State Key Laboratory of Environmental Chemistry and Eco-toxicology, Research Centre for Eco-environmental Sciences, Chinese Academy of Sciences , 18 Shuangqing Road, P.O. Box 2871, Beijing 100085, China.
ACS Appl Mater Interfaces. 2013 Dec 26;5(24):13035-41. doi: 10.1021/am403937y. Epub 2013 Dec 12.
A graphene-based two-dimensional (2D) nanoplatform provides new opportunities for fabricating 2D heterojunction interfaces to fortify charge transfer in semiconductor assemblies. In this report, TiO2 nanosheet/graphene composite based 2D-2D heterojunctions were fabricated by a solvothermal process. Microscopic and spectroscopic characterization revealed a homogeneous sheetlike morphology with intimate interfacial contact between the TiO2 nanosheet and graphene due to chemical interactions. Compared with 0D-2D Degussa P25 (TiO2)/graphene and 1D-2D TiO2 nanotube/graphene composites, the 2D-2D TiO2 nanosheet/graphene hybrid demonstrated higher photocatalytic activity toward the degradation of rhodamine B and 2,4-dichlorophenol under UV irradiation. Radical trapping and ESR experiments revealed the enhanced generation of ·OH and O2(•-) in the 2D-2D heterojunction system. By analyzing TiO2 excited state deactivation lifetime, the interfacial electron transfer rates determined for 0D-2D, 1D-2D, and 2D-2D TiO2/graphene composites were 1.15 × 10(8) s(-1), 3.47 × 10(8) s(-1), and 1.06 × 10(9) s(-1), respectively. It was therefore proposed that the fast charge separation in the TiO2 nanosheet/graphene photocatalyst promoted the generation of reactive oxygen species and enhanced the photodegradation reactions. The results underscore the key role of nanomaterial dimensionality in interfacial charge transfer processes.
基于石墨烯的二维(2D)纳米平台为制造二维异质结界面提供了新的机会,以增强半导体组件中的电荷转移。在本报告中,通过溶剂热法制备了 TiO2 纳米片/石墨烯复合二维-二维异质结。微观和光谱特性揭示了由于化学相互作用,TiO2 纳米片和石墨烯之间具有均匀的片状形态和紧密的界面接触。与 0D-2D Degussa P25(TiO2)/石墨烯和 1D-2D TiO2 纳米管/石墨烯复合材料相比,2D-2D TiO2 纳米片/石墨烯杂化在紫外光照射下对罗丹明 B 和 2,4-二氯苯酚的降解表现出更高的光催化活性。自由基捕获和 ESR 实验表明,在 2D-2D 异质结体系中增强了·OH 和 O2(•-)的生成。通过分析 TiO2 激发态失活寿命,确定 0D-2D、1D-2D 和 2D-2D TiO2/石墨烯复合材料的界面电子转移速率分别为 1.15×10(8)s(-1)、3.47×10(8)s(-1)和 1.06×10(9)s(-1)。因此,提出 TiO2 纳米片/石墨烯光催化剂中快速的电荷分离促进了活性氧物质的生成,并增强了光降解反应。研究结果强调了纳米材料维度在界面电荷转移过程中的关键作用。