热退火气氛对溶液法制备的Sb2S3薄膜组成、 结构及光伏性能的影响

doi:10.7503/cjcu20180482

高等学校化学学报 ›› 2019, Vol. 40 ›› Issue (2): 342.doi: 10.7503/cjcu20180482

热退火气氛对溶液法制备的Sb₂S₃薄膜组成、结构及光伏性能的影响

齐娟娟^1,², 董超^1,², Getinet Y. Ashebir^1,², 陈俊伟^1,², 万智阳^1,², 陈王伟^1,², 赵秋原^1,², 王命泰¹()

1. 中国科学院合肥物质科学研究院应用技术研究所, 合肥 230031
2. 中国科学技术大学研究生院科学岛分院, 合肥 230026

收稿日期:2018-07-05 出版日期:2019-02-10 发布日期:2018-12-18
作者简介:
联系人简介: 王命泰, 男, 博士, 研究员, 博士生导师, 主要从事太阳电池材料与器件性能方面的研究. E-mail: mtwang@ipp.ac.cn
基金资助:
国家自然科学基金(批准号: 11274307, 91333121, 11474286)、安徽省科技攻关计划项目(批准号: 1604a0902148)和合肥物质科学技术中心重要/创新项目培育基金(批准号: 2016FXZY003)资助

Effects of Annealing Atmosphere on Composition, Structure and Photovoltaic Properties of Solution-processed Sb₂S₃ Thin Films^†

QI Juanjuan^1,², DONG Chao^1,², Getinet Y. Ashebir^1,², CHEN Junwei^1,², WAN Zhiyang^1,², CHEN Wangwei^1,², ZHAO Qiuyuan^1,², WANG Mingtai^1,^*()

1. Institute of Applied Technology, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei 230031, China
2. Science Island Branch of Graduate School, University of Science and Technology of China, Hefei 230026, China

Received:2018-07-05 Online:2019-02-10 Published:2018-12-18
Contact: WANG Mingtai E-mail:mtwang@ipp.ac.cn
Supported by:
† Supported by the National Natural Science Foundation of China(Nos.11274307, 91333121, 11474286), the Science and Technology Project of Auhui Province, China(No.1604a0902148) and the Major/Innovative Program of Development Foundation of Hefei Center for Physical Science and Technology, China(No.2016FXZY003)

摘要/Abstract

摘要：

采用化学浴(CBD)法在TiO₂薄膜表面制备结晶性Sb₂S₃膜层, 获得了TiO₂/Sb₂S₃平板异质结, 并结合聚[2,6-{4,4-双-(2-乙基己基)-4H-环戊并[2,1-b;3,4-b']-二噻吩}-交替-4,7-(2,1,3-苯并噻二唑)](PCPDTBT)空穴传输层和MoO₃电极界面修饰层, 制备了FTO/TiO₂/Sb₂S₃/PCPDTBT/MoO₃/Au平板结构太阳能电池, 研究了CBD方法中热退火气氛对Sb₂S₃薄膜的组成、结构及光伏性能的影响. 结果表明, 在N₂气氛下退火时, 所得的Sb₂S₃膜层不致密且含有Sb₂O₃杂相, 电池效率仅为0.90%; 而在N₂-S气氛下退火时, 硫会与杂相Sb₂O₃发生反应生成Sb₂S₃, 进而得到纯净、致密、平整的结晶Sb₂S₃膜层. 在平板结构太阳能电池中, 光生空穴对电池光电流的产生有明显的贡献; 随着Sb₂O₃杂相的消除, Sb₂S₃薄膜中载流子的复合减少且传输速率增大, 使太阳能电池器件中电子与空穴的收集效率和短路电流显著提高, 电池效率提高了1.34倍, 达到2.04%.

关键词: 三硫化二锑, 化学浴沉积, 热退火气氛, 太阳能电池

Abstract:

Chemical bath deposition(CBD) method was used to deposit Sb₂S₃ on condensed TiO₂ film to prepare TiO₂/Sb₂S₃ planar heterojunction, and the FTO/TiO₂/Sb₂S₃/PCPDTBT/MoO₃/Au planar devices were fabricated with poly[2,6-{4,4-bis-(2-ethylhexyl)-4H-cyclopenta[2,1-b;3,4-b']-dithiophene}-alt-4,7-(2,1,3-benzothiadiazole)](PCPDTBT) hole transporting layer and MoO₃ interfacial layer to modify Au electrode. The effects of annealing atmospheres on the composition, structure and photovoltaic properties of solution-processed Sb₂S₃ thin films were investigated. The results show that the cell efficiency only reaches 0.90% when the TiO₂/Sb₂S₃ film is annealed in N₂ atmosphere due to the presence of Sb₂O₃ secondary phase and a poor compactness in the resulting Sb₂S₃ thin film, while the smooth, well condensed and pure Sb₂S₃ thin film is obtained when annealing the TiO₂/Sb₂S₃ film in N₂-S atmosphere, leading to the elimination of Sb₂O₃ secondary phase and a significant increase in efficiency by 1.34 folds to 2.04%. It is found that the removal of Sb₂O₃ impurity reduces the charge recombination and facilitates the transport and collection efficiency of both electron and holes in bulk Sb₂S₃ layer, leading to improved device performance.

Key words: Sb₂S₃, Chemical bath deposition, Annealing atmosphere, Solar cell

中图分类号:

O646
O614

TrendMD:

齐娟娟, 董超, Getinet Y. Ashebir, 陈俊伟, 万智阳, 陈王伟, 赵秋原, 王命泰. 热退火气氛对溶液法制备的Sb₂S₃薄膜组成、结构及光伏性能的影响. 高等学校化学学报, 2019, 40(2): 342.

QI Juanjuan,DONG Chao,Getinet Y. Ashebir,CHEN Junwei,WAN Zhiyang,CHEN Wangwei,ZHAO Qiuyuan,WANG Mingtai. Effects of Annealing Atmosphere on Composition, Structure and Photovoltaic Properties of Solution-processed Sb₂S₃ Thin Films^†. Chem. J. Chinese Universities, 2019, 40(2): 342.

图/表 7

Fig.1 Architecture of solar cell

Fig.2 XRD patterns of TiO2(a), TiO2/Sb2S3(Am)(b), TiO2/Sb2S3(N2-S)(c) and TiO2/Sb2S3(N2)(d) filmsFor pattern a, ▲ indicates the XRD peak of anatase TiO2, other peaks are of FTO substrate.

Fig.3 XPS spectra of Sb3d of TiO2/Sb2S3(Am)(a), TiO2/Sb2S3(N2-S)(b) and TiO2/Sb2S3(N2)(c)

Fig.4 UV-Vis absorption spectra of TiO2/Sb2S3(Am)(a),TiO2/Sb2S3(N2)(b) and TiO2/Sb2S3(N2-S)(c)The inset shows the absorption spectrum of PCPDTBT film.

Fig.5 Sectional SEM images of TiO2/Sb2S3(Am)(A),TiO2/Sb2S3(N2)(B) and TiO2/Sb2S3(N2-S)(C)

Fig.6 J-V curves(A), IPCE spectra(B), band level alignments(C) and IMPS spectra(D) of the solar cells based on TiO2/Sb2S3(N2) and TiO2/Sb2S3(N2-S) heterojunctionsThe dotted line in (D) shows the tendency of IMPS response to reach III quadrant when the frequency is above 100 kHz that is beyond the frequency limit of our CIMPS system.

Table 1 Device performance under AM1.5 illumination*

Annealing atmosphere	V_oc/V	J_sc/(mA·cm^-2)	FF(%)	η(%)	R_s/kΩ	R_sh/kΩ	τ_D/μs
N₂	0.45±0.03	6.20±0.39	32.54±0.19	0.90±0.08	1.08±0.12	3.04±0.28	12.00±0.00
N₂-S	0.45±0.03	12.59±0.47	36.36±1.27	2.04±0.09	0.44±0.05	2.15±0.16	7.00±1.00

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热退火气氛对溶液法制备的Sb₂S₃薄膜组成、结构及光伏性能的影响

Effects of Annealing Atmosphere on Composition, Structure and Photovoltaic Properties of Solution-processed Sb₂S₃ Thin Films^†

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