Activation of H2O2 by carbonaceous iron sludge-derived catalyst for methylene blue wastewater treatment

doi:10.19965/j.cnki.iwt.2023-0044

Abstract

Abstract:

Resource utilization of waste iron sludge from wastewater treatment plants can be achieved by leveraging iron sludge-based catalysts to construct Fenton-like systems. Notably，the pyrolysis temperature modulates the composition of metal and non-metal sites on the catalyst surface，thus affecting the activation of hydrogen peroxide（H₂O₂）. The catalysts prepared at different pyrolysis temperatures（400-700 ℃） were analyzed in terms of morphology，composition，structure and activity. It was found that the degradation efficiency of methylene blue（MB） could reach 92.0% within 100 min with the activation of H₂O₂ by the catalyst obtained at 700 °C. Additionally，the specific surface area and C content of the catalyst increased as the pyrolysis temperature increased from 400 ℃ to 700 ℃. The mechanistic investigation revealed that Fe⁰，C $̿$ C/C—C and C $̿$ O active sites on the catalyst surface were critical for the activation of H₂O₂，which facilitated MB degradation. Moreover，hydroxyl radicals（·OH） and singlet oxygen（¹O₂） were the dominant active species in the iron sludge-derived catalyst/H₂O₂ system，with superoxide radicals（O₂ ^·-） playing a minor role.

Key words: waste iron sludge, Fenton-like, dye wastewater

摘要：

利用铁泥基催化剂构建类Fenton体系可实现污水厂废弃铁泥的资源化利用。热解温度可调控催化剂表面金属和非金属位点组成，影响其对过氧化氢（H₂O₂）的活化效果。对不同热解温度（400~700 ℃）下制备的催化剂进行形貌、组成、结构和活性等方面的测试。研究发现，700 ℃下制备的催化剂活化H₂O₂，在100 min内对亚甲基蓝（MB）降解率达92.0%。当热解温度在400~700 ℃范围内增大时，催化剂比表面积和C含量均增大。机理探究表明，催化剂表面的Fe⁰、C $̿$ C/C—C和C $̿$ O活性位点对活化H₂O₂发挥重要作用，有利于促进亚甲基蓝降解。此外，铁泥基催化剂/H₂O₂体系中羟基自由基（·OH）和单线态氧（¹O₂）是主要活性物种，超氧自由基（O₂ ^·-）发挥作用较小。

关键词: 废弃铁泥, 类Fenton, 染料废水

CLC Number:

TQ426
X703.5

Lia WANG, Shuang WU, Xiaoshuang CHENG, Lan LIANG, Ning LI, Guanyi CHEN, Li’an HOU. Activation of H₂O₂ by carbonaceous iron sludge-derived catalyst for methylene blue wastewater treatment[J]. Industrial Water Treatment, 2024, 44(2): 125-132.

王俩, 吴霜, 程小双, 梁澜, 李宁, 陈冠益, 侯立安. 含碳铁泥基催化剂活化H₂O₂处理亚甲基蓝废水[J]. 工业水处理, 2024, 44(2): 125-132.

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URL: https://www.iwt.cn/EN/10.19965/j.cnki.iwt.2023-0044

https://www.iwt.cn/EN/Y2024/V44/I2/125

Figures/Tables 8

Fig.1 XRD patterns of iron sludge-derived catalysts under different heating temperatures

Table 1 The specific surface area and pore characteristics of iron sludge-derived catalysts under different heating temperatures

样品名称	比表面积/ （m²·g^-1）	平均孔径/nm	总孔体积/（cm³·g^-1）
Cat-400	49.94	57.36	0.14
Cat-500	48.48	61.73	0.15
Cat-600	55.76	54.06	0.15
Cat-700	83.87	33.78	0.14

Fig.2 SEM images of Cat-400（a），Cat-500（b），Cat-600（c）and Cat-700（d）

Fig.3 XPS spectra of Cat-400，Cat-500，Cat-600 and Cat-700

Fig.4 The content of active sites of Cat-400，Cat-500，Cat-600 and Cat-700

Fig.5 MB degradation （a） and degradation kinetics （b） under different heating temperatures，MB degradation under different H₂O₂（c） and Cat-700 dosage （d）

Fig.6 MB degradation（a） and degradation kinetics（b） with different quenchers；EPR spectra of DMPO-·OH，DMPO-O₂ ^·- and TEMP-¹O₂ in Cat-700/H₂O₂ system（c）

Table 2 The correlation coefficients between MB degradation and active sites on iron sludge-derived catalyst surface under different heating temperatures

活性位点	MB降解
C $̿$ C/C—C	+0.95
C $̿$ O	+0.50
Fe⁰	+0.91

Table 2 The correlation coefficients between MB degradation and active sites on iron sludge-derived catalyst surface under different heating temperatures

活性位点	MB降解
C $̿$ C/C—C	+0.95
C $̿$ O	+0.50
Fe⁰	+0.91

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Activation of H₂O₂ by carbonaceous iron sludge-derived catalyst for methylene blue wastewater treatment

含碳铁泥基催化剂活化H₂O₂处理亚甲基蓝废水

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