零价铁活化过氧乙酸降解水中双酚A的效果与机制

doi:10.11949/0438-1157.20231341

摘要/Abstract

摘要：

双酚A（BPA）是含酚工业废水中代表性污染物，采用零价铁（ZVI）活化过氧乙酸（PAA）去除水中BPA，探究了ZVI和PAA投量、pH值以及工业废水中典型共存阴离子对PAA活化和BPA降解的影响，并通过探究反应活性物种和活性位点解析了ZVI活化PAA的反应机制。在投加50 mg/L ZVI， 1 mM PAA和初始pH为3.4的最优工艺条件下，ZVI/PAA体系反应30 min可去除水中99.24%的BPA；HCO₃^-和SO₄^2-对BPA降解具有抑制作用，Cl^-（0 - 20.0 mM）则加速BPA降解。反应中ZVI及其表面氧化层分别释放溶解性Fe（II）和Fe（III），溶出的Fe（II）活化PAA贡献26.46%的BPA降解，非均相ZVI活化PAA对BPA降解起主要作用；淬灭实验表明，ZVI/PAA体系存在CH₃C（O）OO•、CH₃C（O）O•、•OH和Fe^IVO²⁺，其中CH₃C（O）OO•和Fe^IVO²⁺是降解BPA的主要活性物种。本研究为工业废水中双酚A的有效去除提供理论和数据支撑。

关键词: 含酚废水, 双酚A, 过氧乙酸, 零价铁, 高级氧化

Abstract:

Bisphenol A (BPA) is a representative pollutant in phenolic industrial wastewater. Zero valent iron (ZVI) was used to activate peroxyacetic acid (PAA) to remove BPA from water. The effects of ZVI and PAA dosage, pH value, and typical coexisting anions in industrial wastewater on PAA activation and BPA degradation were investigated, and the reaction mechanism of ZVI activation of PAA was analyzed by exploring the reactive species and active sites. Under the optimal process conditions of adding 50 mg/L ZVI, 1 mM PAA and an initial pH of 3.4, the ZVI/PAA system can remove 99.24% of BPA in water for 30 minutes. HCO₃^- and SO₄^2- showed inhibitory effects on BPA degradation, while Cl^- (0 - 20.0 mM) accelerated the degradation of BPA in ZVI/PAA system. Soluble Fe(II) and Fe(III) were released from ZVI and its surface oxide layer, respectively, during the reaction. The released Fe(II) activation of PAA contributed 26.46% of BPA degradation, while heterogeneous ZVI activation of PAA played a major role in BPA degradation. Scavenging experiment showed that CH₃C(O)OO•, CH₃C(O)O•, •OH and Fe^IVO²⁺ were produced in ZVI/PAA system, among which CH₃C(O)OO• and Fe^IVO²⁺ were the major reactive species contributing to BPA degradation. This study provided data and theoretical support for the effective removal of bisphenol A in industrial wastewater.

Key words: phenolic wastewater, bisphenol A, peroxyacetic acid, zero valent iron, advanced oxidation processes

中图分类号:

TE 991

李琢宇, 金鹏, 陈孝彦, 赵泽玉, 王庆宏, 陈春茂, 詹亚力. 零价铁活化过氧乙酸降解水中双酚A的效果与机制[J]. 化工学报, DOI: 10.11949/0438-1157.20231341.

Zhuoyu LI, Peng JIN, Xiaoyan CHEN, Zeyu ZHAO, Qinghong WANG, Chunmao CHEN, Yali ZHAN. Effect and mechanism on the degradation of aqueous bisphenol A by zero valent iron activated peroxyacetic acid system[J]. CIESC Journal, DOI: 10.11949/0438-1157.20231341.

图/表 13

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		BPA		PAA
		k_obs (min^-1)	R²	k_obs (min^-1)	R²
ZVI浓度 (mg/L)	0	0.0014	0.7915	0.0030	0.8333
	25	0.0549	0.9994	0.0195	0.9835
	50	0.1658	0.9909	0.0776	0.8932
	75	0.2942	0.9722	0.2358	0.8677
	100	0.4630	0.9919	0.4978	0.8877
PAA浓度 (mM)	0	0.0029	0.7982	-	-
	0.10	0.0226	0.9227	0.0443	0.9950
	0.25	0.0653	0.9711	0.0907	0.9864
	1.00	0.1658	0.9909	0.0776	0.8932
	2.00	0.1168	0.9967	0.0305	0.9981
pH值	3.0	0.1104	0.9167	0.3233	0.7890
	4.0	0.1171	0.9364	0.3908	0.9155
	5.0	0.0353	0.9813	0.0471	0.9684
	6.0	0.0094	0.919	0.0076	0.9836
	7.0	0.0029	0.6745	0.0117	0.9408
	8.0	0.0021	0.7382	0.0104	0.9782
Cl^-浓度 (mM)	0.0	0.1658	0.9909	0.0776	0.8932
	0.2	0.1725	0.9986	0.0767	0.9727
	0.5	0.2866	0.9961	0.2192	0.8798
	1.0	0.2662	0.974	0.2388	0.9131
	2.0	0.2678	0.9787	0.2942	0.9267
	5.0	0.2795	0.9832	0.2134	0.8857
	10.0	0.3197	0.9954	0.2605	0.8823
	20.0	0.3465	0.978	0.2987	0.9484
HCO₃^-浓度 (mM)	0.0	0.1658	0.9909	0.0776	0.8932
	0.2	0.0658	0.9953	0.0272	0.9815
	0.5	0.0364	0.9910	0.0168	0.9889
	1.0	0.0082	0.8913	0.0087	0.8600
	2.0	0.0053	0.9704	0.0088	0.9176
	5.0	0.0023	0.9777	0.0072	0.8708
	10.0	0.0022	0.9104	0.0152	0.9843
	20.0	0.0006	0.3193	0.0239	0.9969
SO₄^2-浓度 (mM)	0.0	0.1658	0.9909	0.0776	0.8932
	0.2	0.1205	0.9890	0.0363	0.9868
	0.5	0.1347	0.9939	0.0622	0.9560
	1.0	0.1195	0.9917	0.0417	0.9867
	2.0	0.0819	0.9961	0.0333	0.9958
	5.0	0.0730	0.9950	0.0305	0.9995
	10.0	0.0923	0.9946	0.0522	0.9883
	20.0	0.0803	0.9985	0.0512	0.9883

		BPA		PAA
		k_obs (min^-1)	R²	k_obs (min^-1)	R²
ZVI浓度 (mg/L)	0	0.0014	0.7915	0.0030	0.8333
	25	0.0549	0.9994	0.0195	0.9835
	50	0.1658	0.9909	0.0776	0.8932
	75	0.2942	0.9722	0.2358	0.8677
	100	0.4630	0.9919	0.4978	0.8877
PAA浓度 (mM)	0	0.0029	0.7982	-	-
	0.10	0.0226	0.9227	0.0443	0.9950
	0.25	0.0653	0.9711	0.0907	0.9864
	1.00	0.1658	0.9909	0.0776	0.8932
	2.00	0.1168	0.9967	0.0305	0.9981
pH值	3.0	0.1104	0.9167	0.3233	0.7890
	4.0	0.1171	0.9364	0.3908	0.9155
	5.0	0.0353	0.9813	0.0471	0.9684
	6.0	0.0094	0.919	0.0076	0.9836
	7.0	0.0029	0.6745	0.0117	0.9408
	8.0	0.0021	0.7382	0.0104	0.9782
Cl^-浓度 (mM)	0.0	0.1658	0.9909	0.0776	0.8932
	0.2	0.1725	0.9986	0.0767	0.9727
	0.5	0.2866	0.9961	0.2192	0.8798
	1.0	0.2662	0.974	0.2388	0.9131
	2.0	0.2678	0.9787	0.2942	0.9267
	5.0	0.2795	0.9832	0.2134	0.8857
	10.0	0.3197	0.9954	0.2605	0.8823
	20.0	0.3465	0.978	0.2987	0.9484
HCO₃^-浓度 (mM)	0.0	0.1658	0.9909	0.0776	0.8932
	0.2	0.0658	0.9953	0.0272	0.9815
	0.5	0.0364	0.9910	0.0168	0.9889
	1.0	0.0082	0.8913	0.0087	0.8600
	2.0	0.0053	0.9704	0.0088	0.9176
	5.0	0.0023	0.9777	0.0072	0.8708
	10.0	0.0022	0.9104	0.0152	0.9843
	20.0	0.0006	0.3193	0.0239	0.9969
SO₄^2-浓度 (mM)	0.0	0.1658	0.9909	0.0776	0.8932
	0.2	0.1205	0.9890	0.0363	0.9868
	0.5	0.1347	0.9939	0.0622	0.9560
	1.0	0.1195	0.9917	0.0417	0.9867
	2.0	0.0819	0.9961	0.0333	0.9958
	5.0	0.0730	0.9950	0.0305	0.9995
	10.0	0.0923	0.9946	0.0522	0.9883
	20.0	0.0803	0.9985	0.0512	0.9883

AOP的种类	反应条件	BPA降解情况	活性物种	共存阴离子影响	参考文献
VUV/H₂O₂	[H₂O₂] = 25 mg/L，[BPA] = 100 mg/L，pH = 3.0	60 min降解97.6%	•OH	100 mg/L HCO₃^-、Cl^-、NO₃^-、SO₄^2-对BPA的降解无明显影响	^[40]
Fe(IV)/H₂O₂	[Fe(VI)] = 250 µg/L，[H₂O₂] = 2.5 mg/L，[BPA] = 50 µg/L，pH = 8.0	60 min降解99.8%	Fe(V)、Fe(IV)、•OH、O^•-	350 µg/L Cl^-、NO₃^-对BPA的降解无明显影响，PO₄^3-（350 µg/L）显著抑制BPA的降解	^[41]
CuO/还原氧化石墨烯泡沫（RGF）/PDS	[CuO/RGF] = 0.5 g/L，[PDS] = 0.1 g/L，[BPA] = 10 mg/L，pH = 7.0	120 min吸附48.97%，后120 min降解37.13%	¹O₂、•OH、SO₄^•-	12 mg/L HCO₃^-抑制BPA的降解，Cl^-对BPA的降解无明显影响	^[42]
可见光（VL）/没食子酸（GA）/Fe³⁺/PI	[Fe³⁺] = 0.10 mM，[GA] = 0.10 mM，[PI] = 1 mM，[BPA] = 20 μM，pH = 7.0	30 min降解100%	¹O₂、•OH、O₂^•-、•IO₃、•IO₄、Fe(IV)	10 mM Cl^-、NO₃^-、SO₄^2-对BPA的降解无明显影响HCO₃^-抑制BPA的降解	^[43]
介质阻挡放电（DBD）/PAA	[输入功率] = 445 W，[液体流速] = 100 mL/min，[频率] = 3500 Hz，[PAA] = 3.0 mM，[BPA] = 40 µg/L，pH = 4.5	15 min降解93.4%	•OH、CH₃C(O)OO•、¹O₂、O₂^•-、e^-	10 mM Cl^-、SO₄^2-对BPA的降解无明显影响，HCO₃^-显著抑制BPA的降解	^[44]
ZIF-67/PAA	[HP] = 16.9 mM，[ZIF-67] = 0.1 g/L，[PAA] = 5 mM， [BPA] = 0.1 mM，pH = 3.4	30 min降解93.0%	R-O•、•OH、Co³⁺	10 mM Cl^-略微促进BPA的降解，NO₃^-、SO₄^2-对BPA的降解无明显影响，HCO₃^-显著抑制BPA的降解	^[45]
CuCo₂O₄/PAA	[CuCo₂O₄] = 0.2 g/L，[PAA] = 400 µM，[BPA] = 0.088 mM，pH = 7.0	60 min降解92.3%	¹O₂、R-O•	2 mM HCO₃^-、CO₃^2-、Cl^-略微抑制BPA的降解，NO₃^-、SO₄^2-对BPA的降解无明显影响	^[46]
ZVI/PAA	[ZVI] = 50 mg/L，[PAA] = 1 mM，[BPA] = 10 mg/L，pH = 3.4	30 min降解99.24%	R-O•、•OH、Fe(IV)	20 mM Cl^-显著促进BPA的降解，HCO₃^-显著抑制BPA的降解，SO₄^2-抑制BPA的降解	本实验

AOP的种类	反应条件	BPA降解情况	活性物种	共存阴离子影响	参考文献
VUV/H₂O₂	[H₂O₂] = 25 mg/L，[BPA] = 100 mg/L，pH = 3.0	60 min降解97.6%	•OH	100 mg/L HCO₃^-、Cl^-、NO₃^-、SO₄^2-对BPA的降解无明显影响	^[40]
Fe(IV)/H₂O₂	[Fe(VI)] = 250 µg/L，[H₂O₂] = 2.5 mg/L，[BPA] = 50 µg/L，pH = 8.0	60 min降解99.8%	Fe(V)、Fe(IV)、•OH、O^•-	350 µg/L Cl^-、NO₃^-对BPA的降解无明显影响，PO₄^3-（350 µg/L）显著抑制BPA的降解	^[41]
CuO/还原氧化石墨烯泡沫（RGF）/PDS	[CuO/RGF] = 0.5 g/L，[PDS] = 0.1 g/L，[BPA] = 10 mg/L，pH = 7.0	120 min吸附48.97%，后120 min降解37.13%	¹O₂、•OH、SO₄^•-	12 mg/L HCO₃^-抑制BPA的降解，Cl^-对BPA的降解无明显影响	^[42]
可见光（VL）/没食子酸（GA）/Fe³⁺/PI	[Fe³⁺] = 0.10 mM，[GA] = 0.10 mM，[PI] = 1 mM，[BPA] = 20 μM，pH = 7.0	30 min降解100%	¹O₂、•OH、O₂^•-、•IO₃、•IO₄、Fe(IV)	10 mM Cl^-、NO₃^-、SO₄^2-对BPA的降解无明显影响HCO₃^-抑制BPA的降解	^[43]
介质阻挡放电（DBD）/PAA	[输入功率] = 445 W，[液体流速] = 100 mL/min，[频率] = 3500 Hz，[PAA] = 3.0 mM，[BPA] = 40 µg/L，pH = 4.5	15 min降解93.4%	•OH、CH₃C(O)OO•、¹O₂、O₂^•-、e^-	10 mM Cl^-、SO₄^2-对BPA的降解无明显影响，HCO₃^-显著抑制BPA的降解	^[44]
ZIF-67/PAA	[HP] = 16.9 mM，[ZIF-67] = 0.1 g/L，[PAA] = 5 mM， [BPA] = 0.1 mM，pH = 3.4	30 min降解93.0%	R-O•、•OH、Co³⁺	10 mM Cl^-略微促进BPA的降解，NO₃^-、SO₄^2-对BPA的降解无明显影响，HCO₃^-显著抑制BPA的降解	^[45]
CuCo₂O₄/PAA	[CuCo₂O₄] = 0.2 g/L，[PAA] = 400 µM，[BPA] = 0.088 mM，pH = 7.0	60 min降解92.3%	¹O₂、R-O•	2 mM HCO₃^-、CO₃^2-、Cl^-略微抑制BPA的降解，NO₃^-、SO₄^2-对BPA的降解无明显影响	^[46]
ZVI/PAA	[ZVI] = 50 mg/L，[PAA] = 1 mM，[BPA] = 10 mg/L，pH = 3.4	30 min降解99.24%	R-O•、•OH、Fe(IV)	20 mM Cl^-显著促进BPA的降解，HCO₃^-显著抑制BPA的降解，SO₄^2-抑制BPA的降解	本实验

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