Room-temperature synthesis of lead-free copper(I)-antimony(III)-based double perovskite nanocrystals

材料科学 钙钛矿(结构) 纳米晶 带隙 亚稳态 化学工程 纳米技术 无机化学 光电子学 化学 有机化学 冶金 工程类
作者
Shizhe Wang,Dan Han,Clément Maheu,Zehua Xu,Alexander Biewald,Hannah Illner,Rik Hooijer,Thomas Mayer,Achim Hartschuh,H. Ebert,Thomas Bein
出处
期刊:APL Materials [American Institute of Physics]
卷期号:11 (4) 被引量:7
标识
DOI:10.1063/5.0144708
摘要

In the field of perovskite solar cells, explorations of new lead-free all-inorganic perovskite materials are of great interest to address the instability and toxicity issues of lead-based hybrid perovskites. Recently, copper-antimony-based double perovskite materials have been reported with ideal band gaps, which possess great potential as absorbers for photovoltaic applications. Here, we synthesize Cs2CuSbCl6 double perovskite nanocrystals (DPNCs) at ambient conditions by a facile and fast synthesis method, namely, a modified ligand-assisted reprecipitation method. We choose methanol as a solvent for precursor salts as it is less toxic and easily removed in contrast to widely used dimethylformamide. Our computational structure search shows that the Cs2CuSbCl6 structure containing alternating [CuCl6]5− and [SbCl6]3− octahedral units is a metastable phase that is 30 meV/atom higher in energy compared to the ground state structure with [CuCl3]2− and [SbCl6]3− polyhedra. However, this metastable Cs2CuSbCl6 double perovskite structure can be stabilized through solution-based nanocrystal synthesis. Using an anion-exchange method, Cs2CuSbBr6 DPNCs are obtained for the first time, featuring a narrow bandgap of 0.9 eV. Finally, taking advantage of the solution processability of DPNCs, smooth and dense Cs2CuSbCl6 and Cs2CuSbBr6 DPNC films are successfully fabricated.
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