Liu Yanfei, Chai Yongli, Zhang Chen, Li Yanan, Zheng Yang, Xiao Ze, Li Ming, Kang Shifei, Chu Meile
Henan Chemical Industry Research Institute Co., Ltd., Henan Academy of Sciences, Zhengzhou 450052, China; Quality Inspection and Analytical Test Research Center, Henan Academy of Sciences, Zhengzhou 450008, China.
Henan Chemical Industry Research Institute Co., Ltd., Henan Academy of Sciences, Zhengzhou 450052, China.
J Colloid Interface Sci. 2025 Jul 24;700(Pt 3):138501. doi: 10.1016/j.jcis.2025.138501.
Solar-driven photocatalytic water splitting provides a sustainable route for producing green H, but there are still several challenges in its practical application, including severe recombination of photogenerated charge carriers, low separation and transfer efficiency of photogenerated electron and hole pairs, and inefficient photocatalysts. To address these issues, we successfully constructed an S-scheme CN/FTO (CN/FeTiO) heterojunction photocatalyst system based on CN (CN) and FeTiO (FTO) nanoparticles by simple hydrothermal assembly of two pre-fabricated semiconductors. Under simulated solar irradiation, the CN/FTO heterojunction exhibits significantly improved photocatalytic H production rate, reaching 607.7 μmol g h, which is 9.5- and 7.1-fold higher than pure CN and FTO, respectively. The improvement in photocatalytic efficiency is attributed to synergistic modulation of photogenerated charge transfer by the internal electric field (IEF) formed at the CN/FTO interface and intrinsic structural and electronic features of the nitrogen-rich CN. This collaboration significantly accelerates the separation and directional transfer of photogenerated charge carriers between the CN and FTO interface and within the CN itself. Based on experimental characterizations, an S-scheme photogenerated charge carrier transfer mechanism is proposed. The combined effects of the CN/FTO heterojunction IEF and the CN structural features induce favorable band bending and facilitate efficient charge separation and transfer via the S-scheme pathway, thereby enhancing photocatalytic activity. This study emphasizes the crucial role of the interfacial IEF and the intrinsic structural and electronic properties of CN in synergistically regulating the directional migration of photogenerated charge carriers. It presents insights into the dynamics of photogenerated charge migration and photocatalytic reaction control through S-scheme heterojunction engineering, particularly utilizing nitrogen-rich carbon nitrides.
太阳能驱动的光催化水分解为生产绿色氢气提供了一条可持续的途径,但在其实际应用中仍存在若干挑战,包括光生电荷载流子的严重复合、光生电子和空穴对的低分离与转移效率以及低效的光催化剂。为解决这些问题,我们通过简单水热组装两种预制半导体,成功构建了基于氮化碳(CN)和钛酸亚铁(FTO)纳米颗粒的S型CN/FTO(CN/FeTiO)异质结光催化剂体系。在模拟太阳光照下,CN/FTO异质结表现出显著提高的光催化产氢速率,达到607.7 μmol g⁻¹ h⁻¹,分别比纯CN和FTO高9.5倍和7.1倍。光催化效率的提高归因于在CN/FTO界面形成的内建电场(IEF)对光生电荷转移的协同调制以及富氮CN的固有结构和电子特性。这种协同作用显著加速了光生电荷载流子在CN和FTO界面之间以及CN自身内部的分离和定向转移。基于实验表征,提出了一种S型光生电荷载流子转移机制。CN/FTO异质结IEF和CN结构特征的综合作用导致有利的能带弯曲,并通过S型途径促进有效的电荷分离和转移,从而增强光催化活性。本研究强调了界面IEF以及CN的固有结构和电子性质在协同调节光生电荷载流子定向迁移方面的关键作用。它通过S型异质结工程,特别是利用富氮碳氮化物,揭示了光生电荷迁移动力学和光催化反应控制的见解。