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Enhanced electro-catalytic activity of TNTs/SnO2-Sb electrode through the effect mechanism of TNTs architecture

YANG Lisha GUO Yanming

杨莉莎, 郭颜铭. TNTs结构强化TNTs/SnO2-Sb电极电催化活性的影响机制[J]. 燃料化学学报(中英文), 2024, 52(5): 687-697. doi: 10.1016/S1872-5813(23)60390-1
引用本文: 杨莉莎, 郭颜铭. TNTs结构强化TNTs/SnO2-Sb电极电催化活性的影响机制[J]. 燃料化学学报(中英文), 2024, 52(5): 687-697. doi: 10.1016/S1872-5813(23)60390-1
YANG Lisha, GUO Yanming. Enhanced electro-catalytic activity of TNTs/SnO2-Sb electrode through the effect mechanism of TNTs architecture[J]. Journal of Fuel Chemistry and Technology, 2024, 52(5): 687-697. doi: 10.1016/S1872-5813(23)60390-1
Citation: YANG Lisha, GUO Yanming. Enhanced electro-catalytic activity of TNTs/SnO2-Sb electrode through the effect mechanism of TNTs architecture[J]. Journal of Fuel Chemistry and Technology, 2024, 52(5): 687-697. doi: 10.1016/S1872-5813(23)60390-1

TNTs结构强化TNTs/SnO2-Sb电极电催化活性的影响机制

doi: 10.1016/S1872-5813(23)60390-1
详细信息
  • 中图分类号: X703.1

Enhanced electro-catalytic activity of TNTs/SnO2-Sb electrode through the effect mechanism of TNTs architecture

Funds: The project was supported by National Natural Science Foundation of China (52000061).
More Information
  • 摘要: 采用溶剂热法制备了TNTs/SnO2-Sb电极,通过调整氧化电压和氧化时间构建出不同结构的二氧化钛纳米管(TNTs)阵列,以探究其对电极结构和电化学性能的影响。SEM和接触角测试表明,相较于阳极氧化时间,阳极氧化电压是影响TNTs阵列形貌和表面亲水性的主要因素。SEM、XRD、LSV和EIS结果表明,TNTs阵列孔径的大小影响了催化涂层的形貌、晶粒尺寸以及电极的析氧电位。XPS、EPR和羟基自由基(·OH)生成测试表明,涂层表面致密且粒径较小有利于电极表面获得更多的氧空位,且氧空位浓度越高,吸附氧物种越多,从而增强了活性自由基的形成以及对有机物的降解。以长度950 nm,孔径100 nm 的TNTs 阵列层为基底时,所制备的电极TNTs (25 V) / SnO2-Sb展现出了最佳的苯酚处理效果(92%±4.6%,2 h)。
  • FIG. 3130.  FIG. 3130.

    FIG. 3130.  FIG. 3130.

    Figure  1  TNTs substrate architectures under different preparation conditions ((a) 15V-1h, (b) 15V-2h, (c) 15V-3h, (d) 20V-1h, (e) 20V-2h, (f) 20V-3h, (g) 25V-1h, (h) 25V-2h, (i) 25V-3h, (j) 30V-1h, (k) 30V-2h, (l) 30V-3h)

    Figure  2  Contact angle of (a) Ti, (b) TNTs (15 V-2 h), (c) TNTs (20 V-2 h), (d) TNTs (25 V-2 h), (e) TNTs (30 V-2 h), (f) TNTs (25 V-1 h) and (g) TNTs (25 V-3 h)

    Figure  3  SEM images of (a) Ti/SnO2-Sb, (b) TNTs (15 V)/SnO2-Sb, (c) TNTs (20 V)/SnO2-Sb, (d) TNTs (25 V)/SnO2-Sb electrode, (e) TNTs (30 V)/SnO2-Sb electrode

    Figure  4  XRD patterns of (a) TNTs (25 V) substrate and (b) TNTs/SnO2-Sb electrodes with different substrate preparation voltages

    Figure  5  OEP of TNTs/SnO2-Sb electrodes with different substrate preparation voltages

    Figure  6  EIS spectrums of TNTs/SnO2-Sb electrodes with different substrate preparation voltages

    Figure  7  Electrochemical degradation of phenol on TNTs/SnO2-Sb electrodes with TNTs substrates under different preparation conditions ((a) Variations of concentration of phenol with electrolysis time, (b) The first-order kinetics curves of phenol degradation)

    Figure  8  XPS pattern of Sn 3d of SnO2-Sb different electrodes

    Figure  9  XPS patterns of the fitted curves of O 1s and Sb 3d of electrodes prepared by different voltages

    Figure  10  EPR spectra of TNTs/SnO2-Sb electrodes with different substrate preparation voltages

    Figure  11  The hydroxyl radicals generation ability on the SnO2-Sb electrode with different substrate preparation voltages

    Figure  12  The quenching experiment of the active radicals on the SnO2-Sb electrodes with different substrate preparation voltages

    Table  1  Effect of preparation conditions for TNTs arrays on the average crystal size of SnO2-Sb calculated by Scherrer formula

    SampleCrystallite size/nm
    Ti/SnO2-Sb23±0.3
    TNTs (15 V)/SnO2-Sb20±0.3
    TNTs (20 V)/SnO2-Sb17±0.4
    TNTs (25 V)/SnO2-Sb15±0.3
    TNTs (30 V)/SnO2-Sb13±0.4
    Scherrer formula: D=kλ/(βcosθ), where D is the crystallite size, k is the Scherrer constant (0.89), λ is the wavelength of incident ray, β is the full width at half maximum of the peak, and θ is the position of plane peak[30].
    下载: 导出CSV

    Table  2  EIS fitting results of TNTs/SnO2-Sb electrodes with different substrate preparation voltages

    SampleRsCh/FRhCt/FRt
    Ti/SnO2-Sb4.725.33×10−849.32.02×10−549
    TNTs (15 V)/SnO2-Sb4.715.62×10−847.62.06×10−548
    TNTs (20 V)/SnO2-Sb4.695.84×10−846.92.11×10−547
    TNTs (25 V)/SnO2-Sb4.676.33×10−844.32.20×10−545
    TNTs (30 V)/SnO2-Sb4.746.12×10−845.42.16×10−546
    下载: 导出CSV

    Table  3  Effect of preparation voltage of TNTs arrays on the contact angle of substrate surface and loading amount of SnO2-Sb

    SampleContact angle/(°)Loading amount/(mg·cm−2)
    Ti522.05±0.05
    TNTs (15 V-2 h)432.15±0.04
    TNTs (20 V-2 h)342.24±0.04
    TNTs (25 V-2 h)132.36±0.03
    TNTs (30 V-2 h)102.42±0.02
    下载: 导出CSV

    Table  4  XPS analysis of TNTs/SnO2-Sb electrodes with different substrate preparation voltages

    SampleBinding energy/eVOads
    (at% = $\dfrac{\rm{O}_{\mathrm{a}\mathrm{d}\mathrm{s} }}{\mathrm{S}\mathrm{n} + \mathrm{S}\mathrm{b} + \mathrm{O}_{\mathrm{a}\mathrm{d}\mathrm{s}} + \mathrm{O}_{\mathrm{l}\mathrm{a}\mathrm{t} }}$ × 100% )
    Atom ratio of Olat/(Sn + Sb)
    Sn 3d5/2Sb 3d5/2OadsOlat
    Control486.91530.89532.03530.7314.62.65
    15 V486.84530.90531.98530.6917.92.41
    20 V486.46531.19531.96530.6419.82.18
    25 V486.21531.12531.89530.5525.61.88
    30 V486.35530.94531.91530.5923.21.97
    下载: 导出CSV

    Table  5  The computed result from the quenching experiment

    SampleThe contribution to phenol degradation/%
    ·O2 ·OH
    Control42.174
    15 V45.776.3
    20 V4779
    25 V50.584
    30 V48.681
    下载: 导出CSV
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出版历程
  • 收稿日期:  2023-09-04
  • 修回日期:  2023-09-25
  • 录用日期:  2023-09-26
  • 网络出版日期:  2023-10-31
  • 刊出日期:  2024-05-01

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