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介孔二氧化钛/导电碳毡光电极制备及其苯甲醛降解机理分析

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李铭, 李佑稷, 徐鹏, 林晓, 李小康. 介孔二氧化钛/导电碳毡光电极制备及其苯甲醛降解机理分析[J]. 环境工程学报, 2016, 10(5): 2567-2575. doi: 10.12030/j.cjee.201412215
引用本文: 李铭, 李佑稷, 徐鹏, 林晓, 李小康. 介孔二氧化钛/导电碳毡光电极制备及其苯甲醛降解机理分析[J]. 环境工程学报, 2016, 10(5): 2567-2575. doi: 10.12030/j.cjee.201412215
shu
Li Ming, Li Youji, Xu Peng, Lin Xiao, Li Xiaokang. Preparation, photoelectric catalysis performance and degradation mechanism of mesoporous titanium dioxide/conductive carbon felt electrode[J]. Chinese Journal of Environmental Engineering, 2016, 10(5): 2567-2575. doi: 10.12030/j.cjee.201412215
Citation: Li Ming, Li Youji, Xu Peng, Lin Xiao, Li Xiaokang. Preparation, photoelectric catalysis performance and degradation mechanism of mesoporous titanium dioxide/conductive carbon felt electrode[J]. Chinese Journal of Environmental Engineering, 2016, 10(5): 2567-2575. doi: 10.12030/j.cjee.201412215
shu

介孔二氧化钛/导电碳毡光电极制备及其苯甲醛降解机理分析

  • 1.

    吉首大学化学化工学院, 吉首 416000

  • 基金项目:

    教育部新世纪优秀人才支撑计划(NCET-12-0720)

    湖南省自然科学杰出青年基金(13JJ1023)

    湖南省高校科技创新团队支持计划

    吉首大学研究生项目资助(2014KFXM03)

  • 中图分类号: X701

Preparation, photoelectric catalysis performance and degradation mechanism of mesoporous titanium dioxide/conductive carbon felt electrode

  • 1.

    College of Chemistry and Chemical Engineering, Jishou University, Jishou 416000, China

  • Fund Project:

摘要

  • 摘要: 基于表面活性剂十六烷基三甲基溴化铵为液晶模板,以四氯化钛为钛源,导电碳毡为载体,通过超声波辅助水热法(ultrasound-assisted hydrothermal method, UH)制备介孔二氧化钛/导电碳毡复合体材料(mesoporous titania/conductive carbon felt, MPT/CCF) (UH-MPT/CCF),为了探讨其结构与光电催化活性,直接采用水热法制备介孔二氧化钛/导电碳毡(H-MPT/CCF)和无孔二氧化钛/导电碳毡(no porous titania/conductive carbon felt, NPT/CCF)复合体材料,利用XRD、XPS、SEM、TEM、TG-DTA、N2吸附-脱附等方法对样品结构进行表征,以气相苯甲醛为目标降解物,研究UH-MPT/CCF的光电催化性能及其对气相苯甲醛的降解机理。结果表明,UH-MPT/CCF材料通过介孔化增加了活性中心(·OH和Ti3+),通过CCF的负载提高了对目标降解物的吸附富集,通过偏电压促进光生电子-空穴对的分离,在这三方的协同作用下UH-MPT/CCF对苯甲醛在100 min内降解率为83.9%,分别是H-MPT/CCF、NPT/CCF和P25/CCF的1.38、1.75和2.38倍。气相苯甲醛光电催化降解产生的主要中间产物是苯、1,3-己二烯-5-炔,以及少量的3,3,5-三甲基环己烯、2,3-二甲基-1,3-庚二烯、3-甲基-3-环己烯-1-醇等。根据GC/MS分析结果,进一步提出了气相苯甲醛的降解机理。
    Abstract: Based on a liquid crystal template, consisting of cetyltrimethyl ammonium bromide surfactant, titanium tetrachloride and conductive carbon felt were used as a titanium source and carrier, respectively. Mesoporous titanium dioxide/conductive carbon felt (UH-MPT/CCF) composites were prepared by using an ultrasound-assisted hydrothermal synthesis method. In order to investigate the structure and photoelectrocatalytic performance, a hydrothermal method was applied to synthesize mesoporous titanium dioxide/conductive carbon felt (H-MPT/CCF) and non-porous titania/conductive carbon felt (NPT/CCF). The structures of obtained samples were examined via X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), thermogravimetry (TG)-differential thermal analysis (DTA), and nitrogen adsorption-desorption. By choosing benzaldehyde as the target degradation product, the photoelectrocatalytic performance of UH-MPT/CCF under ultraviolet light irradiation was discussed. The results showed that UH-MPT/CCF increased active center (·OH and Ti3+) through a mesoporous effect, enhanced the adsorption of the target objects through the CCF support, and led to separation of photogenerated electron-hole pairs via the bias voltage. As a result of the synergy of these three effects, degradation rate of gaseous benzaldehyde by UH-MPT/CCF after 100 min was 83.9%, which were 1.38, 1.75, and 2.38 times as high as those of H-MPT/CCF, NPT/CCF, and P25/CCF, respectively. Photoelectrocatalytic products of gaseous benzaldehyde included the main intermediates of benzene, 1,3-hexadien-5-yne and a small amount of 3,5,5-trimethylcyclohexene, 2,3-dimethyl-1,3-heptadiene, and 3-methyl-3-cyclohexen-1-alcohol. According to the results of gas chromatography/mass spectrometry (GC/MS) analysis, the mechanism of the degradation process of gaseous benzaldehyde was proposed.
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  • 收稿日期:  2015-01-19
  • 刊出日期:  2016-06-03
李铭, 李佑稷, 徐鹏, 林晓, 李小康. 介孔二氧化钛/导电碳毡光电极制备及其苯甲醛降解机理分析[J]. 环境工程学报, 2016, 10(5): 2567-2575. doi: 10.12030/j.cjee.201412215
引用本文: 李铭, 李佑稷, 徐鹏, 林晓, 李小康. 介孔二氧化钛/导电碳毡光电极制备及其苯甲醛降解机理分析[J]. 环境工程学报, 2016, 10(5): 2567-2575. doi: 10.12030/j.cjee.201412215
shu
Li Ming, Li Youji, Xu Peng, Lin Xiao, Li Xiaokang. Preparation, photoelectric catalysis performance and degradation mechanism of mesoporous titanium dioxide/conductive carbon felt electrode[J]. Chinese Journal of Environmental Engineering, 2016, 10(5): 2567-2575. doi: 10.12030/j.cjee.201412215
Citation: Li Ming, Li Youji, Xu Peng, Lin Xiao, Li Xiaokang. Preparation, photoelectric catalysis performance and degradation mechanism of mesoporous titanium dioxide/conductive carbon felt electrode[J]. Chinese Journal of Environmental Engineering, 2016, 10(5): 2567-2575. doi: 10.12030/j.cjee.201412215
shu

介孔二氧化钛/导电碳毡光电极制备及其苯甲醛降解机理分析

  • 1. 吉首大学化学化工学院, 吉首 416000
  • 收稿日期:  2015-01-19
基金项目:

教育部新世纪优秀人才支撑计划(NCET-12-0720)

湖南省自然科学杰出青年基金(13JJ1023)

湖南省高校科技创新团队支持计划

吉首大学研究生项目资助(2014KFXM03)

摘要: 基于表面活性剂十六烷基三甲基溴化铵为液晶模板,以四氯化钛为钛源,导电碳毡为载体,通过超声波辅助水热法(ultrasound-assisted hydrothermal method, UH)制备介孔二氧化钛/导电碳毡复合体材料(mesoporous titania/conductive carbon felt, MPT/CCF) (UH-MPT/CCF),为了探讨其结构与光电催化活性,直接采用水热法制备介孔二氧化钛/导电碳毡(H-MPT/CCF)和无孔二氧化钛/导电碳毡(no porous titania/conductive carbon felt, NPT/CCF)复合体材料,利用XRD、XPS、SEM、TEM、TG-DTA、N2吸附-脱附等方法对样品结构进行表征,以气相苯甲醛为目标降解物,研究UH-MPT/CCF的光电催化性能及其对气相苯甲醛的降解机理。结果表明,UH-MPT/CCF材料通过介孔化增加了活性中心(·OH和Ti3+),通过CCF的负载提高了对目标降解物的吸附富集,通过偏电压促进光生电子-空穴对的分离,在这三方的协同作用下UH-MPT/CCF对苯甲醛在100 min内降解率为83.9%,分别是H-MPT/CCF、NPT/CCF和P25/CCF的1.38、1.75和2.38倍。气相苯甲醛光电催化降解产生的主要中间产物是苯、1,3-己二烯-5-炔,以及少量的3,3,5-三甲基环己烯、2,3-二甲基-1,3-庚二烯、3-甲基-3-环己烯-1-醇等。根据GC/MS分析结果,进一步提出了气相苯甲醛的降解机理。

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