carbon activated persulfate for tetracycline degradation

MnFe₂O₄@水热炭活化过硫酸盐降解四环素的性能与机理研究

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