ALD Al_2O_3改性量子点敏化TiO_2纳米管阵列的制备及其光电性能提升
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摘要
CdS和PbS量子点是一种很具发展潜力的宽带隙半导体的共敏化剂,但是存在界面空穴转移速率小、可见光区的内量子效率低等需要解决的技术瓶颈。用原子层沉积技术(Atomic layer deposition,ALD)在量子点敏化TiO_2纳米管阵列结构的外表面沉积一层均匀、保形性好的超薄Al_2O_3覆盖层,能大幅提高电极的光电性能。在100 mW cm~(-2)的模拟太阳光照下,沉积了30个ALD周期Al_2O_3层的光电极显示出了最高的光电流密度5.19 mA cm~(-2),是纯TiO_2纳米管阵列电极的52倍,比未经Al_2O_3修饰的量子点敏化TiO_2纳米管阵列的光电流密度提升了60%。并且,光电转换效率(IPCE)在350 nm处高达83%,在450 nm波长以下均高于30%。系统研究超薄Al_2O_3包覆层对量子点敏化电极的作用后发现,ALD包覆Al_2O_3层能显著降低界面电荷转移阻抗、提高载流子浓度、以及增强电极稳定性,同时发挥表面钝化、场效应钝化和表面电荷效应的协同作用。该方法简单方便,非常适用于光电化学分解水高性能光电极的研发和优化。
Al_2O_3 overcoating by atomic layer deposition(ALD) can drastically enhance the photoelectrochemical performance of the quantum dot-sensitized TiO_2 nanotube arrays. 30 ALD cycles of Al_2O_3 overlayer can achieve a good balance between surface coverage and charge transfer resistance. The resulting maximum photocurrent density of 5.19 mA cm~(-2) under simulated solar illumination has a 52 times improvement on the pure TiO_2 nanotube arrays, and a 60% enhancement over bare quantum dot-sensitized TNTAs. The IPCE can reach the record value of 83% at 350 nm. Systematic examination of the role of the ALD Al_2O_3 overlayer indicates that surface recombination passivation, catalytic improvement in interfacial charge transfer kinetics, and chemical stabilization might synergistically enhance the photoelectrochemical performance in the visible region.
引文
[1]Zeng,M;Peng,X;Liao,J;Wang,G;Li,Y;Li,J;Qin,Y;Wilson,J;Song,A;Lin,S.Phys.Chem.Chem.Phys.2016,accepted.
    [2]Zhang,X;Zeng,M;Zhang,J;Song,A;Lin,S.RSC Adv.2016,6:8118.
    [3]Zhang,X;Lin,S;Liao,J;Pan,N;Li,D;Cao,X;Li,J.Electrochim.Acta.2013,108:296.

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