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

• Published in: Advanced materials (Weinheim) 2024-11, p.e2415138
• Main Authors: Dan, Meng, Yu, Shan, Lin, Weihua, Abdellah, Mohamed, Guo, Zhen, Liu, Zhao-Qing, Pullerits, Tõnu, Zheng, Kaibo, Zhou, Ying
• Format: Article
• Language: English
• Subjects: Chemical Sciences; Kemi; Materialkemi; Materials Chemistry; Natural Sciences; Naturvetenskap
• ISSN: 0935-9648; 1521-4095; 1521-4095
• DOI: 10.1002/adma.202415138

Solar-driven photocatalytic green hydrogen (H ) 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 H production, withthe H production rate of 55.61 mmol h g 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.