Removal of bisphenol A in water by iron-manganese co-oxide film and its influencing factors

doi:10.16085/j.issn.1000-6613.2020-0828

Abstract

Abstract:

Previous studies have found that the iron-manganese co-oxide film on the surface of the quartz sand has a high catalytic oxidation capacity for the removal of ammonium and manganese in water. In this study, two pilot-scale filter columns were used to study the removal of bisphenol A (BPA) by the ripening filters, and how the loading change of Mn²⁺ affected the removal of BPA was also investigated. The results showed that 0.48mg/L of BPA was removed with 95.6% of the removal efficiency of BPA and 5.44mg/L of consumed dissolved oxygen (DO). When the Mn²⁺ in influent was about 2.0mg/L, 0.56mg/L of BPA was removed in the 65cm depth of the filter column, and the concentration of BPA did not change obviously in the rest layers of the filter. From scanning electron microscope (SEM), some substance was generated after the oxidation of BPA, which was blocked in the pore structure of the oxide film, causing the compaction of the filter material. At the same time, a small amount of oxide film was found to crack and fall off. Energy dispersive spectrometer (EDS) spectrum indicated that the content increased from 12.14% to 21.10% for C and from 18.50% to 22.58% for O, respectively, but the Mn on the film surface decreases from 63.18% to 42.49%. The reduced manganese substance on the film surface may lead to the decrease in removal of BPA. X-ray Photoelectron Spectroscopy (XPS) energy spectrum showed that the main chemical forms of the oxide film were Mn₃O₄ and MnFe₂O₄, and the presence of [—CH₂—H(OH)]_n covered and blocked the dense porous pores of the film after dosing BPA, which was the main reason for the decrease in the removal efficiency of BPA.

Key words: iron-manganese co-oxide film, bisphenol A, catalytic oxidation, manganese

摘要：

前期研究已发现表面负载铁锰氧化膜的石英砂滤料，对水中常见污染物（氨氮、铁、锰等）具有较高的催化氧化能力。本文利用中试过滤系统研究成熟滤料对水中双酚A（BPA）的去除能力，同时考察进水中Mn²⁺的负荷变化对去除水中BPA的影响。结果表明：该系统在仅有BPA负荷时，可去除ΔC_BPA为0.48mg/L，去除率高达95.6%，消耗溶解氧（DO）为5.44mg/L；进水中同时投加BPA和Mn²⁺，当Mn²⁺浓度达到2.0mg/L时，在滤柱前65cm处即可去除ΔC_BPA为0.56mg/L，BPA在后半段无法有效去除。由扫描电子显微镜（SEM）可知，BPA氧化后生成了某种物质，阻塞在氧化膜的孔隙结构中，造成滤料板结，同时发现少许氧化膜裂开脱落；能谱仪（EDS）能谱图显示投加BPA后，C、O元素的含量分别由之前的12.14%、18.50%增加到21.10%、22.58%，而Mn元素由之前的63.18%减少至42.49%，导致氧化膜表面锰氧化物减少；X射线光电子能谱（XPS）能谱图显示，在不同阶段氧化膜的主要化学形态为Mn₃O₄和MnFe₂O₄，而投加BPA后，有机物[—CH₂—H(OH)]_n覆盖在氧化膜表面及空隙中，降低了氧化膜表面的有效活性位，导致了BPA去除效果下降。

关键词: 铁锰氧化膜, 双酚A, 催化氧化, 锰

CLC Number:

X523

HUANG Jianxiong, GUO Yingming, YANG Jing, XU Wei, WANG Xu, ZHANG Ruifeng. Removal of bisphenol A in water by iron-manganese co-oxide film and its influencing factors[J]. Chemical Industry and Engineering Progress, 2021, 40(3): 1551-1557.

黄建雄, 郭英明, 杨靖, 许伟, 王旭, 张瑞峰. 铁锰复合氧化膜对水中双酚A的去除及影响因素[J]. 化工进展, 2021, 40(3): 1551-1557.

Figures/Tables 7

References 24

1	程光. 环糊精聚合材料去除水中染料及内分泌干扰物的研究[D]. 上海: 华东理工大学, 2019.
	CHENG G. Study on removal of dyes and endocrine disruptors in water by cyclodextrins polymeric materials[D]. Shanghai: East China University of Science and Technology, 2019.
2	CHEN D, KANNAN K, TAN H, et al. Bisphenol analogues other than BPA: environmental occurrence, human exposure, and toxicity—a review[J]. Environmental Science & Technology, 2016, 50(11): 5438-5453.
3	BIGNARDI C, CAVAZZA A, LAGANA C, et al. UHPLC high resolution mass spectrometry determination of bisphenol A and plastic additives released by polycarbonate tableware: influence of ageing and surface damage[J]. Analytical and Bioanalytical Chemistry, 2015, 407(26): 7917-7924.
4	陈玫宏, 郭敏, 徐怀洲, 等. 太湖表层水体及沉积物中双酚A类似物的分布特征及潜在风险[J]. 环境科学, 2017, 38(7): 2793-2800.
	CHEN M H, GUO M, XU H Z, et al. Distribution characteristics and potential risk of bisphenol analogues in surface water and sediments of Lake Taihu[J]. Environmental Science, 2017, 38(7): 2793-2800.
5	ZHANG L, WANG W Z, SUN S M, et al. Elimination of BPA endocrine disruptor by magnetic BiOBr@SiO₂@Fe₃O₄ photocatalyst[J]. Applied Catalysis B: Environmental, 2014, 148: 164-169.
6	刘畅, 黄雅丹, 张莹, 等. 培养条件下双酚A对稻田土壤微生物群落特征的影响[J]. 环境科学, 2016, 37(11): 4380-4388.
	LIU C, HUANG Y D, ZHANG Y, et al. Effects of bisphenol A on characteristics of paddy soil microbial community under different cultural conditions[J]. Environmental Science, 2016, 37(11): 4380-4388.
7	NOTARDONATO I, RUSSO M V, AVINO P. Phthalates and bisphenol A residues in water samples: an innovative analytical approach[J]. Rendiconti Lincei-Scienze Fisiche E Naturali, 2018, 29(4): 831-840.
8	叶圣杰. 基于纳米材料或适配体的修饰电极检测从食品包装材料迁移的双酚A[D]. 福州: 福建师范大学, 2018.
	YE S J. Detection of bisphenol A from food packaging materials based on nanomaterial or aptamer modified electrode[D]. Fuzhou: Fujian Normal University, 2018.
9	HU L, ZHANG G, WANG Q, et al. Facile synthesis of novel Co₃O₄-Bi₂O₃catalysts and their catalytic activity on bisphenol A by peroxymonosulfate activation[J]. Chemical Engineering Journal, 2017, 326: 1095-1104.
10	张塞, 邹英桐, 陈中山, 等. 可见光驱动RGO/g-C₃N₄活化过硫酸盐降解水中双酚A[J]. 无机材料学报, 2020, 35(3): 329-336.
	ZHANG S, ZOU Y T, CHEN Z S, et al. Visible-light-driven activation of persulfate by RGO/g-C₃N₄ composites for degradation of BPA in wastewater[J]. Journal of Inorganic Materials, 2020, 35(3): 329–336.
11	李蒋, 王雁, 张秀芳, 等.Co₃O₄/BiVO₄复合阳极活化过一硫酸盐强化光电催化降解双酚A[J]. 环境科学, 2018, 39(8): 3713-3718.
	LI J, WANG Y, ZHANG X F, et al. Enhancement of photoelectrocatalytic degradation of bisphenol A with peroxymonosulfate activated by a Co₃O₄/BiVO₄ composite photoanode[J]. Environmental Science, 2018, 39(8): 3713-3718.
12	XU L, YANG L, JOHANSSON E M J, et al. Photocatalytic activity and mechanism of bisphenol a removal over TiO_2-_x/rGO nanocomposite driven by visible light[J]. Chemical Engineering Journal, 2018, 350: 1043-1055.
13	郭婷婷, 杨艳玲, 李星, 等. 膜滤特性对混凝–超滤组合去除双酚A的影响[J]. 水处理技术, 2019, 45(5): 38-41.
	GUO T T, YANG Y L, LI X, et al. Effect of filtration characteristics on bisphenol A removal by coagulation ultrafiltration combination[J]. Technology of Water Treatment, 2019, 45(5): 38-41.
14	LI C, LU Q, YE J, et al. Metabolic and proteomic mechanism of bisphenol A degradation by Bacillus thuringiensis[J]. Science of the Total Environment, 2018, 640/641: 714-725.
15	GUO Y M, HUANG T L, WEN G, et al. The simultaneous removal of ammonium and manganese from groundwater by iron manganese co-oxide filter film: the role of chemical catalytic oxidation for ammonium removal[J]. Chemical Engineering Journal, 2017, 308: 322-329.
16	CHENG Y, HUANG T L, SUN Y K, et al. Catalytic oxidation removal of ammonium from groundwater by manganese oxides filter: performance and mechanisms[J]. Chemical Engineering Journal, 2017, 322: 82-89.
17	国家环境保护总局. 水和废水监测分析方法[M]. 4版. 北京: 中国环境科学出版社, 2002: 370-372.
	SEPA. Analytical methods of water and wastewater[M]. 4th ed. Beijing: China Environmental Science Press, 2002: 370-372.
18	白筱莉, 黄廷林, 张瑞峰, 等. 铁锰复合氧化膜同步去除地表水中氨氮和锰[J]. 中国环境科学, 2017, 37(12): 4534-4540.
	BAI X L, HUANG T L, ZHANG R F, et al. The simultaneous removal of ammonium and manganese from surface water by iron-manganese co-oxides film[J]. China Environmental Science, 2017, 37(12): 4534-4540.
19	AUDI A A, SHERWOOD P M A. Valence-band X-ray photoelectron spectroscopic studies of manganese and its oxides interpreted by cluster and band structure calculations[J]. Surface and Interface Analysis, 2002, 33(3): 274–282.
20	JUNTA J L, HOCHELLA M F. Manganese (Ⅱ) oxidation at mineral surfaces: a microscopic and spectroscopic study[J]. Geochimica et Cosmochimica Acta, 1994, 58(22): 4985-4999.
21	SHCHUKAREV A, KOROLKOV D. XPS study of group ⅠA carbonates[J]. Central European Journal of Chemistry, 2004, 2(2): 347-362.
22	STOYANOV P, AKHTER S, WHITE J M. XPS study of metal/polymer interaction: evaporated aluminum on polyvinyl alcohol polymer[J]. Surface and Interface Analysis, 1990, 15(9): 509-515.
23	STROHMEIER B R, HERCULES D M. Surface spectroscopic characterization of manganese/aluminum oxide catalysts[J]. The Journal of Physical Chemistry, 1984, 88(21): 4922-4929.
24	NOHIRA H, TSAI W, BESLING W, et al. Characterization of ALCVD-Al₂O₃ and ZrO₂ layer using X-ray photoelectron spectroscopy[J]. Journal of Non-Crystalline Solids, 2002, 303(1): 83-87.

水质指标	单位	数值	地下水质量标准（GB/T 14848—2017）	水质指标	单位	数值	地下水质量标准（GB/T 14848—2017）
氨氮	mg·L^-1	0.018~0.022	≤0.50	溶解氧	mg·L^-1	7.07~8.22	—
硝态氮	mg·L^-1	3.862~4.103	≤20.0	COD_Mn	mg·L^-1	1.98~2.10	—
亚硝态氮	mg·L^-1	0~0.001	≤1.00	总硬度CaCO₃计	mg·L^-1	166~180	≤450
铁	mg·L^-1	0.051~0.062	≤0.30	温度	℃	15.2~18.1	—
锰	mg·L^-1	0~0.05	≤0.10	pH	—	7.2~7.6	6.5~8.5

水质指标	单位	数值	地下水质量标准（GB/T 14848—2017）	水质指标	单位	数值	地下水质量标准（GB/T 14848—2017）
氨氮	mg·L^-1	0.018~0.022	≤0.50	溶解氧	mg·L^-1	7.07~8.22	—
硝态氮	mg·L^-1	3.862~4.103	≤20.0	COD_Mn	mg·L^-1	1.98~2.10	—
亚硝态氮	mg·L^-1	0~0.001	≤1.00	总硬度CaCO₃计	mg·L^-1	166~180	≤450
铁	mg·L^-1	0.051~0.062	≤0.30	温度	℃	15.2~18.1	—
锰	mg·L^-1	0~0.05	≤0.10	pH	—	7.2~7.6	6.5~8.5

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