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镍铁水滑石/聚S,S-二氧-二苯并噻吩复合材料的合成及其光催化产氢性能

罗旌崧 付清瑶 刘玉祥 汪锋

罗旌崧, 付清瑶, 刘玉祥, 等. 镍铁水滑石/聚S,S-二氧-二苯并噻吩复合材料的合成及其光催化产氢性能[J]. 复合材料学报, 2021, 39(0): 1-10
引用本文: 罗旌崧, 付清瑶, 刘玉祥, 等. 镍铁水滑石/聚S,S-二氧-二苯并噻吩复合材料的合成及其光催化产氢性能[J]. 复合材料学报, 2021, 39(0): 1-10
Jingsong LUO, Qingyao FU, Yuxiang LIU, Feng WANG. Synthesis and photocatalytic hydrogen production performance of nickel-iron hydrotalcite/poly(dibenzothiophene-S,S-dioxide)composites[J]. Acta Materiae Compositae Sinica.
Citation: Jingsong LUO, Qingyao FU, Yuxiang LIU, Feng WANG. Synthesis and photocatalytic hydrogen production performance of nickel-iron hydrotalcite/poly(dibenzothiophene-S,S-dioxide)composites[J]. Acta Materiae Compositae Sinica.

镍铁水滑石/聚S,S-二氧-二苯并噻吩复合材料的合成及其光催化产氢性能

基金项目: 湖北省教育厅重点项目(批准号: D20181505);光电化学材料与器件教育部重点实验室(江汉大学) (批准号: JDGD-202003)
详细信息
    通讯作者:

    汪锋 博士,教授,博士生导师,研究方向为光催化材料 E-mail: psfwang@wit.edu.cn

  • 中图分类号: O644.1

Synthesis and photocatalytic hydrogen production performance of nickel-iron hydrotalcite/poly(dibenzothiophene-S,S-dioxide)composites

  • 摘要: 镍铁水滑石(Ni7Fe1)易于合成、来源丰富、价格低廉,是目前催化体系中性能优良的催化剂之一,可望用于替代成本高昂的贵金属催化剂。采用原位聚合法将二维层状结构的Ni7Fe1与聚S,S-二氧-二苯并噻吩(PDBTSO)复合,制备了无机/有机复合材料Ni7Fe1/PDBTSO,并验证了其光催化性能。实验得到:复合材料15-Ni7Fe1/PDBTSO相较于添加3wt% Pt助催化剂PDBTSO的光催化产氢效率提高了22.6%,其产氢效率达到36.8 mmol·g−1·h−1且具有良好的循环稳定性,表明Ni7Fe1为替代光催化制氢反应中贵金属助催化剂理想的候选材料之一。结合XRD、FTIR、TEM和XPS等手段进一步讨论了复合材料光催化产氢的机制。Ni7Fe1/PDBTSO高效的光催化制氢性能及低成本的制备方法为光催化制氢领域提供了新的思路。

     

  • 图  1  Ni7Fe1/聚S,S-二氧-二苯并噻吩(PDBTSO)的合成路线

    Figure  1.  Synthetic route for Ni7Fe1/ poly(dibenzothiophene-S, S-dioxide) (PDBTSO)

    图  2  Ni7Fe1、PDBTSO和Ni7Fe1/PDBTSO的XRD谱图

    Figure  2.  XRD patterns of Ni7Fe1, PDBTSO and Ni7Fe1/PDBTSO

    图  3  Ni7Fe1、PDBTSO和Ni7Fe1/PDBTSO的FTIR图谱

    Figure  3.  FTIR spectra of Ni7Fe1, PDBTSO and Ni7Fe1/PDBTSO

    图  4  Ni7Fe1 (a)、PDBTSO (b)和15-Ni7Fe1/PDBTSO (c)的SEM图;(d)15-Ni7Fe1/PDBTSO的EDX图; C (e), O (f), S (g), Ni (h)和Fe (i)元素分布图

    Figure  4.  SEM image of PDBTSO (a), Ni7Fe1 (b) and 15-Ni7Fe1/PDBTSO(c);(d)EDX image of a single 15-Ni7Fe1/PDBTSO and multi-elemental image of C (e), O (f), S (g), Ni (h), Fe (i) elemental maps

    图  5  Ni7Fe1 (a)、15-Ni7Fe1/PDBTSO (b)的TEM图; Ni7Fe1(c) and 15-Ni7Fe1/PDBTSO (d)的HRTEM图

    Figure  5.  TEM image of Ni7Fe1 (a) and15-Ni7Fe1/PDBTSO (b); HRTEM image of Ni7Fe1 (c) and15-Ni7Fe1/PDBTSO (d)

    图  6  (a) 15-Ni7Fe1/PDBTSO XPS全谱图; C 1s (b)、O 1s (c)、S 2p (d)、Ni 2p (e)、Fe 2p (f)的XPS谱图

    Figure  6.  (a) XPS spectra of 15-Ni7Fe1/PDBTSO and Comparison results of the deconvoluted XPS spectra of Ni7Fe1, PDBTSO and 15-Ni7Fe1/PDBTSO for C 1s (b), O 1s (c), S 2p (d), Ni 2p (e), Fe 2p (f)

    图  7  Ni7Fe1, PDBTSO和Ni7Fe1/PDBTSO紫外-可见光固体紫外漫反射吸收光谱图

    Figure  7.  UV-vis DRS of Ni7Fe1, PDBTSO and Ni7Fe1/PDBTSO

    图  8  (a)Ni7Fe1/PDBTSO的光催化产氢性能;(b)PDBTSO添加3wt% Pt助催化剂、15-Ni7Fe1/PDBTSO的光催化产氢性能;(c)15-Ni7Fe1/PDBTSO光催化制氢稳定性测试;光催化反应前后15-Ni7Fe1/PDBTSO (d) XRD谱图;(e)FTIR谱图;(f)UV-DRS FTIR谱图

    Figure  8.  (a)The HERs of Ni7Fe1/PDBTSO and (b)PDBTSO with 3 wt% Pt and 15-Ni7Fe1/PDBTSO, (c)Stability test of 15-Ni7Fe1/PDBTSO before and after the photocatalytic reaction (d)XRD patterns, (e)FTIR patterns, (f)UV-DRS patterns

    图  9  (a)PDBTSO和15-Ni7Fe1/PDBTSO的稳态荧光光谱图;(b)PDBTSO和15-Ni7Fe1/PDBTSO的荧光寿命图;(c)Ni7Fe1、PDBTSO和15-Ni7Fe1/PDBTSO的阻抗图谱;(d)PDBTSO和15-Ni7Fe1/PDBTSO的光电流响应图谱

    Figure  9.  (a)PL spectra, (b)Time-resolved PL spectra of PDBTSO and 15-Ni7Fe1/PDBTSO, (c)EIS image of Ni7Fe1、PDBTSO and 15-Ni7Fe1/PDBTSO, (d)Photoelectrode transient photocurrent response image of PDBTSO and 15-Ni7Fe1/PDBTSO

    图  10  (a)Ni7Fe1和PDBTSO的CV曲线; (b)Ni7Fe1/PDBTSO的产氢机制图

    Figure  10.  (a)CV curves of Ni7Fe1 and PDBTSO; (b)Proposed mechanism for photocatalytic hydrogen evolution at the Ni7Fe1/PDBTSO composite

    LUMO(CB)—conduction band; HOMO(VB)—valence band; Eg—optical band gaps; TEOA—triethanolamine

    表  1  PDBTSO和15-Ni7Fe1/PDBTSO荧光寿命

    Table  1.   Fitted decay time of the PDBTSO and 15-Ni7Fe1/PDBTSO

    Sampleτ1/nsRel/%τ2/nsRel/%τ3/nsRel/%τ/ns
    PDBTSO0.29143.680.76731.622.94624.700.502
    15-Ni7Fe1/PDBTSO0.46853.542.12237.308.2529.160.751
    Notes: τ1, τ2—fast decay component,slow decay component;τ—average lifetimes;Rel—related function.
    下载: 导出CSV

    表  2  Ni7Fe1和PDBTSO的光化学性能

    Table  2.   Optical and electrochemical properties for the PDBTSO and Ni7Fe1

    SAMPLEReduction potential/eVOxidation potential/eVELUMO(CB)/eVEHOMO(VB)/eVEga/eVEgb/eV
    PDBTSO−1.151.51−3.35−6.012.662.55
    Ni7Fe1−0.651.60−3.86−6.112.252.20
    Notes:ELUMO(CB)—conduction band potential;EHOMO(VB)—valence band potential;Ega—band gaps calculated from ELUMO(CB)-EHOMO(VB)Egb—optical band gaps;Fc/Fc+—the potential ferrocene/ferrocenium;Fc/Fc+=0.29 (vs SCE)/V;Egb=1240/λ.
    下载: 导出CSV
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  • 收稿日期:  2021-09-22
  • 录用日期:  2021-11-26
  • 修回日期:  2021-11-09
  • 网络出版日期:  2021-12-21

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