Research progress on degradation of organic pollutants by single atom activated persulfate

doi:10.19965/j.cnki.iwt.2023-0474

Abstract

Abstract:

With the rapid development of industry, large amount of refractory organic pollutants in domestic and industrial wastewater are discharged into water bodies, posing a serious threat to human health and the environment. Advanced oxidation processes (AOPs) based on persulfates have shown outstanding performance in treating refractory organic wastewater, and the use of single-atom catalysts (SACs) can maximize the utilization of metal atoms and reduce the leaching of metal ions, which has a promising application prospect in the activation of persulfates for the degradation of organic pollutants. The preparation methods of single-atom catalysts were summarized, and the advantages and disadvantages of various methods were discussed. The application of single-atom catalysts with metals such as Fe, Co, Mn and Cu in the activation of persulfates for the degradation of organic pollutants was discussed. The mechanisms of single-atom catalysts in activating persulfates and the degradation mechanisms of the persulfate system catalyzed by single-atom catalysts towards organic pollutants were summarized. Finally, the future development of single-atom catalysts in activating persulfates for the degradation of organic pollutants was discussed.

Key words: single-atom catalysts, persulfate, organic pollutants, metal-based catalysts

摘要：

随着工业的迅速发展，含有大量难降解有机污染物的生活生产废水被排入水体，对人体健康与环境产生严重威胁。基于过硫酸盐的高级氧化技术在处理难降解有机废水上有着突出表现，而采用单原子催化剂能最大限度地利用金属原子，减少金属离子溶出，在活化过硫酸盐降解有机污染物中有很好的应用前景。综述了单原子催化剂的制备方法，并阐述了各种方法的优缺点。分别论述了Fe、Co、Mn和Cu等金属单原子催化剂活化过硫酸盐降解有机污染物的应用，并总结了单原子催化剂活化过硫酸盐的机理以及单原子催化剂活化过硫酸盐体系对有机污染物的降解机理。最后对单原子催化剂活化过硫酸盐降解有机污染物未来的发展做出了讨论及展望。

关键词: 单原子催化剂, 过硫酸盐, 有机污染物, 金属基催化剂

CLC Number:

X703.1

Jie ZHAO, Junfeng WU, Yanyan DOU, Fedorov Svyatoslav VIKTOROVICH, Xianli WANG, Biao LIU, Xinfeng ZHU, Yanli MAO, Hongbin GAO. Research progress on degradation of organic pollutants by single atom activated persulfate[J]. Industrial Water Treatment, 2024, 44(7): 38-46.

赵杰, 吴俊峰, 窦艳艳, VIKTOROVICH Fedorov Svyatoslav, 王现丽, 刘彪, 朱新锋, 毛艳丽, 高宏斌. 单原子活化过硫酸盐降解有机污染物研究进展[J]. 工业水处理, 2024, 44(7): 38-46.

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URL: https://www.iwt.cn/EN/10.19965/j.cnki.iwt.2023-0474

https://www.iwt.cn/EN/Y2024/V44/I7/38

Figures/Tables 7

References 61

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方法	过程	优点	缺点	参考文献
质量分离软着陆法	高频激光蒸发源使金属气化，质谱仪精确调控，负载到载体表面	适用性广	实验条件苛刻、成本较高、产率较低	〔15〕
共沉淀法	加沉淀剂或调节pH，生成沉淀物，经过滤、洗涤、焙烧后得到	条件简单、易于操作	负载量和载体利用率较低	〔16〕
原子层沉积法	将金属镀在载体表面，交替地暴露在不同前体溶液中，经化学吸附沉积	沉积均匀性和重复性好，防止了单原子的聚集现象	稳定性不佳、成本高	〔17〕
湿浸渍法	载体在含有活性成分的溶液中浸泡，反应平衡后剩余液体倒出或载体取出	制备条件及装备简单	负载量低，易发生团簇，导致催化剂失活	〔18〕
固相熔融法	载体和单原子前驱体在高温下直接混合，经气相反应和热处理制得	热稳定性较好	制备工艺复杂、成本高	〔19〕
强静电吸附法	金属离子配合物通过强静电作用吸附到载体表面	可以实现金属单原子的最大负载量	易受载体影响	〔20〕
直接转化法	将贵金属纳米颗粒经高温直接转化成热稳定贵金属单原子催化剂	热稳定性好、催化活性高、选择性强	制备条件苛刻	〔21〕
光化学合成法	纳米颗粒经光照射后得到单原子催化剂	反应条件温和、易于控制、污染小	转化率低、光能利用率低	〔22〕

方法	过程	优点	缺点	参考文献
质量分离软着陆法	高频激光蒸发源使金属气化，质谱仪精确调控，负载到载体表面	适用性广	实验条件苛刻、成本较高、产率较低	〔15〕
共沉淀法	加沉淀剂或调节pH，生成沉淀物，经过滤、洗涤、焙烧后得到	条件简单、易于操作	负载量和载体利用率较低	〔16〕
原子层沉积法	将金属镀在载体表面，交替地暴露在不同前体溶液中，经化学吸附沉积	沉积均匀性和重复性好，防止了单原子的聚集现象	稳定性不佳、成本高	〔17〕
湿浸渍法	载体在含有活性成分的溶液中浸泡，反应平衡后剩余液体倒出或载体取出	制备条件及装备简单	负载量低，易发生团簇，导致催化剂失活	〔18〕
固相熔融法	载体和单原子前驱体在高温下直接混合，经气相反应和热处理制得	热稳定性较好	制备工艺复杂、成本高	〔19〕
强静电吸附法	金属离子配合物通过强静电作用吸附到载体表面	可以实现金属单原子的最大负载量	易受载体影响	〔20〕
直接转化法	将贵金属纳米颗粒经高温直接转化成热稳定贵金属单原子催化剂	热稳定性好、催化活性高、选择性强	制备条件苛刻	〔21〕
光化学合成法	纳米颗粒经光照射后得到单原子催化剂	反应条件温和、易于控制、污染小	转化率低、光能利用率低	〔22〕

催化剂	过硫酸盐	目标污染物	去除率/%	所需时间/min	主要活性物质	参考文献
Fe-SAC	PMS	双酚A	100	30	高价铁氧化物	〔28〕
Fe-g-C₃N₄	PMS	磺胺甲唑	98.70	6	高价铁氧化物	〔29〕
SACo@NG	PMS	苯甲醇	90	180	¹O₂、SO₄ ^·-、·OH	〔30〕
SA-Co-N/C	PMS	萘普生	100	50	Co	〔31〕
Mn-SACs	PMS	双酚A	100	6	SO₄ ^·-、·OH	〔33〕
Cu-SACs	PMS	土霉素	96.47	60	·OH、¹O₂	〔36〕
Ni-N-C-10	PMS	苯酚	94.7	60	SO₄ ^·-、·OH、¹O₂	〔38〕
SA-Cu/rGO	PMS	磺胺甲唑	90	60	SO₄ ^·-	〔55〕
SA-Cu/g-C₃N₄	PDS	罗丹明B	99	30	O₂ ^·-、SO₄ ^·-、·OH	〔56〕
Co-C-N	PMS	金橙Ⅱ	100	10	SO₄ ^·-	〔57〕
BCN/CoN	PMS	四环素	100	30	¹O₂	〔58〕
Fe@COF	PMS	金橙Ⅱ	100	45	¹O₂	〔59〕
C₃N₄-Fe-rGO	PDS	四环素	100	15	·OH	〔60〕
Fe-g-C₃N₄	PMS	亚甲基蓝	100	20	高价铁氧化物	〔61〕

催化剂	过硫酸盐	目标污染物	去除率/%	所需时间/min	主要活性物质	参考文献
Fe-SAC	PMS	双酚A	100	30	高价铁氧化物	〔28〕
Fe-g-C₃N₄	PMS	磺胺甲唑	98.70	6	高价铁氧化物	〔29〕
SACo@NG	PMS	苯甲醇	90	180	¹O₂、SO₄ ^·-、·OH	〔30〕
SA-Co-N/C	PMS	萘普生	100	50	Co	〔31〕
Mn-SACs	PMS	双酚A	100	6	SO₄ ^·-、·OH	〔33〕
Cu-SACs	PMS	土霉素	96.47	60	·OH、¹O₂	〔36〕
Ni-N-C-10	PMS	苯酚	94.7	60	SO₄ ^·-、·OH、¹O₂	〔38〕
SA-Cu/rGO	PMS	磺胺甲唑	90	60	SO₄ ^·-	〔55〕
SA-Cu/g-C₃N₄	PDS	罗丹明B	99	30	O₂ ^·-、SO₄ ^·-、·OH	〔56〕
Co-C-N	PMS	金橙Ⅱ	100	10	SO₄ ^·-	〔57〕
BCN/CoN	PMS	四环素	100	30	¹O₂	〔58〕
Fe@COF	PMS	金橙Ⅱ	100	45	¹O₂	〔59〕
C₃N₄-Fe-rGO	PDS	四环素	100	15	·OH	〔60〕
Fe-g-C₃N₄	PMS	亚甲基蓝	100	20	高价铁氧化物	〔61〕

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