Zhong Fengyi, Sheng Jianping, Du Chenyu, He Ye, Zhang Fengying, Sun Yanjuan, Zhou Ying, Dong Fan
School of Resources and Environment, University of Electronic Science and Technology of China, Chengdu, 611731, China.
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, 611731, China.
Adv Sci (Weinh). 2025 Mar;12(9):e2410437. doi: 10.1002/advs.202410437. Epub 2025 Jan 10.
Heterojunctions, known for their decent separation of photo-generated electrons and holes, are promising for photocatalytic CO reduction. However, a significant obstacle in traditional post-assembled heterojunctions is the high interfacial barrier for charge transfer caused by atomic lattice mismatch at multiphase interfaces. Here, as research prototypes, the study creates a lattice-matched co-atomic interface within CsPbBr-CsPbBr polytypic nanocrystals (113-125 PNs) through the proposed in situ hybrid strategy to elucidate the underlying charge transfer mechanism within this unique interface. Compared to CsPbBr nanocrystals, the 113-125 PNs exhibit a remarkable 3.6-fold increase in photocatalytic CO reduction activity (173.3 µmol g within 5 h). Furthermore, Kelvin probe force microscopy results reveal an increase in the built-in electric field within this lattice-matched co-atomic interface from 43.5 to 68.7 mV, providing a stronger driving force for charge separation and directional migration. Additionally, ultrafast transient absorption spectroscopy uncovers the additional charge carrier transfer pathways across this lattice-matched co-atomic interface. Thus, this unique co-atomic interface significantly promotes the interfacial electronic coupling and mitigates the charge transfer barrier, thus facilitating efficient charge separation and transfer. These insights underscore the importance of interfacial structure in heterojunction design and comprehending the intricate interplay between interface and carrier dynamics.
异质结以其对光生电子和空穴的良好分离而闻名，在光催化CO还原方面具有广阔前景。然而，传统后组装异质结的一个重大障碍是多相界面处原子晶格失配导致的电荷转移界面势垒较高。在此，作为研究原型，该研究通过所提出的原位杂化策略在CsPbBr - CsPbBr多型纳米晶体（113 - 125 PNs）内创建了一个晶格匹配的共原子界面，以阐明该独特界面内潜在的电荷转移机制。与CsPbBr纳米晶体相比，113 - 125 PNs的光催化CO还原活性显著提高了3.6倍（5小时内达到173.3 µmol g）。此外，开尔文探针力显微镜结果显示，该晶格匹配的共原子界面内的内建电场从43.5 mV增加到68.7 mV，为电荷分离和定向迁移提供了更强的驱动力。此外，超快瞬态吸收光谱揭示了跨该晶格匹配共原子界面的额外电荷载流子转移途径。因此，这种独特的共原子界面显著促进了界面电子耦合并降低了电荷转移势垒，从而促进了有效的电荷分离和转移。这些见解强调了界面结构在异质结设计中的重要性以及理解界面与载流子动力学之间复杂相互作用的重要性。
