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化学进展 2020, Vol. 32 Issue (9): 1412-1426 DOI: 10.7536/PC191225 前一篇   后一篇

• 综述 •

污泥碳基催化材料的合成及在水环境中的应用

谷麟1,**(), 章凯1, 俞海祥1, 董光霞1, 乔兴博1, 闻海峰1   

  1. 1. 上海理工大学 上海 200093
  • 收稿日期:2019-12-27 修回日期:2020-05-01 出版日期:2020-09-24 发布日期:2020-06-30
  • 通讯作者: 谷麟
  • 作者简介:
    ** Corresponding author e-mail:
  • 基金资助:
    *国家自然科学基金项目(51408358)
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Synthesis of Sludge Carbon-Based Catalytic Materials and Their Application in Water Environment

Lin Gu1,**(), Kai Zhang1, Haixiang Yu1, Guangxia Dong1, Xingbo Qiao1, Haifeng Wen1   

  1. 1. University of Shanghai for Science and Technology, Shanghai 200093, China
  • Received:2019-12-27 Revised:2020-05-01 Online:2020-09-24 Published:2020-06-30
  • Contact: Lin Gu
  • Supported by:
    the National Natural Science Foundation of China(51408358)

污泥是城市污水处理厂的副产物,是一种典型的固体废弃物,具有污染与资源的双重属性。以污泥作为原材料制备碳基催化材料并用于水环境催化是一种新型的污泥减量化和资源化利用方式。由于污泥是生物质有机质和多种无机氧化物、金属离子的混合物,因此以其制备的碳基催化剂或载体材料具有原料易得、活性位点分散、表面化学官能团易于调控、比表面积高等特点,并被广泛地用于多相Fenton催化、电催化、光催化、湿式氧化和臭氧氧化等水环境催化领域。本文将阐述污泥碳基催化剂材料的制备和改性方法,通过材料物理、化学性质与催化作用的构效关系并结合其在水环境催化领域的应用特点,说明碳基催化剂参与水中污染物吸附、电子转移和有机物降解的作用机制,同时对提高污泥基材料的稳定性、可重复利用性和催化活性提出新的展望。

关键词： 污泥, 碳基材料, 催化剂, 有机污染物

With dual attributes of pollutant and resources, sewage sludge(SS) is the byproduct from wastewater treatment plant, which belongs to typical urban solid waste. The use of SS as raw materials for the synthesis of carbon-based catalysts and their application in water environment catalysis is an implement of sludge reduction and resource reutilization. As SS is a mixture of organic matter from biomass and various inorganic oxides and metal ions, the carbon-based catalyst or carrier prepared from SS has the properties of easy availability of raw materials, strong dispersibility of active components on the carrier, easy adjustment of surface chemical functional groups, and high specific surface area. It is widely used in the field of multiphase Fenton reaction, electrochemical catalytic oxidation, complex photocatalytic reaction, catalytic wet oxidation and catalytic ozonation. This paper will describe the preparation and modification methods of sludge carbon-based catalyst materials. In addition, the mechanism, which carbon-based catalysts participate in pollutant adsorption, electron transfer, and organic degradation in water, is explained by the structure-activity relationship between physico-chemical properties of materials and catalytic action, combined with its application characteristics in the field of water environment catalysis. At the same time, a new prospect is put forward to improve the stability, reusability and catalytic activity of sludge-based materials.

Contents

1 Introduction

2 Physical and chemical properties of sludge carbon-based precursors

2.1 Chemical composition

2.2 Physical structure

2.3 Surface chemical properties

3 Sludge carbon-based catalyst material preparation method

3.1 Direct pyrolysis

3.2 Load method

3.3 Blending method

3.4 Hydrothermal carbonization

4 Surface modification of sludge carbon-based catalyst materials

5 Application of sludge carbon-based catalyst in the field of water environment catalysis

5.1 Catalytic H2O2 heterogeneous Fenton reaction

5.2 Catalytic degradation based on persulfate(PS) and peroxymonosulfate(PMS)

5.3 Composite photocatalytic reaction

5.4 Heterogeneous catalytic ozonation

5.5 Heterogeneous catalytic wet oxidation

5.6 Electrochemical catalytic oxidation

6 Stability of sludge carbon-based catalyst

7 Conclusion and outlook

Key words: sludge, carbonized materials, catalyst, organic pollutants
()
图1 硅氧化物催化H2O2的机理示意图[19]
Fig.1 Schematic diagram of the mechanism of catalysis of H2O2 with silicon oxide[19]
表1 各种污泥碳基催化剂材料制备方法及其物理化学性质
Table 1 A summary of the sewage sludge based carbon catalysts and their physiochemical properties
Catalyst Preparation procedure Method BET surface area(m2/g) Catalytic components ref
FeSC Dried sludge impregnated into 0.5 M FeSO4 solution and subsequently carbonized at 800 ℃ in the presence of N2 Wetness impregnation 14.3 Magnetite, Quartz, Al2O3 19
SC Dried sludge carbonized at 800 ℃ in the presence of N2 Direct pyrolysis 57.6 Carbon, ash 14, 22
SBC Dried sludge impregnated into 3 M ZnCl2 solution and carbonized at 700 ℃ in the presence of N2 wash: 3 M HCl Wetness chemical activation 363 Carbon 23
FMSAC Carbonized sludge(by ZnCl2 pre-activation) was co-precipitated with Fe2+ and Fe3+ with NaOH addition Chemical activation plus co-precipitation 880~940 Fe3O4, CaO, Quiz 24
R1 Solid mixing of dried sludge with FeCl3(w/w=1∶1) and subsequently carbonized at 700 ℃ wash: 3 M HCl Solid chemical activation 517~836 Fe species 25
szSAC Dried sludge impregnated into the mixture of 3 M H2SO4 and ZnCl2 and then carbonized at 550 ℃ wash: 10% HCl Wetness chemical activation 179.9 Surface-OH 18
szSAC/Mn szSAC impregnated into KMnO4 solution and carbonized at 550 ℃ in the presence of N2 Wetness impregnation 3.7~11.7 Mn(Ⅱ), Mn(Ⅲ), Mn(Ⅳ), surface-OH 18
DR-SA-A Dried sludge was firstly carbonized with N2 and then activated with steam at 838 ℃, acid washed. Steam activation 497.4 Dissolved organic matters and iron 26
nO x /SBAC FeO x /SBAC Dried sludge was firstly activated with ZnCl2 and carbonized at 700 ℃ and had acid washed, then the carbonized products was impregnated into Mn/Fe solutions and re-carbonized at 600 ℃ Chemical activation and wetness impregnation 327~339 Mn3O4, Fe3O4 15
CFA/SC Combined ZnCl2 activation and carbonization at 800 ℃ for the mixture of sewage sludge and fly ash(3 M HCl wash) Chemical activation 415 Fe2O3, SiO2, Al2O3 27
SS-Ti-700 Combined hydrothermal reaction with TiOSO4 and carbonization at 700 ℃ Hydrothermal reaction 35.46 TiO2, α-Fe2O3 28
FAS-1-350 Dried sludge impregnated into(NH4)2Fe(SO4)2 solutions, separated and calcined at 350 ℃ in the air Wetness impregnation 15.17 α-Fe2O3, SiO2 crystallites 29
MC600 Combined microwave digestion and KOH activation, then carbonized in the N2 Chemical activation 378 O-containing groups, Fe3O4, α-Fe 30
SC-F-0.2 Combined Fenton’s activation and carbonization at 600 ℃ Radical activation 46.3 Fe3O4, α-Fe 31
图2 表面酸性官能团吸附底物分子示意图[52]
Fig.2 Schematic diagram of adsorption of surface acidic functional group by substrate molecule[52]
图3 铁负载污泥基活性炭的基本结构示意图及其催化过氧化氢示意图[8]
Fig.3 Basic structure of sewage sludge based catalyst and their catalytic process[8]
图4 磁性污泥基催化剂对过硫酸盐和二萘酚的化学吸附[30]
Fig.4 Chemical adsorption of persulfate and 2-naphthol by magnetic sludge carbon-based catalyst[30]
图5 模板法制备污泥TiO2光催化剂示意图[51]
Fig.5 Schematic diagram of preparation of sludge TiO2 photocatalyst by template method[51]
图6 富铁污泥碳化产物参与光Fenton反应示意图[28]
Fig.6 Schematic diagram of photo-Fenton reaction involving sludge iron carbide supported by iron salt[28]
图7 影响污泥碳基催化剂稳定性的三种因素示意图
Fig.7 Schematic diagram of three factors affecting the stability of sludge carbon-based catalyst
表2 几种污泥碳基材料在不同催化体系中的稳定性和可重复利用性比较
Table 2 Comparison of stability and recyclability of several sludge carbonized materials in different catalytic systems
Leaching Species Leaching Concentration Reaction Recyclability ref
Fe 0.6 g/L(2.5%of the total Fe load) CWPO 14.2% of the Fe load 25
Fe not detectable CWPO 96% degradation efficiency obtained in third cycles of reaction 92
Fe 0.037 mg/L(0.14% of total Fe loaded) Ca: 0.813 Cu: 0.029 Mg: 0.271 Zn: 0.027 CWPO 97% removal of AOII until at least 600 min 19
Fe 1.9 mg/L for HNO3 treated SW 2.1 mg/L for H2SO4 treated SW 1.2mg/L for HCl treated SW 0.7 mg/L for SW CWPO 26.3% conversion of cresol for HCl-SW at 432 h 100% conversion of cresol for H2SO4-SW at 432 h 85.1% conversion of cresol for HNO3-SW at 432 h 40% to lower than 10% conversion rate for SW 52
Fe 10.8 mg/L for HNO3 treated SW 11.7 mg/L for H2SO4 treated SW 0.8 mg/L for HCl treated SW 1.2 mg/L for SW CWAO Not mentioned 7
Fe Fe: 18 mg/L Ni: 12 mg/L Zn: 4 mg/L Mn: 3 mg/L Cr: 3mg/L Mg: 2 mg/L CWAO For the fourth experiment, the differences after 4 h of reaction only amounted to 2.2% for phenol conversion and 9% for TOC conversion. 26
Fe 27 mg/L(7% of the total Fe load) CWAO After 4 runs, the 2-CP conversion and the TOC removal were still very high. 14
Fe 4.32 mg/L for SS-Fe-105 after 60 min 0.66 mg/L for SS-Fe-350 after 30min Photo-Fenton No obvious deactivation of the SS-Fe-350 catalyst in the six repetitive experiments was observed when compared with the first cycle. 28
Zn, Cu 0.014 mg/L PMS The distributions of these heavy metals were unchanged though the MnO x /HCAS catalyst was reused up to 5 cycles. 93
Fe pH 2.03:4.69 mg/L(2.14% of total iron) pH 3.01:3.06 mg/L PS three times for the oxidative degradation of AO7 65
Fe total Fe: 3.01 mg/L; Fe3+: 2.12mg/L CWPO It was observed that the mineralization rate decreased from 60.6 to 46.5% when the degradation rate of NOR decreased from 98.8 to 76.4%. 94
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