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g-C3N4光催化降解2，4-DCP的活性及机理

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吴斌, 方艳芬, 任慧君, 赵萍, 黄应平. g-C3N4光催化降解2，4-DCP的活性及机理[J]. 环境化学, 2017, 36(7): 1484-1491. doi: 10.7524/j.issn.0254-6108.2017.07.2016102508
引用本文: 吴斌, 方艳芬, 任慧君, 赵萍, 黄应平. g-C3N4光催化降解2，4-DCP的活性及机理[J]. 环境化学, 2017, 36(7): 1484-1491. doi: 10.7524/j.issn.0254-6108.2017.07.2016102508
shu
WU Bin, FANG Yanfen, REN Huijun, ZHAO Ping, HUANG Yingping. Activity and mechanism of photocatalytic degradation for 2,4-DCP over g-C3N4[J]. Environmental Chemistry, 2017, 36(7): 1484-1491. doi: 10.7524/j.issn.0254-6108.2017.07.2016102508
Citation: WU Bin, FANG Yanfen, REN Huijun, ZHAO Ping, HUANG Yingping. Activity and mechanism of photocatalytic degradation for 2,4-DCP over g-C3N4[J]. Environmental Chemistry, 2017, 36(7): 1484-1491. doi: 10.7524/j.issn.0254-6108.2017.07.2016102508
shu

g-C3N4光催化降解2，4-DCP的活性及机理

  • 1.

    三峡大学水利与环境学院, 宜昌, 443002;

  • 2.

    三峡库区生态环境教育部工程研究中心(三峡大学), 宜昌, 443002;

  • 3.

    三峡地区地质灾害与生态环境湖北省协同创新中心(三峡大学), 宜昌, 443002

  • 基金项目:

    国家自然科学基金（21377067，21677086，21577078）， 湖北省创新群体项目（2015CFA021）和国家水专项子课题（2012ZX07104-003-04）资助.

Activity and mechanism of photocatalytic degradation for 2,4-DCP over g-C3N4

  • 1.

    College of Hydraulic &.Environmental Engineering, China Three Gorges University, Yichang, 443002, China;

  • 2.

    China Engineering Research Center of Eco-environment in Three Gorges Reservoir Region, Ministry of Education, China Three Gorges University, Yichang, 443002, China;

  • 3.

    Collaborative Innovation Center for Geo-Hazards and Eco-Environment in Three Gorges Area, China Three Gorges University, Yichang, 443002, China

  • Fund Project: Supported by National Natural Science Foundation of China (21377067,21677086,21577078),Hubei Innovation Group Project (2015CFA021) and the Special S & T Project on Treatment and Control of Water Pollution (2012ZX07104-003-04).

  • 摘要: 以三聚氰胺（Melamine）为原料，在高温条件下采用热缩合反应合成了石墨型氮化碳（g-C3N4）光催化剂.通过X-射线衍射（XRD）、扫描电镜（SEM）、紫外-可见漫反射光谱（UV-Vis DRS）、衰减全反射红外光谱（ATR-IR）等技术对其物理结构及性质进行了表征，结果表明实验制备的g-C3N4为片层状结构，比表面积为15.34 m2·g-1.在可见光（λ>420 nm）照射下，用g-C3N4降解有机小分子污染物2，4-二氯苯酚（2，4-Dichlorophenol，2，4-DCP），该过程反应符合一级动力学，反应速率常数为0.0113 min-1，以0.67 g·L-1的用量反应250 min后2，4-DCP矿化率达到60%；2，4-DCP在弱酸性条件下（pH=5.4）的降解效率最高；通过捕获实验及电子自旋共振（ESR）实验表明，超氧自由基（O2·-）是g-C3N4光催化降解2，4-DCP过程中的主要活性物种.2，4-DCP的降解路径主要涉及脱氯、苯环开环和碳链断裂等反应历程.
    Abstract: Graphite carbon nitride (g-C3N4) photocatalyst was synthesized via thermal condensation at high temperatures using melamine as a starting material. The structure and properties of the catalyst was characterized by scanning electron microscopy (SEM),X-ray diffraction (XRD),UV-Vis diffuse reflectance spectroscopy (UV-Vis DRS), and attenuated total reflection infrared spectroscopy (ATR-IR).The results indicate that the as-synthesized g-C3N4 had a layered structure with a specific surface area of 15.34 m2·g-1 and possed strong visible light absorption capacity. Photocatalytic degradation of 2,4-dichlorophenol (2,4-DCP) using g-C3N4 under visible light irradiation (λ>420 nm) corresponds to the first order kinetics with a reaction rate constant of 0.0113 min-1.After 250 min,the mineralization rate of 2,4-DCP in the presence of 0.67 g·L-1g-C3N4 reached 60%. The degradation efficiency of 2,4-DCP was highly enhanced in weak acid. Trapping experiments and electron spin resonance (ESR) experiments show that superoxide radical (O2·-) was the main active species in the photocatalytic degradation of 2,4-DCP.The main degradation pathways of 2,4-DCP include dechlorination,aromatic ring opening and carbon chain rupture.
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出版历程
  • 收稿日期:  2016-10-25
  • 刊出日期:  2017-07-15
吴斌, 方艳芬, 任慧君, 赵萍, 黄应平. g-C3N4光催化降解2，4-DCP的活性及机理[J]. 环境化学, 2017, 36(7): 1484-1491. doi: 10.7524/j.issn.0254-6108.2017.07.2016102508
引用本文: 吴斌, 方艳芬, 任慧君, 赵萍, 黄应平. g-C3N4光催化降解2，4-DCP的活性及机理[J]. 环境化学, 2017, 36(7): 1484-1491. doi: 10.7524/j.issn.0254-6108.2017.07.2016102508
shu
WU Bin, FANG Yanfen, REN Huijun, ZHAO Ping, HUANG Yingping. Activity and mechanism of photocatalytic degradation for 2,4-DCP over g-C3N4[J]. Environmental Chemistry, 2017, 36(7): 1484-1491. doi: 10.7524/j.issn.0254-6108.2017.07.2016102508
Citation: WU Bin, FANG Yanfen, REN Huijun, ZHAO Ping, HUANG Yingping. Activity and mechanism of photocatalytic degradation for 2,4-DCP over g-C3N4[J]. Environmental Chemistry, 2017, 36(7): 1484-1491. doi: 10.7524/j.issn.0254-6108.2017.07.2016102508
shu

g-C3N4光催化降解2，4-DCP的活性及机理

  • 1.  三峡大学水利与环境学院, 宜昌, 443002;
  • 2.  三峡库区生态环境教育部工程研究中心(三峡大学), 宜昌, 443002;
  • 3.  三峡地区地质灾害与生态环境湖北省协同创新中心(三峡大学), 宜昌, 443002
  • 收稿日期:  2016-10-25
基金项目:

国家自然科学基金（21377067，21677086，21577078）， 湖北省创新群体项目（2015CFA021）和国家水专项子课题（2012ZX07104-003-04）资助.

摘要: 以三聚氰胺（Melamine）为原料，在高温条件下采用热缩合反应合成了石墨型氮化碳（g-C3N4）光催化剂.通过X-射线衍射（XRD）、扫描电镜（SEM）、紫外-可见漫反射光谱（UV-Vis DRS）、衰减全反射红外光谱（ATR-IR）等技术对其物理结构及性质进行了表征，结果表明实验制备的g-C3N4为片层状结构，比表面积为15.34 m2·g-1.在可见光（λ>420 nm）照射下，用g-C3N4降解有机小分子污染物2，4-二氯苯酚（2，4-Dichlorophenol，2，4-DCP），该过程反应符合一级动力学，反应速率常数为0.0113 min-1，以0.67 g·L-1的用量反应250 min后2，4-DCP矿化率达到60%；2，4-DCP在弱酸性条件下（pH=5.4）的降解效率最高；通过捕获实验及电子自旋共振（ESR）实验表明，超氧自由基（O2·-）是g-C3N4光催化降解2，4-DCP过程中的主要活性物种.2，4-DCP的降解路径主要涉及脱氯、苯环开环和碳链断裂等反应历程.

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