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Pd-Fe/C催化氯酚还原脱氯-氧化联合降解

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武雯, 于嘉文, 刘苏静, 刘莺, 马宣宣, 夏传海. Pd-Fe/C催化氯酚还原脱氯-氧化联合降解[J]. 环境化学, 2018, 37(11): 2522-2531. doi: 10.7524/j.issn.0254-6108.2018053001
引用本文: 武雯, 于嘉文, 刘苏静, 刘莺, 马宣宣, 夏传海. Pd-Fe/C催化氯酚还原脱氯-氧化联合降解[J]. 环境化学, 2018, 37(11): 2522-2531. doi: 10.7524/j.issn.0254-6108.2018053001
shu
WU Wen, YU Jiawen, LIU Sujing, LIU Ying, MA Xuanxuan, XIA Chuanhai. Remediation of chlorophenols by the combination of catalytic reductive dechlorination-oxidation over Pd-Fe/C catalyst[J]. Environmental Chemistry, 2018, 37(11): 2522-2531. doi: 10.7524/j.issn.0254-6108.2018053001
Citation: WU Wen, YU Jiawen, LIU Sujing, LIU Ying, MA Xuanxuan, XIA Chuanhai. Remediation of chlorophenols by the combination of catalytic reductive dechlorination-oxidation over Pd-Fe/C catalyst[J]. Environmental Chemistry, 2018, 37(11): 2522-2531. doi: 10.7524/j.issn.0254-6108.2018053001
shu

Pd-Fe/C催化氯酚还原脱氯-氧化联合降解

  • 1.

    鲁东大学滨海生态高等研究院, 烟台, 264025;

  • 2.

    鲁东大学资源与环境工程学院, 烟台, 264025

  • 基金项目:

    山东省高等学校优势学科人才团队培育计划"蓝黄两区滨海资源与环境"项目，山东省自然基金博士项目（ZR2017BD029），山东省高等学校科技计划项目（J18KA096），环境化学与生态毒理学国家重点实验室开放基金（KF2017-12），中国科学院海岸带环境过程与生态修复重点实验室（烟台海岸带研究所）开放基金资助（2018KFJJ07）和鲁东大学博士基金项目（LA2016010，LB2016039）资助.

Remediation of chlorophenols by the combination of catalytic reductive dechlorination-oxidation over Pd-Fe/C catalyst

  • 1.

    The institute of advanced study of coastal ecology, Ludong university, Yantai, 264025, China;

  • 2.

    School of resources and environmental engineering, Ludong university, Yantai, 264025, China

  • Fund Project: Supported by the Cultivation Plan of Superior Discipline Talent Teams of Universities in Shandong Province:"the Coastal Resources and Environment team for Blue-Yellow Area", Natural Science Foundation of Shandong Province of China (ZR2017BD029), A Project of Shandong Province Higher Educational Science and Technology Program (J18KA096), State Key Laboratory of Environmental Chemistry and Ecotoxicology, and Research Center for Eco-Environmental Sciences, CAS (KF2017-12), Key Laboratory of Coastal Environmental Processes and Ecological Remediation, YICCAS (2018KFJJ07) and Ph.D. Programs Foundation of Ludong University (LA2016010, LB2016039).

  • 摘要: 以Pd和Fe为活性金属组分通过沉积沉淀法制备了负载型Pd-Fe/C双金属催化剂，针对氯酚类污染物进行催化还原脱氯和催化氧化的连续降解处理.通过ICP-MS、XRD和TEM对催化剂进行表征，证实0.5% Pd-0.5% Fe/C催化剂中活性金属组分Pd和Fe在载体表面分散性最好，催化剂比表面积达到718.8 m2·g-1.在温和条件下，以水作为反应介质，研究了负载型Pd-Fe/C催化剂对4-氯苯酚（4-CP）和2，4-二氯苯酚（2，4-DCP）的连续降解过程和反应条件，以及催化剂的重复使用情况.考察了Pd和Fe的负载量及pH值对催化剂活性的影响，得到了最佳反应条件，以0.5% Pd-0.5% Fe/C为催化剂，20 min内完成4-CP和2，4-DCP的催化还原脱氯，产物都为苯酚；之后加酸调节pH=5，并加入H2O2继续进行催化氧化，苯酚被彻底降解为H2O和CO2，而且转化率在60 min内可以达到97.5%以上，从而实现4-CP和2，4-DCP的彻底降解.
    Abstract: A Pd-Fe/C bimetallic catalyst was prepared by deposition-precipitation method. For the remediation of chlorophenols, a combination of catalytic reductive dechlorination-oxidation over Pd-Fe/C bimetallic catalyst was carried out. Based on the analysis of ICP-MS, XRD, and TEM, it was found that the active metal components Pd and Fe in the 0.5% Pd-0.5% Fe/C catalyst exhibited the best dispersibility, and the specific surface area of the catalyst reached 718.8 m2·g-1. With water as the reaction medium, the continuous degradation process and reaction conditions of 4-chlorophenol (4-CP) and 2,4-dichlorophenol (2,4-DCP) over Pd-Fe/C catalyst under mild conditions were studied. Meanwhile, the reuse of Pd-Fe/C catalyst was also studied. The effects of Pd and Fe loadings and pH on the activity of the catalyst were investigated, and the optimum reaction conditions were obtained. With 0.5% Pd-0.5% Fe/C as the catalyst, 4-CP and 2,4-DCP were completely reductive dechlorinated and transformed into phenol within 20 min. After the reductive dechlorination, the pH was adjusted into 5 and H2O2 was added, and phenol was completely oxidized into H2O and CO2. Moreover, the conversion of phenol reached 97.5% within 60 min. Based on the above studies, the thorough degradation of 4-CP and 2,4-DCP could be achieved.
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  • 收稿日期:  2018-05-30
  • 刊出日期:  2018-11-15
武雯, 于嘉文, 刘苏静, 刘莺, 马宣宣, 夏传海. Pd-Fe/C催化氯酚还原脱氯-氧化联合降解[J]. 环境化学, 2018, 37(11): 2522-2531. doi: 10.7524/j.issn.0254-6108.2018053001
引用本文: 武雯, 于嘉文, 刘苏静, 刘莺, 马宣宣, 夏传海. Pd-Fe/C催化氯酚还原脱氯-氧化联合降解[J]. 环境化学, 2018, 37(11): 2522-2531. doi: 10.7524/j.issn.0254-6108.2018053001
shu
WU Wen, YU Jiawen, LIU Sujing, LIU Ying, MA Xuanxuan, XIA Chuanhai. Remediation of chlorophenols by the combination of catalytic reductive dechlorination-oxidation over Pd-Fe/C catalyst[J]. Environmental Chemistry, 2018, 37(11): 2522-2531. doi: 10.7524/j.issn.0254-6108.2018053001
Citation: WU Wen, YU Jiawen, LIU Sujing, LIU Ying, MA Xuanxuan, XIA Chuanhai. Remediation of chlorophenols by the combination of catalytic reductive dechlorination-oxidation over Pd-Fe/C catalyst[J]. Environmental Chemistry, 2018, 37(11): 2522-2531. doi: 10.7524/j.issn.0254-6108.2018053001
shu

Pd-Fe/C催化氯酚还原脱氯-氧化联合降解

  • 1.  鲁东大学滨海生态高等研究院, 烟台, 264025;
  • 2.  鲁东大学资源与环境工程学院, 烟台, 264025
  • 收稿日期:  2018-05-30
基金项目:

山东省高等学校优势学科人才团队培育计划"蓝黄两区滨海资源与环境"项目，山东省自然基金博士项目（ZR2017BD029），山东省高等学校科技计划项目（J18KA096），环境化学与生态毒理学国家重点实验室开放基金（KF2017-12），中国科学院海岸带环境过程与生态修复重点实验室（烟台海岸带研究所）开放基金资助（2018KFJJ07）和鲁东大学博士基金项目（LA2016010，LB2016039）资助.

摘要: 以Pd和Fe为活性金属组分通过沉积沉淀法制备了负载型Pd-Fe/C双金属催化剂，针对氯酚类污染物进行催化还原脱氯和催化氧化的连续降解处理.通过ICP-MS、XRD和TEM对催化剂进行表征，证实0.5% Pd-0.5% Fe/C催化剂中活性金属组分Pd和Fe在载体表面分散性最好，催化剂比表面积达到718.8 m2·g-1.在温和条件下，以水作为反应介质，研究了负载型Pd-Fe/C催化剂对4-氯苯酚（4-CP）和2，4-二氯苯酚（2，4-DCP）的连续降解过程和反应条件，以及催化剂的重复使用情况.考察了Pd和Fe的负载量及pH值对催化剂活性的影响，得到了最佳反应条件，以0.5% Pd-0.5% Fe/C为催化剂，20 min内完成4-CP和2，4-DCP的催化还原脱氯，产物都为苯酚；之后加酸调节pH=5，并加入H2O2继续进行催化氧化，苯酚被彻底降解为H2O和CO2，而且转化率在60 min内可以达到97.5%以上，从而实现4-CP和2，4-DCP的彻底降解.

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