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Inorganic ligands-mediated hole attraction and surface structural reorganization in InP/ZnS QD photocatalysts studied via ultrafast visible and midinfrared spectroscopies

通过瞬态可见和瞬态中红外光谱研究InP/ZnS QDs无机配体诱导的表面空穴转移和构型调整过程

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  • Published: 30 March 2022
  • Volume 65, pages 2529–2539, (2022)
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Science China Materials Aims and scope Submit manuscript
Inorganic ligands-mediated hole attraction and surface structural reorganization in InP/ZnS QD photocatalysts studied via ultrafast visible and midinfrared spectroscopies
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  • Yang Liu  (刘旸)1,2,3,4,
  • Ying Zhou  (周莹)1,3,
  • Mohamed Abdellah5,
  • Weihua Lin  (林炜铧)4,
  • Jie Meng  (孟杰)6,
  • Qian Zhao  (赵乾)6,
  • Shan Yu  (于姗)1,3,
  • Zhanghui Xie  (谢章辉)3,
  • Qinying Pan  (泮琴英)6,
  • Fengying Zhang  (张凤英)1,3,
  • Tonu Pullerits4 &
  • …
  • Kaibo Zheng  (郑凯波)4,6 

  • 987 Accesses

  • 9 Citations

  • Explore all metrics

Abstract

Photoinduced carrier dynamical processes dominate the optical excitation properties of photocatalysts and further determine the photocatalytic performance. In addition, as the electrons generally possess a faster transfer rate than holes, hole transfer and accumulation are critical, and they play the key efficiency-limiting step during the photocatalytic process. Therefore, a comprehensive understanding of the dynamics of photogenerated holes and their determining factors in the photocatalytic system is highly essential to rationalize the full catalytic mechanism and develop highly efficient photocatalysts, which have not yet been revealed. In this work, the photoinduced charge carrier dynamics in InP/ZnS quantum dots (QDs) capped with long-chain L-typed ligands (oleylamine) and inorganic ligands (sulfide ion (S2−)) were explored. Time-resolved photoluminescence and femtosecond transient-absorption spectroscopy unambiguously confirmed the ultrafast hole transfer from the InP core to S2− ligands. Moreover, by probing the bleach of vibrational stretching of the ligands with transient midinfrared absorption spectroscopy, the hole transfer time was determined to be 4.2 ps. The injected holes are long-lived at the S2− ligands (>4.5 ns), and they can remove electrostatically attached surfactants to compensate for the spatial charge redistribution. Finally, compared with other inorganic ligands such as Cl− and PO43−, S2− balances the ionic radii and net charge to ensure the optimal condition for charge transfer. Such observation rationalizes the excellent photocatalytic H2 evolution (213.6 µmol mg−1 within 10 h) in InP/ZnS QDs capped with S2− compared with those capped with other ligands and elucidates the role of surface ligands in the photocatalytic activity of colloidal QDs.

摘要

光生载流子动力学过程可以显著影响材料光催化活性. 通常, 光生电子的转移速率远高于光生空穴的, 致使空穴的转移和累积成为影响光催化效率的关键因素. 因此, 深入探究光生空穴转移过程和动力学可以极大地帮助我们认识和理解光催化机理, 但该工作鲜有人关注研究. 本工作中, 时间分辨荧光光谱(TRPL)和飞秒瞬态可见吸收光谱(fs-TA)表明空穴会从InP转移至表面S2−配体. 此外, 瞬态中红外光谱 (TRIR)中S2−配体伸缩振动信号表明该空穴转移时间为4.2 ps. 转移至S2−配体的空穴具有明显的长寿命特征(>4.5 ns)并且会导致表面活性物的静电解离和构型重组. 最后, 通过与其他无机配体(Cl−、 PO43−)比较, 我们发现S2−配体具有最合适平衡的离子半径和净电荷, 因此带有该配体的InP/ZnS量子点(InP/ZnS QDs)光催化集具有最高的光解硫化氢产氢活性(213.6 µmol mg−1). 本文的研究结果为理解InP QDs光催化过程和机理提供了有价值的见解.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (NSFC, 22002123 and U1862111), Sichuan Science and Technology Program (2020YFH0118, 2021JDGD0029 and 2021YFH0055), the Open Fund of State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation (PLN201802), the Independent Research Fund Denmark-Nature Sciences (DFF-FNU, DFF-7014-00302), the Independent Research Fund Denmark-Sapere Aude starting grant (7026-00037A), the Research Fund for International Young Scientists from NSFC (21950410515), and Swedish Research Council VR Starting Grant (2017-05337). Meng J, Zhao Q, Pan Q and Lin W also acknowledge the financial support from China Scholarship Council (201806320345, 201908440313, 201706170017, and 201806460021). Support from Swedish Energy Agency is acknowledged.

Funding

Funding note Open Access Funding provided by Swedish Research Council VR Starting Grant (2017-05337).

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Authors and Affiliations

  1. State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu, 610500, China

    Yang Liu  (刘旸), Ying Zhou  (周莹), Shan Yu  (于姗) & Fengying Zhang  (张凤英)

  2. College of Optoelectronic Technology, Chengdu University of Information Technology, Chengdu, 610225, China

    Yang Liu  (刘旸)

  3. School of New Energy and Materials, Southwest Petroleum University, Chengdu, 610500, China

    Yang Liu  (刘旸), Ying Zhou  (周莹), Shan Yu  (于姗), Zhanghui Xie  (谢章辉) & Fengying Zhang  (张凤英)

  4. The Division of Chemical Physics and Nano-Lund, Lund University, Lund, 22100, Sweden

    Yang Liu  (刘旸), Weihua Lin  (林炜铧), Tonu Pullerits & Kaibo Zheng  (郑凯波)

  5. Ångström Laboratory, Department of Chemistry, Uppsala University, Uppsala, 75120, Sweden

    Mohamed Abdellah

  6. Department of Chemistry, Technical University of Denmark, Kongens Lyngby, DK-2800, Denmark

    Jie Meng  (孟杰), Qian Zhao  (赵乾), Qinying Pan  (泮琴英) & Kaibo Zheng  (郑凯波)

Authors
  1. Yang Liu  (刘旸)
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  2. Ying Zhou  (周莹)
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  3. Mohamed Abdellah
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  4. Weihua Lin  (林炜铧)
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  5. Jie Meng  (孟杰)
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  6. Qian Zhao  (赵乾)
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  7. Shan Yu  (于姗)
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  8. Zhanghui Xie  (谢章辉)
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  9. Qinying Pan  (泮琴英)
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  12. Kaibo Zheng  (郑凯波)
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Contributions

Author contributions Zhou Y and Zheng K conceived the research and designed the experiments. Liu Y designed the synthesis. Liu Y, Xie Z and Zhao Q performed the synthesis. Abdellah M performed ultrafast mid-IR spectroscopy. Lin W performed ultrafast visible spectroscopy. Liu Y and Meng J performed the TEM and HRTEM characterizations. Liu Y wrote the manuscript with support from Zhou Y and Zheng K. Yu S, Pan Q, Zhang F and Pullerits T revised the manuscript. All authors discussed the results and commented on the manuscript.

Corresponding authors

Correspondence to Ying Zhou  (周莹) or Kaibo Zheng  (郑凯波).

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Conflict of interest The authors declare that they have no conflict of interest.

Additional information

Supplementary information Experimental details and supporting data are available in the online version of the paper.

Yang Liu received his PhD degree from Southwest Petroleum University, China, in 2021. He was an exchange PhD student at Lund University in Sweden, supported by China Scholarship Council. At present, he is a lecturer at Chengdu University of Information Technology. His research interests primarily focus on quantum dot photocatalysts and ultrafast spectroscopies.

Ying Zhou received his BSc and MSc degrees from Central South University and Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, respectively. In 2010, he received his PhD degree at the University of Zurich (UZH) under the supervision of Prof. Greta R Patzke. He then continued his work with a postdoctoral Forschungskredit grant from UZH. He was also awarded a fellowship by the Alexander von Humboldt Foundation at Karlsruhe Institute of Technology with Prof. Jan-Dierk Grunwaldt and was a visiting professor at Kyoto University. He currently holds a professorship at Southwest Petroleum University. His research interest is in the clean utilization of oil and gas, environmental remediation materials and related in situ characterization techniques.

Kaibo Zheng obtained his PhD degree in 2010 from the Department of Materials Science at Fudan University. Then, he joined the Chemical Physics Division at Lund University, Sweden, as a postdoctoral fellow. He is currently a senior researcher in chemical physics at Lund University and dual affiliated as a senior researcher at the Department of Chemistry, Technical University of Denmark. His research interests include the structure and photophysics of semiconductors and perovskite quantum dots as light harvesters.

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Inorganic ligands-mediated hole attraction and surface structural reorganization in InP/ZnS QD photocatalysts studied via ultrafast visible and midinfrared spectroscopies

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Liu, Y., Zhou, Y., Abdellah, M. et al. Inorganic ligands-mediated hole attraction and surface structural reorganization in InP/ZnS QD photocatalysts studied via ultrafast visible and midinfrared spectroscopies. Sci. China Mater. 65, 2529–2539 (2022). https://doi.org/10.1007/s40843-021-1992-3

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  • Received: 20 December 2021

  • Accepted: 08 February 2022

  • Published: 30 March 2022

  • Issue Date: September 2022

  • DOI: https://doi.org/10.1007/s40843-021-1992-3

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Keywords

  • InP/ZnS QD photocatalysts
  • surface ligands
  • ultrafast visible spectroscopies
  • midinfrared spectroscopies
  • hole transfer
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