过渡金属单原子催化剂活化H2O2/PMS/PDS降解有机污染物的研究进展

doi:10.16085/j.issn.1000-6613.2021-2140

摘要/Abstract

摘要：

单原子催化剂（SACs）是一种将金属以原子态负载于载体上的新型材料，具有原子利用率高、催化活性强和易回收等优点，使其在催化降解有机污染物方面备受关注。本文介绍了SACs的催化影响因素，总结了SACs催化降解有机污染物在环境领域中的应用。此外，着重综述了不同过渡金属（Fe、Co、Mn、Cu等）单原子催化剂在基于双氧水或过硫酸盐的高级氧化技术中的催化机理，单原子金属（M）一般与N键合形成活性位点M—N _x，活化氧化剂生成自由基或单线态氧，高效降解有机污染物。最后，提出未来SACs在催化降解有机污染物的研究方向是合成金属负载量高、稳定性高、pH适用范围更广的SACs，以及根据SACs的结构-性能关系和催化机理，对目标污染物设计特定催化剂。

关键词: 单原子催化剂, 高级氧化, 降解, 有机污染物, 机理

Abstract:

Single-atom catalysts (SACs) are a new type of material that can load metal on the carrier in atomic state. They have the advantages of high atom utilization, strong catalytic activity and easy recovery, so they have attracted much attention in the catalytic degradation of organic pollution. In this work, the influencing factors of SACs were introduced, and the applications of SACs in environmental field for catalytic degradation of organic pollutants are summarized. In addition, the catalytic mechanisms of SACs of different transition metals (Fe, Co, Mn, Cu, etc.) in advanced oxidation technology based on hydrogen peroxide or persulfate are reviewed. Single-atom metal (M) generally bonds with N to form the active site M—N _x, which activates the oxidant to generate radicals or singlet oxygen, and effectively degrades organic pollutants. Finally, the research directions of SACs on the catalytic degradation of organic pollutants are the preparation of SACs of high metal loading, high stability and wide range of pH, and the design of specific catalysts for different target pollutants according to the structure-performance relationship and catalytic mechanisms of SACs.

Key words: single-atom catalysts, advanced oxidation process, degradation, organic pollutant, mechanism

中图分类号:

段毅, 邹烨, 周书葵, 杨柳. 过渡金属单原子催化剂活化H₂O₂/PMS/PDS降解有机污染物的研究进展[J]. 化工进展, 2022, 41(8): 4147-4158.

DUAN Yi, ZOU Ye, ZHOU Shukui, YANG Liu. Progress in the degradation of organic pollutants by H₂O₂/PMS/PDS activated by transition metal single-atom catalysts[J]. Chemical Industry and Engineering Progress, 2022, 41(8): 4147-4158.

图/表 8

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图7

表1

单原子催化剂用于高级氧化中降解有机污染物的应用"

金属	催化剂/g·L^-1	合成方法	有机物及浓度 /mg·L^-1	氧化剂及浓度 /mmol·L^-1	循环次数（效率）	降解效率 /%（min）	主要活性基团	参考文献
Fe	Fe _x Mo_1-_x S₂（0.1）	水热解法	PPA（20）	PDS（1）	5（62.1%）	90（30）	SO $4 · -$	［21］
	Fe/MnO₂（0.2）	热处理法	MB（20）	H₂O₂（4.4）	—	82（80）	·OH	［53］
	Fe-N-C（0.02）	球磨法	2,4-DCP（3.3）	PDS（0.2）	—	90（60）	Fe（Ⅴ）	［20］
	Fe₃O₄/MIL-101（1）	超声法	OPD（50）	H₂O₂（0.66）	5（95%）	97.79（25）	·OH	［52］
	FePC/石墨烯（0.2）	煅烧酸洗法	苯酚（50）	H₂O₂（4.4）	5（55%）	77.1（180）	·OH	［54］
	Fe-g-C₃N₄（0.2）	高温热解法	MB（20）	H₂O₂（77）	—	99.16（80）	·OH、¹O₂	［55］
	Fe_SA-N/C（0.15）	热处理法	BPA（20）	PMS（11.77）	5（81%）	99.3（20）	¹O₂	［44］
	SA Fe-g-C₃N₄（0.1）	高温煅烧法	TC（50）	PMS（0.5）	4（91%）	93.29（40）	·OH、SO $4 · -$ 、¹O₂、Fe(Ⅳ)	［51］
Co	SA Co-N/C（0.05）	高温煅烧法	NPX（10）	PMS（0.5）	4（96%）	100（50）	·OH、SO $4 · -$ 、¹O₂	［42］
	Co-N-C（0.5）	煅烧酸洗法	BPA（80）	PMS（0.98）	3（96.3%）	100（60）	¹O₂	［24］
	Co-C-N（0.5）	模板蚀刻法	AO7（50）	PMS（0.1）	6（99.3%）	100（10）	SO $4 · -$ 、¹O₂	［25］
	SA Co-N-C（0.1）	热解法	CQP（10）	PMS（1）	3（80%）	98（20）	SO $4 · -$	［48］
	BCN/CoN（0.03）	高温煅烧法	TC（50）	PMS（8.82）	5（100%）	100（60）	¹O₂	［47］
	FeCo-NC-2（0.1）	热处理法	BPA（20）	PMS（0.65）	8（85%）	98（60）	SO $4 · -$	［56］
Mn	Mn-ISAs@CN（0.2）	热解法	BPA（20）	PMS（0.65）	5（80%）	90（60）	·OH	［27］
	Mn-CN（0.1）	热解法	OA（10）	H₂O₂（—）	5（82%）	100（40）	·OH	［29］
	SA-Mn/NG（0.1）	高温煅烧法	SMX（10）	PMS（1）	4（84%）	97（40）	·OH、SO $4 · -$	［30］
	SA-Mn/g-C₃N₄（0.1）	高温煅烧法	TBBPA（50）	PMS（5）	5（93%）	100（30）	¹O₂、SO $4 · -$	［30］
Cu	Cu-C₃N₄（1）	热解法	RhB（10）	H₂O₂（29.4）	—	99.97（60）	·OH	［31］
	SA-Cu/rGO（0.1）	球磨法	SMX（10）	PMS（1.3）	5（91.6%）	99.6（60）	·OH、SO $4 · -$ 、¹O₂	［32］
	SA-Cu@NBC（0.1）	高温煅烧法	BPA（20）	PMS（11.77）	4（97%）	100（60）	SO $4 · -$	［46］
双金属	Co/Fe-N-C（0.5）	热解法	苯酚（100）	PDS（10）	5（70.4%）	79.2（120）	SO $4 · -$ 、¹O₂	［33］
	Fe-Ce/g-C₃N₄（0.5）	高温煅烧法	MB（200）	H₂O₂（4.4）	3（90%）	100（40）	·OH、·OOH	［36］
	FeBi-NC（0.03）	热解法	RhB（30）	PMS（4.41）	5（99%）	100（5）	·OH、SO $4 · -$ 、¹O₂	［34］
	Fe/Cu-N-C（0.1）	热解法	CAP（20）	PDS（5）	5（90.8%）	90.8（60）	·OH、SO $4 · -$ 、¹O₂	［35］
Pt	Pt/Al₂O₃（0.2）	热处理法	1,4-D（20）	H₂O₂（3.5）	4（76%）	95（60）	SO $4 · -$	［39］
Ag	Ag/mpg-C₃N₄（0.1）	高温煅烧法	BPA（20）	PMS（1）	4（76%）	98（60）	SO $4 · -$	［40］

表1

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过渡金属单原子催化剂活化H₂O₂/PMS/PDS降解有机污染物的研究进展

Progress in the degradation of organic pollutants by H₂O₂/PMS/PDS activated by transition metal single-atom catalysts

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