中国科学引文数据库（CSCD）来源期刊
中国科技核心期刊
环境科学领域高质量科技期刊分级目录T2级期刊
RCCSE中国核心学术期刊
美国化学文摘社（CAS）数据库 收录期刊
日本JST China 收录期刊
世界期刊影响力指数（WJCI）报告 收录期刊

留言板

尊敬的读者、作者、审稿人, 关于本刊的投稿、审稿、编辑和出版的任何问题, 您可以本页添加留言。我们将尽快给您答复。谢谢您的支持!

姓名
邮箱
手机号码
标题
留言内容
验证码

钙钛矿LaBO3催化过氧乙酸降解水中双酚A机制研究

赵莹,  刘晴靓,  王硕,  孙志强,  马军

downloadPDF
文章导航 > 环境工程  > 2023 >  41(12): 1-10
赵莹, 刘晴靓, 王硕, 孙志强, 马军. 钙钛矿LaBO3催化过氧乙酸降解水中双酚A机制研究[J]. 环境工程, 2023, 41(12): 1-10. doi: 10.13205/j.hjgc.202312001
引用本文: 赵莹, 刘晴靓, 王硕, 孙志强, 马军. 钙钛矿LaBO3催化过氧乙酸降解水中双酚A机制研究[J]. 环境工程, 2023, 41(12): 1-10. doi: 10.13205/j.hjgc.202312001
shu
ZHAO Ying, LIU Qingliang, WANG Shuo, SUN Zhiqiang, MA Jun. MECHANISM OF PEROVSKITE LaBO3 CATALYZED PEROXYACETIC ACID DEGRADATION OF BISPHENOL A IN WATER[J]. ENVIRONMENTAL ENGINEERING , 2023, 41(12): 1-10. doi: 10.13205/j.hjgc.202312001
Citation: ZHAO Ying, LIU Qingliang, WANG Shuo, SUN Zhiqiang, MA Jun. MECHANISM OF PEROVSKITE LaBO3 CATALYZED PEROXYACETIC ACID DEGRADATION OF BISPHENOL A IN WATER[J]. ENVIRONMENTAL ENGINEERING , 2023, 41(12): 1-10. doi: 10.13205/j.hjgc.202312001
shu

钙钛矿LaBO3催化过氧乙酸降解水中双酚A机制研究

doi: 10.13205/j.hjgc.202312001

  • 1. 哈尔滨工业大学 城市水资源与水环境国家重点实验室, 哈尔滨 150090;

  • 2. 中国科学院生态环境研究中心, 北京 100085

基金项目: 

国家自然科学基金"基于过渡金属单原子活性中心设计定向调控过一硫酸盐对水中内分泌干扰物的降解机制"(52200010)

详细信息
    作者简介:

    赵莹(1994-),女,博士后,主要研究方向为水处理高级氧化技术。yzhao16@hit.edu.cn

    通讯作者:

    孙志强(1991-),男,副教授,主要研究方向为饮用水安全保障技术。sunhit@hit.edu.cn

    马军(1962-),男,中国工程院院士,教授,主要研究方向为饮用水安全保障技术。majun@hit.edu.cn

MECHANISM OF PEROVSKITE LaBO3 CATALYZED PEROXYACETIC ACID DEGRADATION OF BISPHENOL A IN WATER

  • 1. State Key Laboratory of Urban Water Resources and Water Environment, Harbin Institute of Technology, Harbin 150090, China;

  • 2. Ecological Environment Research Center of the Chinese Academy of Sciences, Beijing 100085, China

    摘要
  • 摘要: 为高效去除水中内分泌干扰物类污染物,采用溶胶-凝胶法合成钙钛矿LaBO3(B=Fe、Cr、Co)催化剂,用于催化过氧乙酸(PAA)降解水中双酚A(BPA)。采用TG-DSC、SEM、TEM、XRD等方法对钙钛矿LaBO3催化剂形貌及微观结构进行表征,研究其在不同条件下催化PAA去除BPA的效果,并提出催化PAA反应机制。结果表明:LaBO3(B=Fe、Cr、Co)为大小不一、表面光滑、团聚的不规则球体,比表面积为11.89 m2/g。研究条件下,LaCoO3/PAA体系对BPA的降解率高达85%,显著高于LaCrO3/PAA(14%)和LaFeO3/PAA(14%)体系。此外,LaCoO3/PAA体系对其他污染物(金橙Ⅰ、磺胺甲噁唑、4-氯苯酚)亦展现出良好的降解效果,并且对水中常见的无机阴离子和腐殖酸具有较强的抗干扰能力,使LaCoO3成为一种有发展前景的环境友好型催化剂。采用淬灭实验和电子自旋共振光谱揭示了有机自由基是LaCoO3/PAA体系导致BPA降解的主要活性物种。直接电子转移途径为LaCoO3/PAA体系催化降解BPA的次要氧化途径。此外,≡CoⅢ/≡CoⅡ的氧化还原对与PAA之间的氧化还原反应确保了自由基的连续生成和较高的降解效能。该研究工作可为水中内分泌干扰物污染治理提供新的思路。
    Abstract: To remove endocrine disruptors in water efficiently, perovskite LaBO3 (B=Fe, Cr, Co) catalyst was synthesized by sol-gel method to catalyze the degradation of bisphenol A (BPA) in water by peracetic acid (PAA). The morphology and microstructure of the catalyst were characterized using TG-DSC, SEM, TEM, XRD, etc. The effect of catalytic PAA removal of BPA under different conditions was studied, and the catalytic PAA reaction mechanism was proposed. The results indicated that LaBO3 (B=Fe, Cr, Co) was an irregular sphere with varying sizes, smooth surfaces, and aggregation. The specific surface area of LaCoO3 was 11.89 m2/g. BPA degradation could reach 85% in the LaCoO3/PAA system, significantly higher than that of LaCrO3/PAA (14%) and LaFeO3/PAA (14%) systems. In addition, the LaCoO3/PAA system also exhibited good degradation efficiency on other pollutants (orange I, sulfamethoxazole, 4-chlorophenol), and had strong anti-interference ability with common inorganic anions and humic acids in water, making LaCoO3 an environmentally friendly catalyst with promising development prospects. The quenching experiment combined with electron spin resonance spectroscopy revealed that organic radicals were the main active species causing BPA degradation in the LaCoO3/PAA system. The electron transfer pathway was the secondary oxidation pathway for the catalytic degradation of BPA in the LaCoO3/PAA system. In addition, the oxidation-reduction reaction between ≡CoⅢ/≡CoⅡ and PAA ensured the continuous generation of radicals and high degradation efficiency. This work can provide new insight into the treatment of endocrine disruptors in water pollution.
    • HTML全文
    • 参考文献(23)
  • [1] 尤洋,夏青,李文攀,等.建设项目中常见的内分泌干扰物的污染和控制建议[J].中国环境监测,2018,2:57-63.
    [2] 黄苑,张维,王瑞国,等.双酚类化合物污染现状和内分泌干扰效应研究进展[J].生态毒理学报,2022,17(1):60-81.
    [3] DA SILVA W P, CARLOS T D, CAVALLINI G S, et al. Peracetic acid: structural elucidation for applications in wastewater treatment[J]. Water Research,2020,168:115143.
    [4] LUUKKONEN T, HEYNINCK T, RÄMÖ J, et al. Comparison of organic peracids in wastewater treatment: disinfection, oxidation and corrosion[J]. Water Research,2015,85:275-285.
    [5] WANG Z, WANG J, XIONG B, et al. Application of cobalt/peracetic acid to degrade sulfamethoxazole at neutral condition: efficiency and mechanisms. Environmental Science & Technology,2020,54:464-475.
    [6] KIM J, ZHANG T, LIU W, et al. Advanced oxidation process with peracetic acid and Fe(Ⅱ) for contaminant degradation[J]. Environmental Science & Technology,2019,53:13312-13322.
    [7] LIANG P, MENG D, LIANG Y, et al. Cation deficiency tuned LaCoO3-δ perovskite for peroxymonosulfate activation towards bisphenol a degradation[J]. Chemical Engineering Journal,2021,409:128196.
    [8] MANOS D, MISERLI K, KONSTANTINOU I. Perovskite and spinel catalysts for sulfate radical-based advanced oxidation of organic pollutants in water and wastewater systems[J]. Catalysts,2020,10(11):1299.
    [9] CHEN C, ZHOU J, GENG J, et al. Perovskite LaNiO3/TiO2 step-scheme heterojunction with enhanced photocatalytic activity[J]. Applied Surface Science,2020,503:144287.
    [10] ZHOU X, WU H, ZHANG L, et al. Activation of peracetic acid with lanthanum cobaltite perovskite for sulfamethoxazole degradation under a neutral pH: the contribution of organic radicals[J]. Molecules,2020,25(12):2725.
    [11] ZHAO X, ZHANG T, ZHOU Y, et al. Preparation of peracetic acid from hydrogen peroxide: Part Ⅰ: kinetics for peracetic acid synthesis and hydrolysis[J]. Journal of Molecular Catalysis A: Chemical,2007,271:246-252.
    [12] PENG Z, LIANG P, WANG X, et al. Copper cadmium titanate prepared by different methods: phase formation, dielectric properties and relaxor behaviors[J]. Ceramics International,2018,44(7):7814-7823.
    [13] ZHUANG S, LIU Y, ZENG S, et al. A modified sol-gel method for low-temperature synthesis of homogeneous nanoporous La1-xSrxMnO3 with large specific surface area[J]. Journal of Sol-Gel Science and Technology,2016,77(1):109-118.
    [14] CHEN S, CAI M, LIU Y, et al. Effects of water matrices on the degradation of naproxen by reactive radicals in the UV/peracetic acid process[J]. Water Research,2019,150:153-161.
    [15] LIU B, GUO W, JIA W, et al. Insights into the oxidation of organic contaminants by Co(Ⅱ) activated peracetic acid: the overlooked role of high-valent cobalt-oxo species[J]. Water Research,2021,201:117313.
    [16] DENG J, WANG H, FU Y, et al. Phosphate-induced activation of peracetic acid for diclofenac degradation: kinetics, influence factors and mechanism[J]. Chemosphere,2022,287:132396.
    [17] YAO K, FANG L, LIAO P, et al. Ultrasound-activated peracetic acid to degrade tetracycline hydrochloride: efficiency and mechanism[J]. Separation and Purification Technology,2023,306:122635.
    [18] WANG J, XIONG B, MIAO L, et al. Applying a novel advanced oxidation process of activated peracetic acid by CoFe2O4 to efficiently degrade sulfamethoxazole[J]. Applied Catalysis B: Environmental,2021,280:119422.
    [19] ZHANG L, CHEN J, ZHENG T, et al. Co-Mn spinel oxides trigger peracetic acid activation for ultrafast degradation of sulfonamide antibiotics: unveiling critical role of Mn species in boosting Co activity[J]. Water Research,2023,229:119462.
    [20] KONG D, ZHAO Y, FAN X, et al. Reduced graphene oxide triggers peracetic acid activation for robust removal of micropollutants: the role of electron transfer[J]. Environmental Science & Technology,2022,56(16):11707-11717.
    [21] HAMMOUDA S B, ZHAO F, SAFAEI Z, et al. Degradation and mineralization of phenol in aqueous medium by heterogeneous monopersulfate activation on nanostructured cobalt based-perovskite catalysts ACoO3 (A=La, Ba, Sr and Ce): characterization, kinetics and mechanism study[J]. Applied Catalysis B: Environmental,2017,215:60-73.
    [22] WANG Y, JI H, LIU W, et al. Novel CuCo2O4 composite spinel with a meso-macroporous nanosheet structure for sulfate radical formation and benzophenone-4 degradation: interface reaction, degradation pathway, and DFT calculation[J]. ACS Applied Materials & Interfaces, 2020, 12(18):20522-20535.
    [23] ZENG W, YIN Z, GAO M, et al. In-situ growth of magnesium peroxide on the edge of magnesium oxide nanosheets: ultrahigh photocatalytic efficiency based on synergistic catalysis[J]. Journal of Colloid and Interface Science,2020,561:257-264.
    • 相关文章
    • 施引文献
  • 资源附件(0)
  • 加载中
WeChat 点击查看大图
计量
  • 文章访问数:  275
  • HTML全文浏览量:  16
  • PDF下载量:  36
  • 被引次数: 0
出版历程
  • 收稿日期:  2023-09-28
  • 网络出版日期:  2024-03-08

目录

    /

    返回文章
    返回

    期刊在线

    作者中心

    友情链接

    版权所有 ©《工业建筑》杂志社有限公司 京ICP备11033253号-1

    本系统由北京仁和汇智信息技术有限公司 设计开发   百度统计