Wu Kaifeng, Li Qiuyang, Du Yongling, Chen Zheyuan, Lian Tianquan
Department of Chemistry , Emory University , Atlanta , Georgia 30322 , USA . Email:
Chem Sci. 2015 Feb 1;6(2):1049-1054. doi: 10.1039/c4sc02994a. Epub 2014 Nov 4.
Two-dimensional (2-D) semiconductor nanomaterials are receiving tremendous research interests due in part to their attractive light absorption and charge transport properties. Integration of catalytic metal nanoparticles with these 2-D semiconductors can potentially lead to new photocatalytic nanoheterostructures for efficient solar-to-fuel conversion. Here we report the synthesis and transient absorption study of colloidal quantum confined CdSe nanosheets with a Pt nanoparticle at the edge or vertex. Due to the large in-plane exciton mobility, ∼86.6 ± 0.5% of excitons generated in CdSe sheets can be transported to NS-Pt interface and quenched by energy transfer to Pt (with a half-life <150 fs). The remaining excitons (13.4 ± 0.5%) become localized due to fast hole trapping and can be dissociated by interfacial electron transfer to Pt (with a half life of ∼9.4 ± 0.7 ps). The resulting charge-separated states (with electrons in Pt and trapped holes in CdSe) are long-lived (half life of ∼75 ± 14 ns), suggesting possible applications for solar driven H generation.
二维(2-D)半导体纳米材料正受到极大的研究关注,部分原因在于其具有吸引人的光吸收和电荷传输特性。将催化金属纳米颗粒与这些二维半导体相结合,有可能产生用于高效太阳能到燃料转换的新型光催化纳米异质结构。在此,我们报告了在边缘或顶点带有铂纳米颗粒的胶体量子限域CdSe纳米片的合成及瞬态吸收研究。由于面内激子迁移率高,在CdSe片中产生的约86.6±0.5%的激子能够传输到纳米片 - 铂界面,并通过能量转移至铂而猝灭(半衰期<150飞秒)。其余的激子(13.4±0.5%)由于快速的空穴俘获而局域化,并可通过界面电子转移至铂而解离(半衰期约为9.4±0.7皮秒)。由此产生的电荷分离态(电子在铂中,空穴被俘获在CdSe中)具有长寿命(半衰期约为75±14纳秒),这表明其在太阳能驱动制氢方面可能具有应用前景。