无机盐工业
主管:中海油天津化工研究设计院有限公司
主办:中海油天津化工研究设计院有限公司
   中海油炼油化工科学研究院(北京)有限公司
   中国化工学会无机酸碱盐专业委员会
ISSN 1006-4990 CN 12-1069/TQ

无机盐工业 ›› 2025, Vol. 57 ›› Issue (1): 113-119.doi: 10.19964/j.issn.1006-4990.2024-0198

• 催化材料 • 上一篇    下一篇

Pd/ZnIn2S4纳米片光催化苯甲醇氧化耦合产氢的研究

孙庆昊(), 李克艳(), 郭新闻()   

  1. 大连理工大学化工学院精细化工国家重点实验室智能材料化工前沿科学中心,辽宁 大连 116024
  • 收稿日期:2024-04-09 出版日期:2025-01-10 发布日期:2024-05-09
  • 通讯作者: 李克艳(1979— ),女,博士,副教授,研究方向为光催化、高级氧化技术;E-mail:keyanli@dlut.edu.cn
    郭新闻(1967— ),男,博士,教授,研究方向为分子筛催化、二氧化碳催化转化;E-mail:guoxw@dlut.edu.cn
  • 作者简介:孙庆昊(1999— ),男,硕士研究生,研究方向为光催化苯甲醇氧化;E-mail:qhsun@mail.dlut.edu.cn
  • 基金资助:
    兴辽英才计划项目(XLYC2008032);中央高校基本科研业务费专项资金资助项目(DUT22LAB602)

Study on photocatalytic benzyl alcohol oxidation coupled with hydrogen production over Pd/ZnIn2S4 nanosheets

SUN Qinghao(), LI Keyan(), GUO Xinwen()   

  1. State Key Laboratory of Fine Chemicals,Frontier Science Center for Smart Materials,School of Chemical Engineering,Dalian University of Technology,Dalian 116024,China
  • Received:2024-04-09 Published:2025-01-10 Online:2024-05-09

摘要:

通过溶剂热-光沉积法制备了Pd颗粒负载的二维ZnIn2S4纳米片用于光催化苯甲醇氧化和产氢的耦合反应。当Pd负载量为1.0%(质量分数)时光催化性能最优,在可见光下苯甲醛和氢气的产生速率分别达到3 804.1、4 629.8 µmol/(g·h),苯甲醛选择性为80.0%。利用X射线衍射仪(XRD)、透射电子显微镜(TEM)、X射线光电子能谱仪(XPS)等表征了光催化剂的形貌与结构,利用光致发光光谱(PL)、时间分辨荧光光谱(tr-PL)、电化学阻抗谱(EIS spectra)、紫外-可见漫反射光谱(UV-visible spectra)等分析了光催化剂的光学和光电化学性质。研究发现,Pd颗粒的表面等离子体共振效应增强了光催化剂的可见光吸收,其较低的费米能级使得ZnIn2S4导带上的光生电子向Pd转移,提高了光生载流子的分离效率,因此提升了光催化氧化还原反应性能。此外,还提出了Pd/ZnIn2S4光催化剂氧化苯甲醇协同产氢的反应机理,即光生空穴将苯甲醇氧化成苯甲醛,光生电子将苯甲醇中的氢质子还原成氢气。

关键词: 光催化, 苯甲醇氧化, 产氢, ZnIn2S4, 贵金属

Abstract:

In this work,Pd particles loaded two-dimensional ZnIn2S4 nanosheets were prepared by a solvothermal-photodeposition method for coupling photocatalytic reactions of benzyl alcohol oxidation and hydrogen production.When the Pd loading was 1.0%(mass fraction),the photocatalytic performance was best.The production rates of benzaldehyde and hydrogen achieved 3 804.1 and 4 629.8 µmol/(g·h),and the selectivity of benzaldehyde was 80.0% under visible light.The morphology and structure of the photocatalysts were characterized using XRD,TEM and XPS,and the optical and photoelectrochemical properties were characterized through PL spectra,tr-PL spectra,EIS spectra and UV-visible spectra.It was found that loading of Pd particles enhanced the absorption of visible light due to its surface plasmon resonance effect.The separation efficiency of carriers was effectively promoted due to the transfer of photogenerated electrons in the conduction band of ZnIn2S4 to Pd with low Fermi level,thereby improving the performance of photocatalytic redox reactions.In addition,a possible mechanism for the photocatalytic oxidation of benzyl alcohol coupling with hydrogen evolution was proposed,i.e.,benzyl alcohols were oxidized to benzaldehyde by photogenerated holes,while the protons from benzyl alcohol were reduced to H2 by photogenerated electrons.

Key words: photocatalysis, benzyl alcohol oxidation, hydrogen evolution, ZnIn2S4, noble metal

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