北京大学学报自然科学版 ›› 2018, Vol. 54 ›› Issue (4): 815-827.DOI: 10.13209/j.0479-8023.2017.188

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载钛羟基磷灰石对水中EE2光催化降解规律及途径研究

鞠传伦1,2, 张健伟1,2, 孙卫玲1,2,†, 若村正人3, 塚田峰春3, 佐佐正名4   

  1. 1. 深圳市重金属污染控制与资源化重点实验室, 北京大学深圳研究生院环境与能源学院, 深圳 518055
    2. 水沙科学教育部重点实验室, 北京大学环境科学与工程学院, 北京 100871
    3. 富士通研究所环境能源研究中心, 日本神奈川县厚木市243-0000
    4. 富士通研究开发中心有限公司, 北京 100025
  • 收稿日期:2017-03-20 修回日期:2017-05-09 出版日期:2018-07-20 发布日期:2018-07-20
  • 通讯作者: 孙卫玲, E-mail: wlsun(at)pku.edu.cn
  • 基金资助:
    日本富士通研究所环境能源研究中心基金(k120400)资助

Photocatalytic Degradation and Reaction Pathway of EE2 in Aqueous Solution by TiHAP

JU Chuanlun1,2, ZHANG Jianwei1,2, SUN Weiling1,2,†, Wakamurac Masato3, Tsukadad Mineharu3, Sasa Masaaki4   

  1. 1. Shenzhen Key Laboratory for Heavy Metal Pollution Control and Reutilization, School of Environment and Energy, Peking University Shenzhen Graduate School, Shenzhen 518055
    2. Key Laboratory of Water and Sediment Sciences (MOE), Department of Environmental Engineering, Peking University, Beijing 100871
    3. Fujitsu Laboratories Limited, Atsugi 243-0000
    4. Fujitsu Research and Development Center Company Limited, Beijing 100025
  • Received:2017-03-20 Revised:2017-05-09 Online:2018-07-20 Published:2018-07-20
  • Contact: SUN Weiling, E-mail: wlsun(at)pku.edu.cn

摘要:

以 17α-乙炔雌二醇(EE2)为目标污染物, 以载钛羟基磷灰石(TiHAP)为催化剂, 对比研究TiHAP和TiO2对EE2的光催化规律、影响因素及机理, 分析光催化降解的中间产物及降解途径。实验结果表明, TiHAP薄膜对EE2的降解速率高于TiO2薄膜; 随着Fe3+浓度增加, TiHAP降解EE2的速率没有明显变化, TiO2降解EE2的速率则先增加后减小; 随着富里酸(FA) 浓度的增加, TiHAP降解EE2的速率减小, 而TiO2降解EE2的速率升高。用LC-MSn对TiHAP光催化降解EE2过程中产生的中间产物进行分析, 在中性pH条件下共确定9种降解产物, 比同样pH值下以TiO2为催化剂检出的产物种类多, 推断其降解的主要途径是苯环羟基化、开环羧基化以及脱羧等一系列反应。

关键词: 载钛羟基磷灰石, 17α-乙炔雌二醇, 光催化降解

Abstract:

Selecting 17α-ethynylestradiol (EE2) as the target pollutant and TiHAP as the catalyst, comparative studies of the photocatalytic degradation of TiHAP and TiO2 were conducted, and the influencing factors and intermediate products were also investigated. The results show that the EE2 degradation rate by TiHAP film was faster than that by TiO2 film. The EE2 degradation rate of TiHAP remained the same with the increase of Fe3+ concentration, but decreased with the increase of FA concentration. For TiO2, the EE2 degradation rate initially increased and then decreased with increasing Fe3+ concentration, and increased with increasing FA concentration. The photocatalitic degradation intermediates of EE2 by TiHAP were identified by LC-MSn. The results show that nine kinds of intermediates were identified. Compared with TiO2, more kinds of intermediates were identified for EE2 photocatalytic degradation by TiHAP. Transformation of the phenolic moiety, hydroxylation, ring opening and carboxylation, and carboxylation were the primary reaction pathways.

Key words: TiHAP, EE2, photocatalysis

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