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Balancing the Charge Separation and Surface Reaction Dynamics in Twin‐Interface Photocatalysts for Solar‐to‐Hydrogen Production

Dan, Meng LU ; Yu, Shan ; Lin, Weihua LU ; Abdellah, Mohamed LU ; Guo, Zhen ; Liu, Zhao‐Qing ; Pullerits, Tõnu LU ; Zheng, Kaibo LU and Zhou, Ying (2025) In Advanced Materials 37(5).
Abstract
Solar-driven photocatalytic green hydrogen (H2) evolution reaction presents a promising route toward solar-to-chemical fuel conversion. However, its efficiency has been hindered by the desynchronization of fast photogenerated charge carriers and slow surface reaction kinetics. This work introduces a paradigm shift in photocatalyst design by focusing on the synchronization of charge transport and surface reactions through the use of twin structures as a unique platform. With CdS twin structure (CdS-T) as a model, the role of twin boundaries in modulating surface reactions and facilitating charge migration is systematically investigated. Utilizing transient absorption (TA) and time-resolved infrared (TRIR) spectroscopies, it is revealed that... (More)
Solar-driven photocatalytic green hydrogen (H2) evolution reaction presents a promising route toward solar-to-chemical fuel conversion. However, its efficiency has been hindered by the desynchronization of fast photogenerated charge carriers and slow surface reaction kinetics. This work introduces a paradigm shift in photocatalyst design by focusing on the synchronization of charge transport and surface reactions through the use of twin structures as a unique platform. With CdS twin structure (CdS-T) as a model, the role of twin boundaries in modulating surface reactions and facilitating charge migration is systematically investigated. Utilizing transient absorption (TA) and time-resolved infrared (TRIR) spectroscopies, it is revealed that CdS-T achieves charge separation on a picosecond timescale and, importantly, the surface reaction at the twin boundary with the involvement of holes also occurs within 100 ps to 3 ns. This synchronization of charge donation and surface regeneration significantly enhances the hydrogen evolution process. Accordingly, CdS-T exhibits superior activity for visible light photocatalytic H2 production, withthe H2 production rate of 55.61 mmol h−1 g−1 and remarkable stability (>30 h), outperforming pristine CdS significantly. This study underscores the transformative potential of twin structures in photocatalysis, offering a new avenue to synchronize charge transport and surface reactions. (Less)
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author
; ; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Advanced Materials
volume
37
issue
5
article number
2415138
publisher
John Wiley & Sons Inc.
external identifiers
  • pmid:39558773
  • scopus:85209799557
ISSN
1521-4095
DOI
10.1002/adma.202415138
language
English
LU publication?
yes
id
d70df0eb-c0ed-447f-a7c3-54846fa1eb35
date added to LUP
2024-12-03 14:57:21
date last changed
2025-04-04 14:19:42
@article{d70df0eb-c0ed-447f-a7c3-54846fa1eb35,
  abstract     = {{Solar-driven photocatalytic green hydrogen (H2) evolution reaction presents a promising route toward solar-to-chemical fuel conversion. However, its efficiency has been hindered by the desynchronization of fast photogenerated charge carriers and slow surface reaction kinetics. This work introduces a paradigm shift in photocatalyst design by focusing on the synchronization of charge transport and surface reactions through the use of twin structures as a unique platform. With CdS twin structure (CdS-T) as a model, the role of twin boundaries in modulating surface reactions and facilitating charge migration is systematically investigated. Utilizing transient absorption (TA) and time-resolved infrared (TRIR) spectroscopies, it is revealed that CdS-T achieves charge separation on a picosecond timescale and, importantly, the surface reaction at the twin boundary with the involvement of holes also occurs within 100 ps to 3 ns. This synchronization of charge donation and surface regeneration significantly enhances the hydrogen evolution process. Accordingly, CdS-T exhibits superior activity for visible light photocatalytic H2 production, withthe H2 production rate of 55.61 mmol h−1 g−1 and remarkable stability (>30 h), outperforming pristine CdS significantly. This study underscores the transformative potential of twin structures in photocatalysis, offering a new avenue to synchronize charge transport and surface reactions.}},
  author       = {{Dan, Meng and Yu, Shan and Lin, Weihua and Abdellah, Mohamed and Guo, Zhen and Liu, Zhao‐Qing and Pullerits, Tõnu and Zheng, Kaibo and Zhou, Ying}},
  issn         = {{1521-4095}},
  language     = {{eng}},
  number       = {{5}},
  publisher    = {{John Wiley & Sons Inc.}},
  series       = {{Advanced Materials}},
  title        = {{Balancing the Charge Separation and Surface Reaction Dynamics in Twin‐Interface Photocatalysts for Solar‐to‐Hydrogen Production}},
  url          = {{http://dx.doi.org/10.1002/adma.202415138}},
  doi          = {{10.1002/adma.202415138}},
  volume       = {{37}},
  year         = {{2025}},
}