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Spatial Grain Growth and Composition Evolution during Sulfurizing Metastable Wurtzite Cu2ZnSnS4 Nanocrystal-Based Coatings
Chemistry of Materials ( IF 7.2 ) Pub Date : 2017-03-01 00:00:00 , DOI: 10.1021/acs.chemmater.6b04603
Xu Liu 1 , Jialiang Huang 1 , Fangzhou Zhou 1 , Fangyang Liu 1 , John A. Stride 2 , Xiaojing Hao 1
Affiliation  

A drawback of nanocrystal-based processing, that leads to the notoriously poor crystallinity of pure-sulfide Cu2ZnSnS4 absorber, was recently reported to be effectively overcome by the annealing of thin films made from the ink of metastable wurtzite Cu2ZnSnS4 nanocrystals in a combined S and SnS atmosphere. However, the formation pathway from nanometer-sized crystals in the wurtzite phase to micrometer-sized grains with the kesterite phase during this process still lacks in-depth study. In this work, the spatial grain growth and composition evolution during the sulfurization of wurtzite nanocrystal coatings are systematically investigated by classifying samples into temperature and time series. In the process of heating up, the reversible migration of Cu and Zn species contributes to a continuous growth of kesterite Cu2ZnSnS4 grains on the surface. At higher temperature, a fast phase-transition growth from wurtzite Cu2ZnSnS4 nanoparticles to kesterite grains is also directly observed in the region away from the surface. After reaching 580 °C, the thin film experiences impressive decomposition and reorganization changes as a function of time, which cause the formation of an absorber with good crystallinity and homogeneous compositional distribution. The solar cell device, fabricated by employing this pure-sulfide Cu2ZnSnS4 absorber from wurtzite nanocrystal-based coatings, demonstrated an energy conversion efficiency of 6.0% in the absence of an antireflection coating.

中文翻译:

硫化亚稳纤锌矿Cu 2 ZnSnS 4纳米晶基涂层中的空间晶粒长大和成分演变

最近报道了基于纳米晶体的工艺的缺点,即纯硫化物Cu 2 ZnSnS 4吸收剂的结晶度极差的问题,该缺点可通过对亚稳纤锌矿Cu 2 ZnSnS 4的油墨制得的薄膜进行退火而得到有效克服。S和SnS混合气氛中形成纳米晶体。然而,在此过程中,从纤锌矿相中的纳米尺寸晶体到具有钾钛矿相的微米级晶粒的形成途径仍然缺乏深入的研究。在这项工作中,通过将样品分为温度和时间序列,系统地研究了纤锌矿纳米晶涂层硫化过程中的空间晶粒长大和成分演变。在加热过程中,Cu和Zn物种的可逆迁移有助于在表面上连续生长kesterite Cu 2 ZnSnS 4晶粒。在高温下,纤锌矿Cu 2 ZnSnS 4的快速相变生长也可以在远离表面的区域中直接观察到纳米颗粒到硅藻土颗粒。达到580°C后,薄膜会经历令人印象深刻的分解和重组变化(随时间变化),从而导致形成具有良好结晶度和均一组成分布的吸收剂。通过使用由纤锌矿纳米晶体基涂层制成的这种纯硫化物Cu 2 ZnSnS 4吸收剂制造的太阳能电池器件在不存在抗反射涂层的情况下显示出6.0%的能量转换效率。
更新日期:2017-03-01
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