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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

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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
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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
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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.
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    • 参考文献(23)
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出版历程
  • 收稿日期:  2023-09-28
  • 网络出版日期:  2024-03-08

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