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2026 26040107

DOI: https://doi.org/10.6023/A26040107

研究论文

二硫化甲脒二盐酸盐的界面工程实现FAPbBr3钙钛矿太阳能电池缺陷钝化

  • 汪佳艳 ,
  • 郭焕焕 ,
  • 殷逍遥 ,
  • 王宇鸿 ,
  • 朱文昊 ,
  • 张闽粤 ,
  • 杨琛 ,
  • 吴季怀 ,
  • 孙伟海
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  • a华侨大学材料科学与工程学院 物理化学研究所,环境友好功能材料教育部工程研究中心,福建省光电功能材料重点实验室,福建,厦门 361021;
    b邢台学院化学工程与生物技术学院,河北省固态电池材料与先进装备制造实验室河北,邢台,054001;
    c中国科学院新疆理化技术研究所,能源与化工工程研究中心,新疆 乌鲁木齐 830011;
    d中国科学院大学,北京 100049

收稿日期: 2026-04-06

  网络出版日期: 2026-08-19

基金资助

国家自然科学基金(No.61804058),华侨大学中青年教师科研提升资助计划(ZQN-706),河北省教育厅科学研究项目(BJK2022068),河北省引进留学人员资助项目(C20220306),邢台学院教育教学研究与实践项目(JGZ24002)

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Interfacial Engineering of Formamidinium Disulfide Dihydrochloride for Defect Passivation in FAPbBr3 Perovskite Solar Cells

  • Wang Jiayan ,
  • Guo Huanhuan ,
  • Yin Xiaoyao ,
  • Wang Yuhong ,
  • Zhu Wenhao ,
  • Zhang Minyue ,
  • Yang Chen ,
  • Wu Jihuai ,
  • Sun Weihai
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  • aEngineering Research Center of Environment-Friendly Functional Materials, Ministry of Education, Fujian Key Laboratory of Photoelectric Functional Materials,Materials Science and Engineering College,Institute of Materials Physical Chemistry, Huaqiao University, Xiamen, 361021, China;
    bSchool of Chemical Engineering and Biotechnology, Xingtai University,Hebei Solid-State Battery Materials and Advanced Equipment Manufacturing Lab, Xingtai, Hebei,054001, China;
    cResearch Center for Energy and Chemical Engineering, Xinjiang Technical Institute of Physics andChemistry, Chinese Academy of Sciences, Urumqi 830011, China;
    dUniversity of Chinese Academy of Sciences (UCAS), Beijing, 100049, China

Received date: 2026-04-06

  Online published: 2026-08-19

Supported by

National Natural Science Foundation of China (No. 61804058),Young and Middle-aged Teachers' Scientific Research Promotion Program of Huaqiao University (ZQN-706),Scientific Research Project of the Education Department of Hebei Province (BJK2022068),Overseas Returnees Support Program of Hebei Province (C20220306),Education and Teaching Research and Practice Project of Xingtai University (JGZ24002)

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摘要

FAPbBr3钙钛矿太阳能电池(PSCs)凭借优异的带隙可调性、晶格稳定性及缺陷钝化潜力,已成为叠层电池中宽带隙顶电池的重要候选。然而,受PbBr2低溶解度及Br⁻半径较小影响,其结晶过程难以有效调控,易引入体相与界面缺陷,导致载流子非辐射复合增强,限制器件光电转换效率(PCE)的进一步提升。针对上述问题,本文采用界面工程策略,在钙钛矿层与碳电极之间引入二硫化甲脒二盐酸盐(FDD)界面层,通过二硫键与甲脒基团协同实现双重缺陷钝化。结果表明,FDD不仅有效降低界面缺陷密度,还显著改善薄膜结晶质量与晶粒尺寸,降低表面粗糙度,提高相纯度与致密性,从而优化载流子传输行为。最终,器件PCE由8.77%提升至11.25%,在当前FAPbBr3无空穴体系中具有较高竞争力。

关键词： 二硫化甲脒二盐酸盐; 界面工程; 两步旋涂; 缺陷钝化; FAPbBr3钙钛矿太阳能电池

本文引用格式

汪佳艳 , 郭焕焕 , 殷逍遥 , 王宇鸿 , 朱文昊 , 张闽粤 , 杨琛 , 吴季怀 , 孙伟海 . 二硫化甲脒二盐酸盐的界面工程实现FAPbBr3钙钛矿太阳能电池缺陷钝化[J]. 化学学报, 2026 : 26040107 . DOI: 10.6023/A26040107

Abstract

Wide-bandgap bromide perovskites, exemplified by FAPbBr3, have emerged as indispensable components in tandem photovoltaics and semi-transparent solar cells, owing to their large bandgap, elevated theoretical open-circuit voltage, and enhanced environmental robustness relative to iodide-based analogues. Nevertheless, the practical efficiency of FAPbBr3 devices remains markedly below their theoretical ceiling, largely constrained by poorly regulated crystallization dynamics during film formation. The intrinsically low solubility of PbBr2, coupled with the rapid conversion kinetics of bromide systems, frequently induces incomplete phase transformation and microstructural heterogeneity, thereby generating pervasive bulk and interfacial defects. These defects act as dominant nonradiative recombination centers, undermining carrier lifetime and operational stability, particularly in carbon-electrode architectures.
To address these limitations, a molecularly engineered interfacial strategy is developed by introducing formamidinium disulfide dihydrochloride (FDD) as a functional interlayer between the FAPbBr3 absorber and the carbon electrode. The FAPbBr3 films are constructed via a two-step spin-coating protocol, followed by the deposition of an ultrathin FDD modification layer. Notably, the molecular configuration of FDD enables a cooperative dual-site passivation mechanism: sulfur-containing groups exhibit strong coordination with undercoordinated Pb2+ species, while the formamidinium moieties contribute to surface defect passivation through intermolecular interactions.This synergistic interaction effectively suppresses interfacial defect formation and modulates crystallization behavior, leading to concurrent improvements in structural order and electronic quality.
A suite of structural, optical, and electrical characterizations systematically elucidates the role of FDD modification. Morphological analyses (SEM, AFM) reveal enlarged grain domains, enhanced film compactness, and reduced macroscopic roughness, indicative of suppressed grain-boundary defects and improved crystallinity. XRD patterns confirm increased phase purity with diminished residual PbBr2 signatures. Optical measurements, including UV-Vis absorption and Tauc analysis, demonstrate enhanced absorption coefficients alongside reduced Urbach energy, reflecting decreased sub-bandgap states and minimized energetic disorder.
Photophysical investigations further corroborate the suppression of nonradiative pathways. Steady-state and time-resolved PL measurements exhibit intensified emission and prolonged carrier lifetimes. Space-charge-limited current analysis indicates a reduced trap-state density, while electrochemical impedance spectroscopy reveals elevated recombination resistance and decreased transport resistance, evidencing facilitated charge extraction. Transient photocurrent and photovoltage responses further confirm accelerated carrier dynamics and extended recombination lifetimes, underscoring improved interfacial charge-transfer kinetics.
Benefiting from these collective enhancements, the optimized FDD-modified device delivers a champion PCE of 11.25%, with an open-circuit voltage of 1.64 V, a short-circuit current density of 7.98 mA cm-2, and a fill factor of 85.96%, substantially surpassing previously reported benchmarks for FAPbBr3 systems. Device statistics indicate improved reproducibility with reduced performance dispersion. Moreover, unencapsulated devices retain 96.88% of their initial efficiency after 30 days under ambient conditions (~20% RH, 25 °C), highlighting markedly enhanced environmental stability.
In essence, this work establishes a refined molecular-level interfacial engineering paradigm for wide-bandgap FAPbBr3 photovoltaics. By constructing a synergistic dual-site passivation framework that concurrently targets Pb2+-related surface defects and other surface defect sites, the FDD interlayer effectively tailors crystallization behavior, suppresses nonradiative recombination, and promotes efficient charge transport. This strategy not only advances the efficiency ceiling of carbon-based wide-bandgap perovskite solar cells but also provides deeper mechanistic insights into defect governance and interface design in bromide perovskite systems.

Key words： Formamidinium disulfide dihydrochloride; Interfacial engineering; Two-step spin coating; Defect passivation; FAPbBr3 perovskite solar cells

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