物理化学学报

所属专题： 太阳能转化与储存

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雾化水诱导表面重构的高效碳基全无机CsPbBr3钙钛矿太阳电池

陈大正1,2, 何逸冰1, 王子昊1, 张泽雨林1, 王之哲3, 田百川1, 张亚男1, 巴延双1, 朱卫东1,2, 周龙1,2, 习鹤1,2, 张春福1,2, 张进成1, 郝跃1   

  1. 1 西安电子科技大学, 集成电路学部, 宽禁带半导体器件与集成技术全国重点实验室, 陕西 西安 710071;
    2 西安电子科技大学广州研究院, 广州第三代半导体创新中心, 广东 广州 510555;
    3 中国电子产品可靠性与环境试验研究所, 电子元器件可靠性物理与应用技术重点实验室, 广东 广州 511370
  • 收稿日期:2025-09-29 修回日期:2025-11-14 录用日期:2025-11-14
  • 通讯作者: 陈大正, 张春福 E-mail:dzchen@xidian.edu.cn;cfzhang@xidian.edu.cn
  • 基金资助:
    国家自然科学基金(62274126, 62474131, 62204189)资助项目

Mist-water-induced surface reconstruction for efficient carbon-based inorganic CsPbBr3 perovskite solar cells

Dazheng Chen1,2, Yibing He1, Zihao Wang1, Zeyulin Zhang1, Zhizhe Wang3, Baichuan Tian1, Yanan Zhang1, Yanshuang Ba1, Weidong Zhu1,2, Long Zhou1,2, He Xi1,2, Chunfu Zhang1,2, Jincheng Zhang1, Yue Hao1   

  1. 1 State Key Laboratory of Wide Bandgap Semiconductor Devices and Integrated Technology, Faculty of Integrated Circuit, Xidian University, Xi'an 710071, Shaanxi Province, China;
    2 Guangzhou Wide Bandgap Semiconductor Innovation Center, Guangzhou Institute of Technology, Xidian University, Guangzhou 510555, Guangdong Province, China;
    3 Science and Technology on Reliability Physics and Application of Electronic Component Laboratory, China Electronic Product Reliability and Environmental Testing Research Institute, Guangzhou 511370, Guangdong Province, China
  • Received:2025-09-29 Revised:2025-11-14 Accepted:2025-11-14
  • Contact: Dazheng Chen, Chunfu Zhang E-mail:dzchen@xidian.edu.cn;cfzhang@xidian.edu.cn

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摘要： 溶液法制备的全无机三溴化铯铅(CsPbBr3)钙钛矿薄膜通常存在大量表面缺陷且粗糙度较高，导致太阳电池开路电压损失较大、光电转换效率偏低。本文提出并实现了一种高效、可扩展的水雾诱导CsPbBr3薄膜表面重构策略，通过低成本、非真空的雾化学气相沉积(Mist-CVD)设备完成了工艺开发与参数优化。根据莱顿弗罗斯特效应原理，雾化后的水微粒可在高温CsPbBr3表面诱发钙钛矿分解和结晶反应，在雾化表面处理最优条件下(275 ℃，30 min)，实现了高质量CsPbBr3薄膜的重构。系统的微观结构、光学与电学表征证实：经雾化表面处理的CsPbBr3薄膜具有更纯钙钛矿相、更低表面粗糙度、更强光吸收、更长载流子寿命、更低缺陷密度及更高效的载流子传输。得益于CsPbBr3薄膜结晶质量与均匀性的提升，碳基太阳电池的光电转换效率、长期稳定性、工艺重复性得到显著改善，制备的小面积(9 mm2)器件效率从9.14%提升至10.06%，开路电压从1.40 V提升至1.50 V，对应大面积(0.6 cm2)器件效率可达8.11%，且在空气中存放30天后器件初始效率衰减小于10%。这种基于Mist-CVD的雾化处理的CsPbBr3表面重构方法为突破CsPbBr3器件效率瓶颈并推动其商业化提供了新途径。

关键词: CsPbBr3, 表面重构, 水, 雾化化学气相沉积, 钙钛矿太阳能电池

Abstract: With the high absorption coefficient, simple preparation method, and the best stability in the halide perovskites, all-inorganic cesium-lead-bromide (CsPbBr3) has attracted increasing attentions in the photovoltaic solar cells. However, the solution-processed CsPbBr3 films usually have many surface defects and large roughness, leading to large open-circuit voltage (VOC) loss and relatively poor efficiency in solar cells. Thus, an effective surface treatment method is highly anticipated to improve the film quality and device performance. It is known that water is one of the most important causes of perovskite decomposition, it can also be used to adjust the crystallization and growth of perovskite films, and the key lies in how to direct the role of water during perovskite formation. In this paper, an efficient and scalable strategy of water-mist-induced surface reconstruction for CsPbBr3 films was proposed and realized by a low-cost, vacuum-free mist chemical vapor deposition (Mist-CVD) system. Inspired by the Leidenfrost effect principle, the water-induced reactions of decomposition and crystallization occur on the local high-temperature surface of CsPbBr3. This reconstruction produced the high-quality CsPbBr3 films at an optimal treat condition of 275 ℃ for 30 min. According to the X-Ray diffraction (XRD) results, the mist treatment could boost the phase transform from impurity phases (Cs4PbBr6, CsPb2Br5) to CsPbBr3 and the film surface obtained the purest CsPbBr3 phase. The atomic force microscope (AFM) tests showed that the surface roughness of target film was reduced from 29.8 nm to 12.7 nm. And the laser scanning confocal microscopy (LSCM) images (4 mm×4 mm) verified the enhanced uniformity of CsPbBr3 film with mist-treatment. Combined with the higher light absorption and longer carrier lifetime, the carbon-based solar cells achieved the improvement of average power conversion efficiency (PCE) from 8.26% to 9.64%, with the champion VOC of 1.50 V and PCE of 10.06%@9 mm2 (8.11%@0.6 cm2). The PCE could maintain over 90% of the original values after 30 days stored in ambient air (20 ℃, 40% RH). The devices also presented better repeatability and steady outputs performance. The statistical results demonstrated that this mist-treatment could improve all photovoltaic parameters and the higher VOC was mainly responsible for the enhanced PCE. Therefore, the Mist-CVD water treatment could reconstruct the CsPbBr3 films with low-defect and smooth surface, which paves the way to further break the efficiency bottleneck of CsPbBr3 perovskite solar cells and promotes the commercialization in the future.

Key words: CsPbBr3, Surface reconstruction, Water, Mist chemical vapor deposition, Perovskite solar cells