微波协同高级氧化技术修复有机污染土壤的研究进展

doi:10.16085/j.issn.1000-6613.2024-1326

摘要/Abstract

摘要：

微波加热相比传统加热在加热方式、活化机理和能耗成本上展现出显著优势，微波协同高级氧化技术（microwave combined advanced oxidation processes，MCAOPs）因具有条件温和、反应可控、处理效率高和适用范围广等特点，在有机污染土壤修复领域广受研究者关注。本文综述了MCAOPs在有机污染土壤修复领域的研究进展：介绍了微波加热技术发展和作用特性；归纳了常见的微波协同高级氧化技术修复污染土壤体系种类；明晰了微波功率和温度、水土比等工艺参数对有机污染物降解的影响；厘清了土壤有机质、土壤矿物和土壤水分对反应体系的影响机制；概述了土壤介质中MCAOPs的反应机制、微波作用机理和环境效应；总结了目前实验室和中试规模尺度的微波装置与优化问题并提出了MCAOPs修复有机污染土壤的放大概念模型。最后，针对当前的研究现状，概述了MCAOPs修复污染土壤领域中有待进一步研究的方向，以期推进MCAOPs理论基础的深入探索和技术的广泛应用。

关键词: 微波加热, 高级氧化, 土壤修复, 有机污染物, 降解

Abstract:

Microwave heating demonstrates notable benefits compared to conventional heating methods in aspect of heating modes, activation processes, and energy usage expenses. The research of microwave combined advanced oxidation processes (MCAOPs) in organic-contaminated soil remediation is on the rise, attributed to their gentle condition, controllable reaction, superior efficiency, and broad usability. This review examined MCAOPs' advancements in organic contaminated soil remediation, delved into microwave heating technology's evolution and features, outlined prevalent microwave-based advanced oxidation remediation technologies, investigated how factors like microwave power, temperature, and the water-to-soil ratio affected organic contaminants breakdown, elucidated the effects of soil organic matter, minerals, and moisture on these systems, outlined the reaction mechanism, microwave action mechanism and environmental effects of MCAOPs in soil, and summarized current lab- and pilot-scale microwave reactors and optimization issues, as well as proposing a viable conceptual model for amplifying MCAOPs in organic contaminant soil remediation. Ultimately, the review outlined the domains requiring additional exploration in MCAOPs for treating polluted soil, with the aim of enhancing the theoretical basis of MCAOPs and promoting their widespread use.

Key words: microwave heating, advanced oxidation, soil remediation, organic pollutants, degradation

中图分类号:

赵锡望, 高丽, 梁振明, 刘希涛. 微波协同高级氧化技术修复有机污染土壤的研究进展[J]. 化工进展, 2025, 44(10): 5911-5925.

ZHAO Xiwang, GAO Li, LIANG Zhenming, LIU Xitao. Progress in remediation of organic contaminated soil by microwave combined advanced oxidation processes[J]. Chemical Industry and Engineering Progress, 2025, 44(10): 5911-5925.

图/表 5

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污染物	微波反应体系	最优反应条件	土壤性质	降解效果/%	参考文献
微波协同氧化剂体系
邻苯二甲酸二丁酯（21.7mg/kg）	MW/过碳酸钠	Power=480W，[SPC]=0.196g/10g土，T=80℃，t=40min，W/S=4/1^①	pH=8.36，SOM=1.11%	85.14	[34]
毒死蜱（100mg/kg）	MW/PS	Power=480W，[PS]=28.57mmol/kg，T=80℃（PDS）/60℃（PMS），t=45min，W/S=1	pH=7.65，SOM=1.96%，sand=80.27%，silt=12.39%，clay=7.34%^③	>90.00	[35]
乙基对硫磷（60mg/kg）	MW/PDS	[PDS]=23.8g/kg，T=100℃，t=60min，W/S=1/10	pH=7.78	75.30	[36]
萘	MW/PDS	[PDS]=1.0mol/L，T=80℃，t=60min，	pH=6.45，Moi=4.37%，SOM=3.45%，sand=19.37%，silt=71.35%，clay=9.28%^④	96.50	[37]
阿特拉津（50mg/kg）	MW/PDS	Power=400W，[PDS]=24mmol/L，T=80℃，t=60min，W/S=1	—	97.90	[38]
对硫磷（50mg/kg）	MW/PDS	Power<900W，[PDS]=2mol/L，T=80℃，t=90min，W/S=1/4	pH=6.8，sand=35.4%，silt=58.8%，clay=5.8%	90.03	[39]
菲（1000mg/kg）	MW/PDS	Power=480W，[PDS]=50g/L，T=80℃，t=5min，W/S=5	pH=7.65，SOM≈2.4%，sand=46%，silt=10%，clay=44%	约96.00	[40]
2,4-二氯酚（500mg/kg）	MW/O₃	Power=750W（C）^②，[O₃]≈3g/h，T≈110℃，t=10min	pH=7.41，SOM=0.71%，sand=29%，silt=14%，clay=57%	90.50	[41]
蒽（50mg/kg）	MW/O₃	Power=750W(C)，[O₃]≈3g/h，T≈110℃，t=10min	pH=7.41，SOM=0.71%，sand=29%，silt=14%，clay=57%	99.60	[41]
微波协同催化剂-氧化剂体系
芘（50mg/kg）	MW/PDS/β-MnO₂	Power<900W，[PDS]=1.5mol/L，[β-MnO₂]=0.10g/5g soil，T=80℃，t=25min，W/S=1/4	pH=6.8，sand=35.4%，silt=58.8%，clay=5.9%	81.30	[42]
芘（50mg/kg）	MW/PDS/Fe₃O₄	[PDS]=1.5mol/L，[Fe₃O₄]=8g/kg，T=60℃，t=45min，W/S=1/5.6	pH=6.8，SOM=1.34%，sand=57.1%，silt=34.7%，clay=8.2%	91.70	[43]
乙基对硫磷（60mg/kg）	MW/PDS/生物炭（Biochar）	[PDS]=23.8g/kg，[Biochar]=30g/kg，T=100℃，t=80min，W/S=1/10	pH=7.78	约95.00	[44]
毒死蜱（100mg/kg）	MW/PMS/暖贴固废（HPW）	Power=480W，[PMS]=28.57mmol/kg，[HPW]=10g/kg，T=60℃，t=45min，W/S=1	pH=7.65，SOM=1.96%，sand=80.27%，silt=12.39%，clay=7.34%	>90.00	[45]
十溴二苯醚（20mg/kg）	MW/PDS/Fe@SiC	Power=240W（C），[PDS]=0.5mol/L，[Fe@SiC]=50g/kg，T<95℃，t=20min，W/S=3	模拟污染硅藻土	90.30	[46]
六氯苯（约167mg/kg）	MW/PDS/Al₂O₃负载石墨棒	Power=1100W（C），[PDS]=15g/L，石墨棒尺寸3cm×5cm，t=3min，W/S=2/3	—	约89.00	[47]
微波协同高级氧化的其他体系
2,4-二氯酚（500mg/kg）	MW/SiC/nZVI/EDTA	Power=540W，[SiC/nZVI]=2.5g/L，[EDTA]=1.2mmol/L，T=95℃，t=30min，W/S=20	模拟污染高岭土	约100.00	[48]
对氯硝基苯（50mg/kg）	MW/PDS/厌氧	[PDS]=1.0mol/L，T=60℃，t=60min，W/S=1/5.6	pH=6.8，SOM=1.34%，sand=57.1%，silt=34.7%，clay=8.2%	84.30	[49]

污染物	微波反应体系	最优反应条件	土壤性质	降解效果/%	参考文献
微波协同氧化剂体系
邻苯二甲酸二丁酯（21.7mg/kg）	MW/过碳酸钠	Power=480W，[SPC]=0.196g/10g土，T=80℃，t=40min，W/S=4/1^①	pH=8.36，SOM=1.11%	85.14	[34]
毒死蜱（100mg/kg）	MW/PS	Power=480W，[PS]=28.57mmol/kg，T=80℃（PDS）/60℃（PMS），t=45min，W/S=1	pH=7.65，SOM=1.96%，sand=80.27%，silt=12.39%，clay=7.34%^③	>90.00	[35]
乙基对硫磷（60mg/kg）	MW/PDS	[PDS]=23.8g/kg，T=100℃，t=60min，W/S=1/10	pH=7.78	75.30	[36]
萘	MW/PDS	[PDS]=1.0mol/L，T=80℃，t=60min，	pH=6.45，Moi=4.37%，SOM=3.45%，sand=19.37%，silt=71.35%，clay=9.28%^④	96.50	[37]
阿特拉津（50mg/kg）	MW/PDS	Power=400W，[PDS]=24mmol/L，T=80℃，t=60min，W/S=1	—	97.90	[38]
对硫磷（50mg/kg）	MW/PDS	Power<900W，[PDS]=2mol/L，T=80℃，t=90min，W/S=1/4	pH=6.8，sand=35.4%，silt=58.8%，clay=5.8%	90.03	[39]
菲（1000mg/kg）	MW/PDS	Power=480W，[PDS]=50g/L，T=80℃，t=5min，W/S=5	pH=7.65，SOM≈2.4%，sand=46%，silt=10%，clay=44%	约96.00	[40]
2,4-二氯酚（500mg/kg）	MW/O₃	Power=750W（C）^②，[O₃]≈3g/h，T≈110℃，t=10min	pH=7.41，SOM=0.71%，sand=29%，silt=14%，clay=57%	90.50	[41]
蒽（50mg/kg）	MW/O₃	Power=750W(C)，[O₃]≈3g/h，T≈110℃，t=10min	pH=7.41，SOM=0.71%，sand=29%，silt=14%，clay=57%	99.60	[41]
微波协同催化剂-氧化剂体系
芘（50mg/kg）	MW/PDS/β-MnO₂	Power<900W，[PDS]=1.5mol/L，[β-MnO₂]=0.10g/5g soil，T=80℃，t=25min，W/S=1/4	pH=6.8，sand=35.4%，silt=58.8%，clay=5.9%	81.30	[42]
芘（50mg/kg）	MW/PDS/Fe₃O₄	[PDS]=1.5mol/L，[Fe₃O₄]=8g/kg，T=60℃，t=45min，W/S=1/5.6	pH=6.8，SOM=1.34%，sand=57.1%，silt=34.7%，clay=8.2%	91.70	[43]
乙基对硫磷（60mg/kg）	MW/PDS/生物炭（Biochar）	[PDS]=23.8g/kg，[Biochar]=30g/kg，T=100℃，t=80min，W/S=1/10	pH=7.78	约95.00	[44]
毒死蜱（100mg/kg）	MW/PMS/暖贴固废（HPW）	Power=480W，[PMS]=28.57mmol/kg，[HPW]=10g/kg，T=60℃，t=45min，W/S=1	pH=7.65，SOM=1.96%，sand=80.27%，silt=12.39%，clay=7.34%	>90.00	[45]
十溴二苯醚（20mg/kg）	MW/PDS/Fe@SiC	Power=240W（C），[PDS]=0.5mol/L，[Fe@SiC]=50g/kg，T<95℃，t=20min，W/S=3	模拟污染硅藻土	90.30	[46]
六氯苯（约167mg/kg）	MW/PDS/Al₂O₃负载石墨棒	Power=1100W（C），[PDS]=15g/L，石墨棒尺寸3cm×5cm，t=3min，W/S=2/3	—	约89.00	[47]
微波协同高级氧化的其他体系
2,4-二氯酚（500mg/kg）	MW/SiC/nZVI/EDTA	Power=540W，[SiC/nZVI]=2.5g/L，[EDTA]=1.2mmol/L，T=95℃，t=30min，W/S=20	模拟污染高岭土	约100.00	[48]
对氯硝基苯（50mg/kg）	MW/PDS/厌氧	[PDS]=1.0mol/L，T=60℃，t=60min，W/S=1/5.6	pH=6.8，SOM=1.34%，sand=57.1%，silt=34.7%，clay=8.2%	84.30	[49]

微波反应体系	主要活性物种	氧化电位	活性物种寿命	其他可能活性物种	参考文献
MW/PDS	SO₄·^-	2.5~3.1V（vs. NHE）	30~40μs	OH·，O₂·^-，¹O₂	[11-12,38]
MW/PMS	¹O₂	0.81~2.2V（vs. NHE）	3.5μs	SO₄·^-，OH·	[35,82]
MW/O₃	O₃	2.07V（vs. NHE）	20min	OH·	[41,83]
MW/SPC或UHP	CO₃·^-（SPC），OH·	1.57~1.78（vs. NHE)（CO₃·^-） 1.8~2.7V（vs. NHE)（OH·）	1μs（OH·） —	O₂·^-	[29,84]

微波反应体系	主要活性物种	氧化电位	活性物种寿命	其他可能活性物种	参考文献
MW/PDS	SO₄·^-	2.5~3.1V（vs. NHE）	30~40μs	OH·，O₂·^-，¹O₂	[11-12,38]
MW/PMS	¹O₂	0.81~2.2V（vs. NHE）	3.5μs	SO₄·^-，OH·	[35,82]
MW/O₃	O₃	2.07V（vs. NHE）	20min	OH·	[41,83]
MW/SPC或UHP	CO₃·^-（SPC），OH·	1.57~1.78（vs. NHE)（CO₃·^-） 1.8~2.7V（vs. NHE)（OH·）	1μs（OH·） —	O₂·^-	[29,84]