A review of activated percarbonate and peroxymonocarbonate in the field of water treatment

doi:10.16085/j.issn.1000-6613.2021-1365

Abstract

Abstract:

In recent years, the application of activated sodium percarbonate (SPC) and peroxymonocarbonate (PMC) in water treatment has received extensive attention from scholars. By investigating a large number of domestic and foreign documents, this article systematically summarizes the current application of activated SPC system and activated PMC system in water treatment, and sorts out the common activators in SPC system, such as iron-based materials, biochar and metal composite systems, etc. , and the common transition metal ions and metal complex activators of PMC system. The main influencing factors and reaction mechanism of activating SPC and activating PMC system to degrade pollutants are explained. The influencing factors include the initial pH of the solution, the oxidant, the activator, the concentration of pollutants, and the coexisting ions. The addition of activators in the SPC and PMC systems will promote the generation of HO· and play a role in the degradation of pollutants. Finally, suggestions are made for the development trend of related research in the future. It is possible to further explore the repair performance of activated SPC and PMC systems on water, as well as their stability and safety in actual water treatment, and clarify the mechanism for free radicals generated in the system to remove pollutants in water.

Key words: percarbonate, peroxymonocarbonate(PMC), activator, wastewater treatment, advanced oxidation, hydrogen peroxide (H₂O₂)

摘要：

近年来，活化过碳酸盐（SPC）和过氧碳酸氢盐（PMC）高级氧化体系在水处理中的应用受到了学者们的广泛关注。本文通过调研大量国内外文献，系统总结了目前活化SPC体系及活化PMC体系在水处理中的应用，梳理了在SPC体系中常见的活化剂，如铁基材料、生物炭及金属复合体系等，在PMC体系常见的过渡金属离子以及金属复合物活化剂等，对比分析了活化SPC及活化PMC体系降解污染物的影响因素及其反应机理，影响因素包括溶液初始pH、氧化剂、活化剂、污染物浓度以及共存离子等，在SPC和PMC体系中添加活化剂均会促进HO·的生成，并对污染物的降解发挥作用，最后对未来相关研究的发展趋势提出了建议，可进一步探究活化SPC和PMC体系对水体的修复性能以及利用其进行实际水处理时的稳定性和安全性，厘清体系中产生的自由基对水体中污染物的去除机制。

关键词: 过碳酸盐, 过氧碳酸氢盐, 活化剂, 水处理, 高级氧化, 过氧化氢

CLC Number:

LIAO Bing, XU Wen, YE Qiuyue. A review of activated percarbonate and peroxymonocarbonate in the field of water treatment[J]. Chemical Industry and Engineering Progress, 2022, 41(6): 3235-3248.

廖兵, 胥雯, 叶秋月. 活化过碳酸盐及过氧碳酸氢盐在水处理领域中的研究进展[J]. 化工进展, 2022, 41(6): 3235-3248.

Figures/Tables 7

活化类型	活化剂	活化剂浓度	目标污染物	污染物浓度	反应时间 /min	降解率 /%	参考文献
铁基材料	Fe(Ⅱ)	1.0mmol/L	PCE	0.12mmol/L	1	90	［16］
	Fe(Ⅱ)	0.3mmol/L	SMT	0.02mmol/L	1	84	［15］
	Fe(Ⅲ)	1.0mmol/L	PCE	0.12mmol/L	60	28	［16］
	Fe²⁺	3.0mmol/L	苯	1.0mmol/L	20	100	［10］
	CIT-Fe²⁺	1mmol/L、5mmol/L	PCE	0.12mmol/L	20	99.99	［26］
	OA-Fe²⁺	5mmol/L、5mmol/L	PCE	0.12mmol/L	20	>90	［26］
	CA-Fe²⁺	1.0mmol/L、0.45mmol/L	TCE	0.15mmol/L	90	98	［18］
	CIA-Fe²⁺	1mmol/L、2mmol/L	苯	1mmol/L	30	96.3	［10］
	Z-nZVI-Ni	250mg/L	TCE	0.15mmol/L	180	99.8	［20］
	Z-nZVI-Cu	200mg/L	TCE	0.15mmol/L	180	＞95	［26］
	G-nZVI	0.8g/L	1,1,1-三氯乙烷（TCA）	0.15mmol/L	120	90	［28］
	NZ-nZVI	—	酸橙52（AO52）	25mg/L	18	100	［27］
生物炭	红藻生物炭	3.0g/L	邻苯二甲酸二(2-乙基己基)酯（DEHP）	0.02mmol/L	12	63	［22］
生物炭	富含铁锰的生物炭	1.67g/L	多环芳烃（PAHs）	1.67g/L	6	＞80	［30］
光活化	UV	—	2-羟基-4-甲氧基二苯甲酮（BP-3）	0.02mmol/L	180	＞78	［32］
光活化	UV	0.1mW·cm^-2	双酚A（BPA）	0.002mmol/L	—	87.8	［33］
其他	Fe₃O₄@ZIF-8	1g/L	亚甲蓝（MB）	20mg/L	120	98.5	［34］
	FeOCl/vis	0.5g/L	罗丹明B（RhB）	20mg/L	60	95.8	［35］
	V(Ⅳ)	1.0mmol/L	苯胺	1.0mmol/L	15	55.62	［36］
	VOSO₄	1.0mmol/L	苯胺	1.0mmol/L	15	41.29	［37］

活化类型	活化剂	活化剂浓度/投加量	目标污染物	污染物浓度	反应时间/min	降解率/%	参考文献
过渡金属离子	Co²⁺	0.02mmol/L	MB	0.134mmol/L	50	100	［42］
	Co²⁺	0.005mmol/L	酸性橙Ⅱ（AOII）	0.05mmol/L	10	>90	［43］
	Co²⁺	0.005mmol/L	AOII	0.25mmol/L	180	>90	［48］
	Cu(Ⅱ)	0.03mmol/L	AOII	0.05mmol/L	10	>90	［12］
	Cu(Ⅱ)	0.01mmol/L	三氯生（TCS）	0.01mmol/L	40	>65	［45］
复合材料	S-CoFe₂O₄	0.1g/L	AOII	50mg/L	60	98	［8］
	CoMgAl	0.03g	亚甲基橙（MO）	49.8mg/L	60	>95	［41］
	CuFeS₂	200mg/L	2，4-DCP	10mg/L	120	>80	［46］
	Co _x Mn_3-_x O₄	0.1g/L	2，4-DCP	10mg/L	120	>85	［47］

活化剂	污染物	初始pH	反应后pH	降解率/%	参考文献
Fe(Ⅱ)	SMT	4.0	3.05	88	［15］
CA-Fe²⁺	TCE	3.01	2.85	93	［18］
Fe₃O₄@ZIF-8	MB	3	—	98.5	［34］
CA-Fe(Ⅱ)	TCE	3.0	2.9	93.1	［49］
HAH/CA-Fe(Ⅱ)	TCE	3	2.5	>99	［50］
CIT/Fe(Ⅱ)	PCE	<4	3.35	92.6	［51］
nZVI	BPA	3	—	100	［7］
Fe²⁺	PCE	6.5	3.44	98	［53］
g-C₃N₄/Vis	MB	7	—	90	［56］
富含铁锰的生物炭	PAHs	11.0	—	85	［30］
O₃	SMX	10.3	8.0	>70	［52］

活化类型	反应式	编号	参考文献
铁基材料	H₂O₂ + Fe(Ⅱ) $→$ Fe(Ⅲ) + HO· + OH^-	（8）	［23，54，59］
	HO·+ H₂O₂ $→$ O $2 · -$ + H₂O + H⁺	（9）
	HO·+ Fe(Ⅱ) $→$ Fe(Ⅲ) + OH^-	（10）
	COOH^- + HO· $→$ H₂O + CO $2 · -$	（11）	［55］
	COOH^- + H· $→$ H₂ + CO $2 · -$	（12）	［55］
	HO· + HO· $→$ H₂O₂	（13）	［26］
	HO·+ Fe(Ⅱ) $→$ Fe(Ⅲ) + OH^-	（10）
	H₂O₂ + HO· $→$ HO₂· + H₂O	（14）
	HO· + CO $3 2 -$ $→$ CO $3 · -$ + OH^-	（7）	［7］
	HO· + HCO $3 -$ $→$ CO $3 · -$ + H₂O	（15）
	Fe⁰ + O₂ + 2H⁺ $→$ Fe²⁺ + H₂O₂	（16）
	Fe⁰ + H₂O₂ + 2H⁺ $→$ Fe²⁺ + 2H₂O	（17）
	Fe²⁺ + H₂O₂ $→$ HO· + Fe³⁺ + OH^-	（18）
	2Fe³⁺+ Fe⁰ $→$ 3Fe²⁺	（19）
	Ni⁺ + H₂O₂ $→$ Ni²⁺ + OH· + OH^-	（20）	［21］
	Ni²⁺ + H₂O₂ $→$ Ni⁺ + ·O₂H + OH^-	（21）
	Fe³⁺ + Ni⁺ $→$ Fe²⁺ +Ni⁺²	（22）
生物炭材料	RSB-π⁺ +H₂O₂ $→$ RSB-π + HO· + OH^-	（23）	［22］
	Fe³⁺ + H₂O₂ $→$ Fe²⁺ + O $2 · -$ + 2H⁺	（24）	［30］
	Fe³⁺ + O $2 · -$ $→$ Fe²⁺ + O₂	（25）
	Fe³⁺ + HO₂· $→$ Fe²⁺ + O₂ + H⁺	（26）
	Mn²⁺ + H₂O₂ $→$ Mn³⁺ + HO· + OH^-	（27）
	Mn³⁺ + H₂O₂ $→$ Mn²⁺ + HO₂· + H⁺	（28）
	Mn³⁺ + H₂O₂ $→$ Mn²⁺ + O $2 · -$ + 2H⁺	（29）
	Mn³⁺ + O $2 · -$ $→$ Mn²⁺ + O₂	（30）
	Mn³⁺ + HO₂· $→$ Mn²⁺ + O₂ + H⁺	（31）
	Fe²⁺ + Mn³⁺ $→$ Fe³⁺ + Mn²⁺	（32）
	PAHs + HO· + O $2 · -$ + O₂ $→$ byproducts + CO₂ + H₂O	（33）
光活化	H₂O₂ + hv $→$ 2HO·	（34）	［32］
	HO· + HCO₃^- $→$ CO $3 · -$ + H₂O	（15）	［33］
	HO· + CO₃^2- $→$ CO $3 · -$ + HO^-	（7）	［33］
其他	VO²⁺ + H₂O $→$ [VOOH]⁺ + H⁺	（35）	［36］
	[VOOH]⁺ + H₂O + H₂O₂ $→$ HVO $4 2 -$ + ·OH + 3H⁺	（36）
	HVO₄^2- + H₂O₂ + 3H⁺ $→$ VO²⁺ + HO₂· + 3H₂O	（37）
	HO· + CO $3 2 -$ $→$ CO $3 · -$ + HO^-	（7）
	H₂O₂ + CO $3 · -$ $→$ HCO $3 -$ + HO₂·	（38）
	HO₂· $→$ O $2 · -$ + H⁺	（39）

活化类型	反应式	编号	参考文献
铁基材料	H₂O₂ + Fe(Ⅱ) $→$ Fe(Ⅲ) + HO· + OH^-	（8）	［23，54，59］
	HO·+ H₂O₂ $→$ O $2 · -$ + H₂O + H⁺	（9）
	HO·+ Fe(Ⅱ) $→$ Fe(Ⅲ) + OH^-	（10）
	COOH^- + HO· $→$ H₂O + CO $2 · -$	（11）	［55］
	COOH^- + H· $→$ H₂ + CO $2 · -$	（12）	［55］
	HO· + HO· $→$ H₂O₂	（13）	［26］
	HO·+ Fe(Ⅱ) $→$ Fe(Ⅲ) + OH^-	（10）
	H₂O₂ + HO· $→$ HO₂· + H₂O	（14）
	HO· + CO $3 2 -$ $→$ CO $3 · -$ + OH^-	（7）	［7］
	HO· + HCO $3 -$ $→$ CO $3 · -$ + H₂O	（15）
	Fe⁰ + O₂ + 2H⁺ $→$ Fe²⁺ + H₂O₂	（16）
	Fe⁰ + H₂O₂ + 2H⁺ $→$ Fe²⁺ + 2H₂O	（17）
	Fe²⁺ + H₂O₂ $→$ HO· + Fe³⁺ + OH^-	（18）
	2Fe³⁺+ Fe⁰ $→$ 3Fe²⁺	（19）
	Ni⁺ + H₂O₂ $→$ Ni²⁺ + OH· + OH^-	（20）	［21］
	Ni²⁺ + H₂O₂ $→$ Ni⁺ + ·O₂H + OH^-	（21）
	Fe³⁺ + Ni⁺ $→$ Fe²⁺ +Ni⁺²	（22）
生物炭材料	RSB-π⁺ +H₂O₂ $→$ RSB-π + HO· + OH^-	（23）	［22］
	Fe³⁺ + H₂O₂ $→$ Fe²⁺ + O $2 · -$ + 2H⁺	（24）	［30］
	Fe³⁺ + O $2 · -$ $→$ Fe²⁺ + O₂	（25）
	Fe³⁺ + HO₂· $→$ Fe²⁺ + O₂ + H⁺	（26）
	Mn²⁺ + H₂O₂ $→$ Mn³⁺ + HO· + OH^-	（27）
	Mn³⁺ + H₂O₂ $→$ Mn²⁺ + HO₂· + H⁺	（28）
	Mn³⁺ + H₂O₂ $→$ Mn²⁺ + O $2 · -$ + 2H⁺	（29）
	Mn³⁺ + O $2 · -$ $→$ Mn²⁺ + O₂	（30）
	Mn³⁺ + HO₂· $→$ Mn²⁺ + O₂ + H⁺	（31）
	Fe²⁺ + Mn³⁺ $→$ Fe³⁺ + Mn²⁺	（32）
	PAHs + HO· + O $2 · -$ + O₂ $→$ byproducts + CO₂ + H₂O	（33）
光活化	H₂O₂ + hv $→$ 2HO·	（34）	［32］
	HO· + HCO₃^- $→$ CO $3 · -$ + H₂O	（15）	［33］
	HO· + CO₃^2- $→$ CO $3 · -$ + HO^-	（7）	［33］
其他	VO²⁺ + H₂O $→$ [VOOH]⁺ + H⁺	（35）	［36］
	[VOOH]⁺ + H₂O + H₂O₂ $→$ HVO $4 2 -$ + ·OH + 3H⁺	（36）
	HVO₄^2- + H₂O₂ + 3H⁺ $→$ VO²⁺ + HO₂· + 3H₂O	（37）
	HO· + CO $3 2 -$ $→$ CO $3 · -$ + HO^-	（7）
	H₂O₂ + CO $3 · -$ $→$ HCO $3 -$ + HO₂·	（38）
	HO₂· $→$ O $2 · -$ + H⁺	（39）

体系	反应式	编号	参考文献
PMC	HCO $3 -$ + H₂O₂ $→$ HCO $4 -$ + H₂O	（3）	［38，67-68］
	HCO $4 -$ + 污染物 $→$ HCO $3 -$	（40）
	HCO $4 -$ $→$ CO $3 · -$ + HO·	（41）
	H₂O₂ + CO $3 · -$ $→$ HCO $3 -$ + HO₂·	（38）
	HO· + HO₂· $→$ H₂O + O $2 · -$	（42）
	HO₂· $→$ H⁺ + O $2 · -$	（39）
	H₂O₂ $→$ 2HO·	（43）
	O $2 · -$ + HO· $→$ ¹O₂ + OH^-	（44）
	HO₂· + HO₂· $→$ ¹O₂ + H₂O₂	（45）
活化PMC	HCO $3 -$ + H₂O₂ $→$ HCO $4 -$ + H₂O	（3）	［46］
	≡≡ Fe(Ⅱ) + 2HCO $4 -$ $→$ ≡≡ Fe(Ⅲ) + 2CO $3 · -$ + HO· + OH^-	（52）
	≡≡ Fe(Ⅲ) + H₂O₂ $→$ ≡≡ Fe(Ⅱ) + O $2 · -$ + H⁺	（53）
	CO $3 · -$ + H₂O₂ $→$ HCO $3 -$ + O $2 · -$ + H⁺	（54）
	O $2 · -$ + HO· $→$ ¹O₂ + OH^-	（44）
	Co²⁺ + HCO $3 -$ $?$ [Co^Ⅱ(HCO $3 -$ )]⁺	（46）	［42］
	[Co^Ⅱ(HCO $3 -$ )]⁺ + AOⅡ $?$ [Co^Ⅱ(HCO $3 -$ )(AOⅡ)]⁺	（47）
	[Co^Ⅱ(HCO $3 -$ )(AOⅡ)]⁺ + H₂O₂ $?$ [Co^Ⅱ(HCO $3 -$ )(AOⅡ)(H₂O₂)]⁺	（48）
	[Co^Ⅱ(HCO $3 -$ )(AOⅡ)(H₂O₂)]⁺ $→$ [Co^Ⅲ(HCO $3 -$ )(AOⅡ)(·OH)]²⁺	（49）
	[Co^Ⅲ(HCO $3 -$ )(AOⅡ)(·OH)]²⁺ $→$ [Co^Ⅲ(HCO $3 -$ )]²⁺ + 氧化产物	（50）
	[Co^Ⅲ(HCO $3 -$ )]²⁺ + H₂O₂ $→$ [Co^Ⅱ(HCO $3 -$ )]⁺+ HOO· + H⁺	（51）

体系	反应式	编号	参考文献
PMC	HCO $3 -$ + H₂O₂ $→$ HCO $4 -$ + H₂O	（3）	［38，67-68］
	HCO $4 -$ + 污染物 $→$ HCO $3 -$	（40）
	HCO $4 -$ $→$ CO $3 · -$ + HO·	（41）
	H₂O₂ + CO $3 · -$ $→$ HCO $3 -$ + HO₂·	（38）
	HO· + HO₂· $→$ H₂O + O $2 · -$	（42）
	HO₂· $→$ H⁺ + O $2 · -$	（39）
	H₂O₂ $→$ 2HO·	（43）
	O $2 · -$ + HO· $→$ ¹O₂ + OH^-	（44）
	HO₂· + HO₂· $→$ ¹O₂ + H₂O₂	（45）
活化PMC	HCO $3 -$ + H₂O₂ $→$ HCO $4 -$ + H₂O	（3）	［46］
	≡≡ Fe(Ⅱ) + 2HCO $4 -$ $→$ ≡≡ Fe(Ⅲ) + 2CO $3 · -$ + HO· + OH^-	（52）
	≡≡ Fe(Ⅲ) + H₂O₂ $→$ ≡≡ Fe(Ⅱ) + O $2 · -$ + H⁺	（53）
	CO $3 · -$ + H₂O₂ $→$ HCO $3 -$ + O $2 · -$ + H⁺	（54）
	O $2 · -$ + HO· $→$ ¹O₂ + OH^-	（44）
	Co²⁺ + HCO $3 -$ $?$ [Co^Ⅱ(HCO $3 -$ )]⁺	（46）	［42］
	[Co^Ⅱ(HCO $3 -$ )]⁺ + AOⅡ $?$ [Co^Ⅱ(HCO $3 -$ )(AOⅡ)]⁺	（47）
	[Co^Ⅱ(HCO $3 -$ )(AOⅡ)]⁺ + H₂O₂ $?$ [Co^Ⅱ(HCO $3 -$ )(AOⅡ)(H₂O₂)]⁺	（48）
	[Co^Ⅱ(HCO $3 -$ )(AOⅡ)(H₂O₂)]⁺ $→$ [Co^Ⅲ(HCO $3 -$ )(AOⅡ)(·OH)]²⁺	（49）
	[Co^Ⅲ(HCO $3 -$ )(AOⅡ)(·OH)]²⁺ $→$ [Co^Ⅲ(HCO $3 -$ )]²⁺ + 氧化产物	（50）
	[Co^Ⅲ(HCO $3 -$ )]²⁺ + H₂O₂ $→$ [Co^Ⅱ(HCO $3 -$ )]⁺+ HOO· + H⁺	（51）

体系	活化类型	活化剂	污染物	体系中自由基种类	起主要作用的物质	参考文献
SPC	铁基材料	Fe(Ⅱ)	SMX	HO·、O $2 · -$	HO·	［23］
		Fe(Ⅱ)	PCE			［53］
		Fe(Ⅱ)	苯			［54］
		Fe(Ⅱ)	四环素			［59］
		Fe(Ⅲ)	苯			［61］
		螯合剂-Fe²⁺	TCE			［18］
		Fe(Ⅱ)-CA	TCE			［49］
		Fe(Ⅱ)-OA	PCE			［51］
		FA/Fe(Ⅱ)	CT	HO·、CO $2 · -$	CO $2 · -$	［55］
	生物炭材料	富含Fe、Mn的生物炭	PAHs	O $2 · -$ 、HO·	HO·	［30］
	光活化	UV	BP-3	HO·		［32］
	光活化	UV	BPA	HO·、CO $3 · -$		［33］
	其他	V(Ⅳ)	苯胺	HO·、O $2 · -$ 、CO₃·^-	O $2 · -$ 、CO $3 · -$	［36］
	其他	VOSO₄	苯胺	HO·、O $2 · -$ 、CO₃·^-	O $2 · -$ 、CO $3 · -$	［37］
PMC	过渡金属	Co²⁺	MB	HO·	HO·	［42］
		Co²⁺	AOⅡ	加密HO·	加密HO·	［43］
		Co²⁺	AOⅡ	HO·、O $2 · -$	HO·	［48］
		Cu(Ⅱ)	AOⅡ	HO·、O $2 · -$ 、¹O₂	Cu（Ⅲ）	［12］
		Cu(Ⅱ)	TCS	O $2 · -$ 、HO·	O $2 · -$ 、HO·	［45］
	金属复合材料	S-CoFe₂O₄	AOⅡ	加密HO·	加密HO·	［8］
		CoMgAl	MO	HO·、O $2 · -$	HO·、O $2 · -$	［41］
		CuFeS₂	2,4-DCP	HO·、¹O₂、O $2 · -$ 、CO $3 · -$	HO·、¹O₂、O $2 · -$	［46］
		Co _x Mn_3-_x O₄	2,4-DCP	HO·、O $2 · -$ 、CO $3 · -$ 、¹O₂	HO·、O $2 · -$ 、CO $3 · -$	［47］

体系	活化类型	活化剂	污染物	体系中自由基种类	起主要作用的物质	参考文献
SPC	铁基材料	Fe(Ⅱ)	SMX	HO·、O $2 · -$	HO·	［23］
		Fe(Ⅱ)	PCE			［53］
		Fe(Ⅱ)	苯			［54］
		Fe(Ⅱ)	四环素			［59］
		Fe(Ⅲ)	苯			［61］
		螯合剂-Fe²⁺	TCE			［18］
		Fe(Ⅱ)-CA	TCE			［49］
		Fe(Ⅱ)-OA	PCE			［51］
		FA/Fe(Ⅱ)	CT	HO·、CO $2 · -$	CO $2 · -$	［55］
	生物炭材料	富含Fe、Mn的生物炭	PAHs	O $2 · -$ 、HO·	HO·	［30］
	光活化	UV	BP-3	HO·		［32］
	光活化	UV	BPA	HO·、CO $3 · -$		［33］
	其他	V(Ⅳ)	苯胺	HO·、O $2 · -$ 、CO₃·^-	O $2 · -$ 、CO $3 · -$	［36］
	其他	VOSO₄	苯胺	HO·、O $2 · -$ 、CO₃·^-	O $2 · -$ 、CO $3 · -$	［37］
PMC	过渡金属	Co²⁺	MB	HO·	HO·	［42］
		Co²⁺	AOⅡ	加密HO·	加密HO·	［43］
		Co²⁺	AOⅡ	HO·、O $2 · -$	HO·	［48］
		Cu(Ⅱ)	AOⅡ	HO·、O $2 · -$ 、¹O₂	Cu（Ⅲ）	［12］
		Cu(Ⅱ)	TCS	O $2 · -$ 、HO·	O $2 · -$ 、HO·	［45］
	金属复合材料	S-CoFe₂O₄	AOⅡ	加密HO·	加密HO·	［8］
		CoMgAl	MO	HO·、O $2 · -$	HO·、O $2 · -$	［41］
		CuFeS₂	2,4-DCP	HO·、¹O₂、O $2 · -$ 、CO $3 · -$	HO·、¹O₂、O $2 · -$	［46］
		Co _x Mn_3-_x O₄	2,4-DCP	HO·、O $2 · -$ 、CO $3 · -$ 、¹O₂	HO·、O $2 · -$ 、CO $3 · -$	［47］

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