冷轧污泥制备Fe/C催化剂催化降解苯酚

doi:10.16085/j.issn.1000-6613.2024-1988

化工进展 ›› 2025, Vol. 44 ›› Issue (12): 7270-7280.DOI: 10.16085/j.issn.1000-6613.2024-1988

• 资源与环境化工 • 上一篇

冷轧污泥制备Fe/C催化剂催化降解苯酚

唐燕¹^,²^,³^,⁴(), 钟广宏¹^,²^,³^,⁴, 李曦同⁵, 高晓亚¹^,²^,³^,⁴, 朱文杰¹^,²^,³^,⁴(), 罗永明²^,³^,⁴

^1.昆明理工大学环境科学与工程学院，云南昆明 650500
^2.昆明理工大学挥发性有机物污染防治与资源化创新团队，云南昆明 650500
^3.云南省高校恶臭挥发性有机物控制重点实验室，云南昆明 650500
^4.云南省含硫精细化工重点实验室，云南昆明 650500
^5.云南师范大学能源与环境学院，云南昆明 650500

收稿日期:2024-12-05 修回日期:2025-03-11 出版日期:2025-12-25 发布日期:2026-01-06
通讯作者: 朱文杰
作者简介:唐燕（1996—），女，硕士研究生，研究方向为高级氧化降解水体有机污染物。E-mail：1725183997@qq.com。

Preparation of Fe/C catalyst from cold-rolled sludge for catalytic degradation of phenol

TANG Yan¹^,²^,³^,⁴(), ZHONG Guanghong¹^,²^,³^,⁴, LI Xitong⁵, GAO Xiaoya¹^,²^,³^,⁴, ZHU Wenjie¹^,²^,³^,⁴(), LUO Yongming²^,³^,⁴

^1.School of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, Yunnan, China
^2.Volatile organic compounds pollution prevention and recycling provincial innovation team in Kunming University of Science and Technology, Kunming 650500, Yunnan, China
^3.Key Laboratory of Odor Volatile Organic Compounds Control in Universities in Yunnan Province, Kunming 650500, Yunnan, China
^4.Key Laboratory of Yunnan Province for Synthesizing Sulfur-containing Fine Chemical, Kunming 650500, Yunnan, China
^5.School of Energy and Environment, Yunnan Normal University，Kunming 650500, Yunnan, China

Received:2024-12-05 Revised:2025-03-11 Online:2025-12-25 Published:2026-01-06
Contact: ZHU Wenjie

摘要/Abstract

摘要：

以冷轧污泥为原材料，采用氨水预处理-热解法制备得到系列Fe/C催化剂，通过X射线衍射、比表面积分析、傅里叶变换红外光谱、Raman光谱和扫描电子显微镜对催化剂的物理化学性质进行分析，探究不同热解温度下Fe/C催化剂活化过二硫酸盐对苯酚的降解性能，其中600℃下制备的Fe/C催化剂（NFC-600）30min可完全去除苯酚，苯酚的降解符合准一级动力学模型。当pH为3~10时，反应30min后苯酚降解率为81.4%~100%，60min后均达到100%。阐明了NFC-600的主要活性位点为C $̿$ O、缺陷和Fe₃O₄。揭示了降解路径，苯酚首先经过自由基反应或者电子转移生成酚类物质，继而被氧化为醌类，再经过开环反应和C $̿$ C键断裂生成小分子酸，最后矿化为H₂O和CO₂。实验结果表明，NFC-600具有良好的催化性能和优异的pH适用性，该研究为冷轧污泥资源化利用和酚类废水降解提供了有效路径。

关键词: 冷轧污泥, Fe/C催化剂, 苯酚, 过二硫酸盐, 资源化利用

Abstract:

A series of Fe/C catalysts were synthesized from cold-rolled sludge using an ammonia pretreatment-pyrolysis method. The physicochemical properties of these catalysts were characterized by X-ray diffraction, porosity measurement, Fourier transfrom infrared spectroscopy, Raman spectroscopy, and scanning electron microscope to evaluate their performance in degrading phenol via activated peroxodisulfate at different pyrolysis temperatures. The Fe/C catalyst prepared at 600℃ (NFC-600) demonstrated superior catalytic performance, achieving complete phenol removal within 30 minutes. The degradation kinetics of phenol followed a quasi-first-order model. The phenol degradation efficiencies ranged from 81.4%—100% after 30 minutes of reaction at pH between 3—10, with all samples reaching 100% degradation after 60 minutes. The primary active sites in NFC-600 were identified as C $̿$ O groups, defects, and Fe₃O₄. The degradation pathway involved initial oxidation of phenol to quinone via free radical reactions or electron transfer, followed by ring-opening reactions and C $̿$ C bond breaking to form small-molecule acids, which were ultimately mineralized to H₂O and CO₂. The results indicated that NFC-600 exhibited excellent catalytic performance and pH adaptability, providing an effective pathway for the resource utilization of cold-rolling sludge and the degradation of phenolic wastewater.

Key words: cold-rolled sludge, Fe/C catalyst, phenol, peroxydisulfate, resourceful utilization

中图分类号:

X703

唐燕, 钟广宏, 李曦同, 高晓亚, 朱文杰, 罗永明. 冷轧污泥制备Fe/C催化剂催化降解苯酚[J]. 化工进展, 2025, 44(12): 7270-7280.

TANG Yan, ZHONG Guanghong, LI Xitong, GAO Xiaoya, ZHU Wenjie, LUO Yongming. Preparation of Fe/C catalyst from cold-rolled sludge for catalytic degradation of phenol[J]. Chemical Industry and Engineering Progress, 2025, 44(12): 7270-7280.

图/表 16

参考文献 56

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元素	质量分数/%
C	8.26
O	43.50
Na	1.21
Si	1.61
P	4.80
S	1.05
Ca	5.87
Ti	4.17
Fe	13.00
AI	15.00

元素	质量分数/%
C	8.26
O	43.50
Na	1.21
Si	1.61
P	4.80
S	1.05
Ca	5.87
Ti	4.17
Fe	13.00
AI	15.00

样品	比表面积/m²·g^-1	总孔容/cm³·g^-1	平均孔径/nm
NFC-500	289.18	0.511	6.6
NFC-600	170.50	0.407	11.1
NFC-700	95.56	0.229	3.4
NFC-800	73.64	0.180	3.5

样品	比表面积/m²·g^-1	总孔容/cm³·g^-1	平均孔径/nm
NFC-500	289.18	0.511	6.6
NFC-600	170.50	0.407	11.1
NFC-700	95.56	0.229	3.4
NFC-800	73.64	0.180	3.5

不同体系	零级反应		一级反应		二级反应
不同体系	k/min^-1	R²	k/min^-1	R²	k/min^-1	R²
NFC-500/PDS	2.9087×10^-4	0.970	0.03636	0.984	0.12889	0.885
NFC-600/PDS	3.1799×10^-4	0.735	0.07776	0.982	0.19653	0.962
NFC-700/PDS	3.0470×10^-4	0.826	0.05386	0.992	0.14052	0.944
NFC-800/PDS	2.6163×10^-4	0.855	0.03361	0.993	0.11678	0.938

冷轧污泥制备Fe/C催化剂催化降解苯酚

Preparation of Fe/C catalyst from cold-rolled sludge for catalytic degradation of phenol

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不同体系	铁离子浸出/mg·L^-1
NFC-500/PDS	0.97
NFC-600/PDS	0.845
NFC-700/PDS	0.9
NFC-800/PDS	0.97

催化剂	催化剂用量/g·L^-1	PDS剂量/g·L^-1	苯酚浓度/mg·L^-1	去除效率/%	k/min^-1	pH	稳定性	参考文献
N-BC	0.4	1.0	50	98.8（120min）	0.0334	3~11（2h, 90%）	循环4次（47.5%）	[41]
Fe₃O₄/NC	1.0	2.0	20	100（120min）	—	3~9（2h, 95%）	循环5次（84.3%）	[42]
nZVI-BC	0.4	0.8	50	100（60min）	0.1049	3~9（2.5h, 85.72%）	循环3次（84.5%）	[43]
FeS@NBC_BM	0.4	1.6	50	92.7（60min）	0.0316	3~9（2.5h, 85.72%）	循环3次（65%）	[44]
ZSBC	1.0	1.0	50	100（180min）	0.04	3~11（2h, 70.7%）	循环2次（64.5%）	[45]
B-nZVI	0.5	0.2	10	73.6（30min）	—	—	—	[46]
FeO	0.3	0.2	0.9	97.8（30min）	0.2359	4~8（0.5h, 18.2%）	—	[47]
GNS TBC900	0.1	0.4	9.4	99（180min）	0.023	—	循环3次（80%）	[48]
NFC-600	0.5	1.0	20	100（30min）	0.0778	3~10（1h, 100%）	循环5次（76%）	本文

中间产物	分子式	分子量	质荷比
苯酚（phenol）	C₆H₅OH	94.11	94.06
对苯二酚（hydroquinone）	C₆H₆O₂	110.11	110.01
邻苯二酚（catechol）	C₆H₆O₂	110.11	110.01
四羟基联苯（3,3,4,4-tetrahydroxybiphenyls）	C₁₂H₁₀O₄	218.21	217.05
对苯醌（1,4-benzoquinone）	C₆H₄O₂	108.10	108.07
1,2-苯醌（1,2-benzoquinone）	C₆H₄O₂	108.10	108.07
羟基对苯二酚（hydroxy-terephthaquinone）	C₆H₄O₃	124.09	123.06
富马酸（fumaric acid）	C₄H₄O₄	116.07	116.10
己二烯二酸（muconic acid）	C₆H₆O₄	142.11	142.15
马来酸（maleic acid）	C₄H₄O₄	116.07	115.09
醋酸（acetic acid）	CH₃COOH	60.05	58.95
草酸（oxalic acid）	C₂H₂O₄	90.03	88.98
碳酸（carbonic acid）	CH₂O₃	62.02	60.09

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