杂原子掺杂碳材料活化过硫酸盐技术的研究进展

doi:10.16085/j.issn.1000-6613.2020-0501

摘要/Abstract

摘要：

碳材料因其比表面积高、吸附性能佳，并且能克服加热、紫外光照射、超声等传统活化方式能耗高、金属催化材料产生二次污染的弊端而在活化过硫酸盐降解有机污染物应用中具有潜力。杂原子（N、S、B、P等）掺杂不仅能打破碳材料网络惰性、提高电导率，还能增加反应活性位点，是提升碳材料活化过硫酸盐性能的有效途径。本文介绍了碳材料活化过硫酸盐的机理，主要包括自由基途径、单线态氧途径及表面电子传递，并进一步总结了杂原子掺杂碳材料活化过硫酸盐的机理；然后综述了杂原子碳材料的种类、制备方法及其在有机污染物降解中的应用，最后指出了已有研究存在的不足，并提出杂原子掺杂碳材料稳定性及可重复利用性的提升和降解机制的深入探索是未来研究的方向。

关键词: 过硫酸盐, 自由基, 杂原子掺杂, 碳材料, 活化, 降解

Abstract:

Various methods have been reported for persulfate activation including the use of heat, UV, ultrasound and transition metals. However, these methods suffer from high energy input or inevitable leaching of toxic metal from metal-based catalysts, which has limited their practical applications. Then, carbonaceous materials have attracted considerable interests as heterogeneous catalysts for persulfate activation owing to their large surface area, unique adsorption property and metal-free nature. Heteroatom (N, S, B, P, etc.) doping can not only break carbonaceous materials’ network inertia to enhance the conductivity, but also can increase the reactive sites, resulting in the improvement of their performance in persulfate activation. In this paper, the persulfate activation mechanisms of carbonaceous materials were introduced, mainly involving free radical pathways, singlet oxygen pathways and surface electron transfer, and those of the heteroatom-doped carbonaceous materials were further discussed. Then, the types and fabrication methods of heteroatomic carbonaceous materials as well as their applications in degradation of organic pollutants were reviewed. Finally, it was proposed that the promotion of stability and reusability and the in-depth study of the mechanisms were the future research directions of heteroatom-doped carbonaceous materials.

Key words: persulfate, radical, heteroatom doping, carbonaceous materials, activation, degradation

中图分类号:

TB383

李小娟, 叶兰妹, 廖凤珍, 叶梓瑜, 叶礼志. 杂原子掺杂碳材料活化过硫酸盐技术的研究进展[J]. 化工进展, 2021, 40(1): 273-281.

Xiaojuan LI, Lanmei YE, Fengzhen LIAO, Ziyu YE, Lizhi YEH. Research progress in the application of heteroatom-doped carbonaceous materials for persulfate activation[J]. Chemical Industry and Engineering Progress, 2021, 40(1): 273-281.

图/表 4

参考文献 37

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单一杂原子掺杂碳材料	掺杂方法	碳基体 /前体	掺杂元素	杂原子源	活化过硫酸盐降解有机污染物效果				机理^①	文献
单一杂原子掺杂碳材料	掺杂方法	碳基体 /前体	掺杂元素	杂原子源	催化剂浓度 /mg·L^-1	过硫酸盐投加量	污染物浓度	降解效果	机理^①	文献
N-SWCNT	液相	SWCNT	N	尿素	200	2.0g·L^-1 PDS	20mg·kg^-1 硝基苯	60min，100%	R	[4]
NMC-850	液相	SBA-15	N	乙二胺和双氰胺	50	1.25g·L^-1 PMS	30mg·L^-1 邻苯基苯酚	150min，81%	¹O₂	[9]
NCNT-550	液相	CNT	N	尿素	100	8mmol·L^-1 PMS	0.106mmol·L^-1 苯酚	20min，100%	¹O₂	[24]
N-ND/PDDA/GO	液相	ND/PDDA/GO	N	NH₃	100	1mmol·L^-1 PMS	0.1mmol·L^-1 4-CP	60min，100%	E	[30]
N-RGO	液相	rGO	N	氨溶液	120	0.8mmol·L^-1 PMS	88mg·L^-1 BPA	7min，100%	R	[31]
N-rGO	液相	rGO	N	三聚氰胺	50	2g·L^-1 PMS	20mg·L^-1 IBP	180min，90%	R	[32]
N-rGO-N₂	液相	rGO	N	尿素	400	6.5mmol·L^-1 PMS	20mg·kg^-1 苯酚	20min，100%	R+¹O₂	[33]
N-AND	液相	AND	N	三聚氰胺	200	6.5mmol·L^-1 PMS	20mg·L^-1 苯酚	45min，100%	R	[34]
N-CNT-35	液相	CNT	N	硝酸铵	200	2g·L^-1 PMS	20mg·kg^-1 苯酚	45min，100%	R	[37]
NoCNT-700	液相	SWCNTs	N	三聚氰胺	100	6.5mmol·L^-1 PMS	20mg·kg^-1 苯酚	20min，100%	R+E	[38]
NG350	液相	rGO	N	硝酸铵	200	2g·L^-1 PMS	20mg·kg^-1 苯酚	180min，85%	R	[44]
G-N	液相	GO	N	硝酸铵	200	2g·L^-1 PMS	20mg·kg^-1 苯酚	45min，100%	—	[48]
NG-700	液相	rGO	N	三聚氰胺	100	6.5mmol·L^-1 PMS	20mg·kg^-1 苯酚	30min，100%	R	[51]
N-G(D)N-G(M) N-G(M)	液相	MIL-100	N	双氰胺三聚氰胺尿素	100	3.25mmol·L^-1 PMS	20mg·kg^-1 PHBA	20min，100% 30min，100% 90min，100%	¹O₂	[52]
N-G(D)	液相	MIL-100	N	双氰胺	100	3.25mmol·L^-1 PMS	50mg·kg^-1 苯酚	30min，100%	¹O₂	[53]
NH₄NO₃-CNT-OH	固相	CNT-OH (0.5∶1)	N	硝酸	100	污染物∶[PDS]= 1∶500	43.48mmol·L^-1 2,4,4-HBP	120min，100%	R	[36]
N-IrGO	固相	IrGO	N	尿素	50	500mg·L^-1 PMS	5mg·L^-1 二苯甲酮-1	60min，100%	¹O₂	[60]
CPPy-F-8	原位	PPy-F	N	聚吡咯	100	3.25mmol·L^-1 PMS	20mg·L^-1 苯酚	120min，97%	R+¹O₂	[25]
NPC-800	原位	ZIF-8	N	2-甲基咪唑	200	0.8g·L^-1 PMS	25mg·L^-1 苯酚	60min，86.1%	R	[39]
N-C-900	原位	ZIF-8	N	2-甲基咪唑	150	5mmol·L^-1 PDS	0.3mmol·L^-1 PCA	120min，＞96.3%	R+¹O₂+E	[40]
ACS-800	原位	聚噻吩	S	噻吩	50	8mmol·L^-1 PDS	40mg·L^-1 4-CP	60min，100%	R	[41]
SDAC-800	原位	聚噻吩	S	噻吩	100	15mmol·L^-1 PDS	80mg·L^-1 4-CP	90min，100%	R+E	[42]
B-OMC	液相	酚醛树脂	B	硼酸	200	1?mmol·L^-1 PMS	20mg·L^-1 BPA	60min，91%	¹O₂	[43]
NPCs	原位	ZIF-8	N	2-甲基咪唑	200	1.6mmol·L^-1 PMS	20mg·kg^-1 苯酚	60min，100%	R	[50]
PNC-800	原位	Zn-Co PBAs	N	钴氰化钾	100	1.0g·L^-1 PMS	100mg·L^-1 MB	10min，100%	R+¹O₂	[57]
CBs@NCCs	原位	Co-Fe PBAs	N	钴氰化钾	60	1.0g·L^-1 PMS	100mg·L^-1 MB	60min，＞95%	R+¹O₂	[58]

单一杂原子掺杂碳材料	掺杂方法	碳基体 /前体	掺杂元素	杂原子源	活化过硫酸盐降解有机污染物效果				机理^①	文献
单一杂原子掺杂碳材料	掺杂方法	碳基体 /前体	掺杂元素	杂原子源	催化剂浓度 /mg·L^-1	过硫酸盐投加量	污染物浓度	降解效果	机理^①	文献
N-SWCNT	液相	SWCNT	N	尿素	200	2.0g·L^-1 PDS	20mg·kg^-1 硝基苯	60min，100%	R	[4]
NMC-850	液相	SBA-15	N	乙二胺和双氰胺	50	1.25g·L^-1 PMS	30mg·L^-1 邻苯基苯酚	150min，81%	¹O₂	[9]
NCNT-550	液相	CNT	N	尿素	100	8mmol·L^-1 PMS	0.106mmol·L^-1 苯酚	20min，100%	¹O₂	[24]
N-ND/PDDA/GO	液相	ND/PDDA/GO	N	NH₃	100	1mmol·L^-1 PMS	0.1mmol·L^-1 4-CP	60min，100%	E	[30]
N-RGO	液相	rGO	N	氨溶液	120	0.8mmol·L^-1 PMS	88mg·L^-1 BPA	7min，100%	R	[31]
N-rGO	液相	rGO	N	三聚氰胺	50	2g·L^-1 PMS	20mg·L^-1 IBP	180min，90%	R	[32]
N-rGO-N₂	液相	rGO	N	尿素	400	6.5mmol·L^-1 PMS	20mg·kg^-1 苯酚	20min，100%	R+¹O₂	[33]
N-AND	液相	AND	N	三聚氰胺	200	6.5mmol·L^-1 PMS	20mg·L^-1 苯酚	45min，100%	R	[34]
N-CNT-35	液相	CNT	N	硝酸铵	200	2g·L^-1 PMS	20mg·kg^-1 苯酚	45min，100%	R	[37]
NoCNT-700	液相	SWCNTs	N	三聚氰胺	100	6.5mmol·L^-1 PMS	20mg·kg^-1 苯酚	20min，100%	R+E	[38]
NG350	液相	rGO	N	硝酸铵	200	2g·L^-1 PMS	20mg·kg^-1 苯酚	180min，85%	R	[44]
G-N	液相	GO	N	硝酸铵	200	2g·L^-1 PMS	20mg·kg^-1 苯酚	45min，100%	—	[48]
NG-700	液相	rGO	N	三聚氰胺	100	6.5mmol·L^-1 PMS	20mg·kg^-1 苯酚	30min，100%	R	[51]
N-G(D)N-G(M) N-G(M)	液相	MIL-100	N	双氰胺三聚氰胺尿素	100	3.25mmol·L^-1 PMS	20mg·kg^-1 PHBA	20min，100% 30min，100% 90min，100%	¹O₂	[52]
N-G(D)	液相	MIL-100	N	双氰胺	100	3.25mmol·L^-1 PMS	50mg·kg^-1 苯酚	30min，100%	¹O₂	[53]
NH₄NO₃-CNT-OH	固相	CNT-OH (0.5∶1)	N	硝酸	100	污染物∶[PDS]= 1∶500	43.48mmol·L^-1 2,4,4-HBP	120min，100%	R	[36]
N-IrGO	固相	IrGO	N	尿素	50	500mg·L^-1 PMS	5mg·L^-1 二苯甲酮-1	60min，100%	¹O₂	[60]
CPPy-F-8	原位	PPy-F	N	聚吡咯	100	3.25mmol·L^-1 PMS	20mg·L^-1 苯酚	120min，97%	R+¹O₂	[25]
NPC-800	原位	ZIF-8	N	2-甲基咪唑	200	0.8g·L^-1 PMS	25mg·L^-1 苯酚	60min，86.1%	R	[39]
N-C-900	原位	ZIF-8	N	2-甲基咪唑	150	5mmol·L^-1 PDS	0.3mmol·L^-1 PCA	120min，＞96.3%	R+¹O₂+E	[40]
ACS-800	原位	聚噻吩	S	噻吩	50	8mmol·L^-1 PDS	40mg·L^-1 4-CP	60min，100%	R	[41]
SDAC-800	原位	聚噻吩	S	噻吩	100	15mmol·L^-1 PDS	80mg·L^-1 4-CP	90min，100%	R+E	[42]
B-OMC	液相	酚醛树脂	B	硼酸	200	1?mmol·L^-1 PMS	20mg·L^-1 BPA	60min，91%	¹O₂	[43]
NPCs	原位	ZIF-8	N	2-甲基咪唑	200	1.6mmol·L^-1 PMS	20mg·kg^-1 苯酚	60min，100%	R	[50]
PNC-800	原位	Zn-Co PBAs	N	钴氰化钾	100	1.0g·L^-1 PMS	100mg·L^-1 MB	10min，100%	R+¹O₂	[57]
CBs@NCCs	原位	Co-Fe PBAs	N	钴氰化钾	60	1.0g·L^-1 PMS	100mg·L^-1 MB	60min，＞95%	R+¹O₂	[58]

杂原子共掺杂碳材料	掺杂方法	碳基体 /前体	掺杂元素	杂原子源	活化过硫酸盐降解有机污染物效果				机理^①	文献
杂原子共掺杂碳材料	掺杂方法	碳基体 /前体	掺杂元素	杂原子源	催化剂浓度 /mg·L^-1	过硫酸盐投加量	污染物浓度	降解效果	机理^①	文献
SNG	液相	rGO	N，S	N：硝酸铵 S：二甲基亚砜	200	6.5mmol·L^-1 PMS	20mg·kg^-1 苯酚	90min，100%	R	[29]
2sNBG-800	液相	rGO	N，B	N：尿素 B：硼酸	200	0.5mmol·L^-1 PMS	10mg·L^-1 SAM	20min，100%	R+E	[35]
N-S-PCs	液相	葡萄糖	N，S	NS：硫脲	50	6.5mmol·L^-1 PDS	20mg·L^-1 磺胺氯哒嗪	20min，100%	R+E	[47]
NPSC-700	液相	ZIF-8	N，P，S	NPS：聚丙腈	60	0.4g·L^-1 PMS	25mg·kg^-1 BPA	30min，90.10%	R	[49]
SNCs	液相	咖啡粉	N，S	NS：L-半胱氨酸	400	2mmol·L^-1 PDS	0.02mmol·L^-1 TeC	60min，100%	¹O₂+E	[59]
i-RGO-NS	固相	rGO	N，S	NS：硫脲	20	307mg·L^-1 PMS	15mg·L^-1 MP	20min，100%	¹O₂	[22]
N,S-rGO	固相	rGO	N，S	NS：硫脲	50	0.9mmol·L^-1 PDS	2mg·L^-1 BPA	20min，100%	R	[46]
NS-CNT-COOH	固相	CNT	N，S	NS：硫脲	100	1.0g·L^-1 PMS	0.01g·L^-1 BP-4	30min，100%	E	[54]

杂原子共掺杂碳材料	掺杂方法	碳基体 /前体	掺杂元素	杂原子源	活化过硫酸盐降解有机污染物效果				机理^①	文献
杂原子共掺杂碳材料	掺杂方法	碳基体 /前体	掺杂元素	杂原子源	催化剂浓度 /mg·L^-1	过硫酸盐投加量	污染物浓度	降解效果	机理^①	文献
SNG	液相	rGO	N，S	N：硝酸铵 S：二甲基亚砜	200	6.5mmol·L^-1 PMS	20mg·kg^-1 苯酚	90min，100%	R	[29]
2sNBG-800	液相	rGO	N，B	N：尿素 B：硼酸	200	0.5mmol·L^-1 PMS	10mg·L^-1 SAM	20min，100%	R+E	[35]
N-S-PCs	液相	葡萄糖	N，S	NS：硫脲	50	6.5mmol·L^-1 PDS	20mg·L^-1 磺胺氯哒嗪	20min，100%	R+E	[47]
NPSC-700	液相	ZIF-8	N，P，S	NPS：聚丙腈	60	0.4g·L^-1 PMS	25mg·kg^-1 BPA	30min，90.10%	R	[49]
SNCs	液相	咖啡粉	N，S	NS：L-半胱氨酸	400	2mmol·L^-1 PDS	0.02mmol·L^-1 TeC	60min，100%	¹O₂+E	[59]
i-RGO-NS	固相	rGO	N，S	NS：硫脲	20	307mg·L^-1 PMS	15mg·L^-1 MP	20min，100%	¹O₂	[22]
N,S-rGO	固相	rGO	N，S	NS：硫脲	50	0.9mmol·L^-1 PDS	2mg·L^-1 BPA	20min，100%	R	[46]
NS-CNT-COOH	固相	CNT	N，S	NS：硫脲	100	1.0g·L^-1 PMS	0.01g·L^-1 BP-4	30min，100%	E	[54]

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