添加剂氯化甲铵对FAPbBr3钙钛矿太阳能电池的光伏性能影响研究

doi:10.6023/A26010027

化学学报 ›› 2026, Vol. 84 ›› Issue (9): 1497-1506.DOI: 10.6023/A26010027 上一篇下一篇

研究论文

添加剂氯化甲铵对FAPbBr₃钙钛矿太阳能电池的光伏性能影响研究

文洁^a, 陈洁^a, 郭焕焕^b^,^*(), 汪佳艳^a, 郑松志^a, 殷逍遥^a, 朱文昊^a, 吴韫佳^a, 孙伟海^a^,^*()

^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厦门 361021
^b 邢台学院化学工程与生物技术学院河北邢台 054001

投稿日期:2026-01-26 发布日期:2026-08-17
通讯作者: 郭焕焕, 孙伟海
基金资助:
国家自然科学基金(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)

Effect of Additive Methylammonium Chloride on the Photovoltaic Performance of FAPbBr₃ Perovskite Solar Cells

Jie Wen^a, Jie Chen^a, Huanhuan Guo^b^,^*(), Jiayan Wang^a, Songzhi Zheng^a, Xiaoyao Yin^a, Wenhao Zhu^a, Yunjia Wu^a, Weihai Sun^a^,^*()

^a School of Materials Science and Engineering, Huaqiao University, Engineering Research Center of Environment-Friendly Functional Materials, Ministry of Education. Fujian Key Laboratory of Photoelectric Functional Materials, Institute of Materials Physical Chemistry, Xiamen 361021, China
^b School of Chemical Engineering and Biotechnology, Xingtai University, Hebei 054001, China

Received:2026-01-26 Published:2026-08-17
Contact: Huanhuan Guo, Weihai Sun
Supported by:
The National Natural Science Foundation of China(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/Abstract

近年来, 钙钛矿太阳能电池(Perovskite solar cells, PSCs)凭借高效率、低成本、带隙可调等优势, 被视为下一代光伏技术的核心竞争者. 本研究系统探究了添加剂氯化甲铵(MACl)对FAPbBr₃钙钛矿薄膜的结晶动力学调控及对器件光伏性能的影响, 旨在通过优化添加剂策略提升电池效率与稳定性. 将MACl引入FABr前驱体溶液中, 制备了结构为FTO/TiO₂/FAPbBr₃-MACl/C的太阳能电池器件. 通过改变MACl-FABr甲醇溶液中MACl相对于FABr的质量分数来调控FAPbBr₃钙钛矿晶体的生长. 研究表明当MACl掺杂浓度为10%时制备出了最高开路电压(Open Circuit Voltage, V_OC)为1.62 V, 短路电流密度(Short Circuit Current Density, J_SC)为8.21 mA•cm⁻², 填充因子(Fill Factor, FF)为83.73%, 光电转换效率(Photoelectric Conversion Efficiency, PCE)达11.14%的最优器件, 这一结果代表了FAPbBr₃器件领域的最高水平, 优于已报道的所有同类数据.

关键词: FAPbBr₃钙钛矿太阳能电池, MACl添加剂, 全溴基钙钛矿, 两步溶液旋涂, 添加剂工程

In recent years, perovskite solar cells (PSCs) have been regarded as core competitors in the next generation of photovoltaic technology due to their high efficiency, low cost, and tunable bandgap. Among them, FAPbBr₃ perovskite has attracted attention due to its wide bandgap characteristics (≈2.23 eV) and high wet heat stability, but its photovoltaic performance is limited by problems such as poor crystal quality, high defect density, and severe carrier recombination. To enhance the performance of FAPbBr₃ perovskite solar cells, this study successfully fabricated devices with an FTO/TiO₂/FAPbBr₃-MACl/C structure by incorporating methylammonium chloride (MACl) into the precursor solution. The effect of MACl mass fraction in the MACl-FABr methanol solution on the crystallization kinetics and film morphology of FAPbBr₃ was systematically investigated. Results indicate that MACl acts as an effective crystallization modulator, facilitating the formation of larger and more uniform grains and producing a compact, pinhole-free film with complete substrate coverage. This structural optimization significantly improved the crystallinity of the perovskite layer, thereby effectively suppressing defect-assisted charge recombination and laying a critical material foundation for enhancing the device's power conversion efficiency. The devices were fabricated using a thin-film deposition process: a TiO₂ electron transport layer was first deposited onto cleaned FTO substrates via treatment with a TiCl₄ aqueous solution. A two-step spin-coating procedure was then applied to deposit PbBr₂ and FABr solutions sequentially, followed by annealing at 150  ℃ to form the FAPbBr₃ perovskite layer. Finally, a low-temperature carbon paste was screen-printed as the counter electrode and cured. The morphological, structural, and photophysical properties of the films were thoroughly characterized using scanning electron microscopy (SEM), X-ray diffraction (XRD), UV-visible spectroscopy (UV-vis), steady-state and time-resolved photoluminescence spectroscopy, and current density-voltage (J-V) measurements. These analyses confirmed that the fabricated devices exhibit high-quality film formation and promising photovoltaic performance. Research shows that when the MACl doping concen- tration is 10%, an optimal device was fabricated, achieving a record open-circuit voltage (V_OC) of 1.62 V, a short-circuit current density (J_SC) of 8.21 mA•cm⁻², a fill factor (FF) of 83.73%, and a resulting power conversion efficiency (PCE) of 11.14%, which represents the highest level in the field of FAPbBr₃ devices, outperforming all previously reported data of the same category.

Key words: FAPbBr₃ perovskite solar cells, MACl additive, all-bromide perovskite, two-step solution spin coating, additive engineering

引用此文

文洁, 陈洁, 郭焕焕, 汪佳艳, 郑松志, 殷逍遥, 朱文昊, 吴韫佳, 孙伟海. 添加剂氯化甲铵对FAPbBr₃钙钛矿太阳能电池的光伏性能影响研究[J]. 化学学报, 2026, 84(9): 1497-1506.

Jie Wen, Jie Chen, Huanhuan Guo, Jiayan Wang, Songzhi Zheng, Xiaoyao Yin, Wenhao Zhu, Yunjia Wu, Weihai Sun. Effect of Additive Methylammonium Chloride on the Photovoltaic Performance of FAPbBr₃ Perovskite Solar Cells[J]. Acta Chimica Sinica, 2026, 84(9): 1497-1506.

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图/表 9

	Device structure	V_OC/V	J_SC/ (mA•cm⁻²)	FF/%	PCE/%
二氧化锡修饰^[17]	FTO/SnO₂/FAPbBr₃/carbon	1.57	8.35	82.8	10.86
溴化铯掺杂^[18]	ITO/SnO₂/FAPbBr₃/carbon	1.47	8.43	72.3	8.97
尿素掺杂^[19]	FTO/TiO₂/FAPbBr₃/Spiro-OMeTAD/Au	1.57	7.67	70.0	8.49
PEABr修饰^[20]	FTO/TiO₂/FAPbBr₃/Spiro-OMeTAD/Au	1.39	8.80	77.6	9.40
Li修饰^[21]	FTO/TiO₂/FAPbBr₃/Spiro-OMeTAD/Au	1.53	7.30	71.0	8.20
本工作	FTO/TiO₂/FAPbBr₃/carbon	1.62	8.21	83.7	11.14

表1. 已报道的FAPbBr3钙钛矿太阳能电池性能对比

Table 1. Performance comparison of reported FAPbBr3 perovskite solar cells

图1. 旋涂不同浓度MACl溶液的PVK, 薄膜的SEM图(a), (b), (e), (f)及对应的粒径分布图(c), (d), (g), (h); 空白组及掺杂组的表面元素分析图(i, j)

Figure 1. SEM images (a), (b), (e), (f) and corresponding particle size distribution histograms (c), (d), (g), (h) of PVK films spin-coated with MACl solutions at different concentrations; Surface element analysis chart of blank group and experimental group (i, j)

图2. 空白组和MACl修饰的PVK薄膜的2D AFM (a, b)和3D AFM (c, d)图像; 空白组及旋涂不同浓度的MACl溶液的PVK薄膜的XRD图(e)和局部放大图(f); (g) 10% MACl掺杂的Br XPS谱图; (h) 对应的Cl XPS谱图

Figure 2. 2D AFM (a, b) and 3D AFM (c, d) patterns of PVK films with and without MACl modification, (e) XRD patterns and (f) local magnified XRD patterns of films spin-coated with different concentrations of MACl; (g) Br XPS spectrum of the 10% MACl-doped film; (h) corresponding Cl XPS spectrum

图3. 空白组和掺杂不同浓度(0%、5%、10%、15%) MACl修饰的PVK薄膜的(a) UV-vis光谱; (b) Tauc图谱; (c) PL光谱; (d) TRPL光谱

Figure 3. (a) UV-vis spectra; (b) Tauc plots; (c) PL spectra; (d) TRPL spectra of the blank group and PVK films doped with different concentrations (0%, 5%, 10%, 15%) of MACl modification

Sample	τ_ave/ns	A₁/%	τ₁/ns	A₂/%	τ₂/ns
Pristine	24.13	68.48	16.07	31.50	41.67
5% MACl	24.24	56.85	10.29	43.15	42.64
10% MACl 15% MACl	43.41 34.52	45.73 48.63	13.05 8.35	54.27 51.37	68.99 59.30

表2. 引入MACl前后PVK薄膜的TRPL参数

Table 2. TRPL parameters of PVK film with and without MACl introduction

图4. (a)空白组和不同浓度MACl掺杂的PSCs器件J-V特性曲线; 空白组和10% MACl掺杂PSCs器件的(b, c)正反扫J-V特性曲线、(d)稳态输出曲线、(e) EQE和JSC曲线、(f~i) 20个独立器件的JSC、VOC、FF、PCE参数直方分布图

Figure 4. (a) J-V characteristic curves of PSCs devices for the blank group and different concentrations of MACl doping; PSCs devices of the blank group and 10% MACl doping: (b, c) forward and reverse scan J-V characteristic curves, (d) steady-state output curve, (e) EQE and JSC curves, and (f~i) histograms of JSC, VOC, FF, and PCE for 20 independent devices

Sample (mg•mL⁻¹)	V_oc/V	J_sc/(mA•cm⁻²)	FF/%	PCE/%
Pristine	1.53	7.62	75.66	8.81
5% MACl	1.57	7.71	77.86	9.42
10% MACl	1.62	8.21	83.73	11.14
15% MACl	1.58	7.72	78.86	9.62

表3. J-V光伏性能参数

Table 3. J-V photovoltaic performance parameters

图5. 空白组FAPbBr3 PSCs和掺杂组FAPbBr3 PSCs的(a) M-S特性曲线, (b) C-V特性曲线, (c) 暗态EIS Nyquist曲线, (d) 暗态J-V曲线, (e) TPC曲线, (f) TPV曲线, 光强依赖性曲线: (g) JSC; (h) VOC

Figure 5. (a) M-S curves, (b) C-V curves, (c) The dark-state EIS Nyquist spectrum, (d) The dark-state J-V characteristic curves, (e) TPC, (f) TPV and the intensity dependence curves of (g) JSC and (h) VOC for the devices of pristine and doped group FAPbBr3 PSCs

图6. 空白组FAPbBr3 PSCs和掺杂组FAPbBr3 PSCs器件的30 d稳定性测试: (a) PCE、(b) VOC、(c) JSC、(d) FF

Figure 6. 30-day evolution of (a) PCE, (b) VOC, (c) JSC and (d) FF for PSCs with and without MACl modification

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添加剂氯化甲铵对FAPbBr₃钙钛矿太阳能电池的光伏性能影响研究

Effect of Additive Methylammonium Chloride on the Photovoltaic Performance of FAPbBr₃ Perovskite Solar Cells

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