Enhancing crystallization and photovoltaic performance of CsPbIBr<sub>2</sub> perovskite through p-aminobenzoic acid

MENG Fanning; WANG Fang; CHENG Long; SUN Zhiyan; WANG Guiqiang

doi:10.7498/aps.74.20250184

Abstract
Inorganic CsPbIBr₂ perovskite features high phase stability and light absorption coefficient, making it suitable for the development of perovskite tandem cells or semi-transparent cells. High-quality CsPbIBr₂ perovskite films are of crucial importance for fabricating efficient solar cells. However, compared with CsPbI₂ and CsPbI₂Br, the CsPbIBr₂ precursor has poor crystallinity and low film coverage, which is prone to generating pinholes and defects. Therefore, serious charge recombination often occurs inside the devices. To solve this problem, p-aminobenzoic acid (PABA) is added to the CsPbIBr₂ precursor to regulate its crystallization dynamics in this work. Electrostatic potential distribution of PABA shows that the electron-rich regions (negative charge regions) are mainly located near the C=O. Fourier transform infrared spectrum indicates the existence of coordination interaction between C=O and Pb²⁺ and the formation of hydrogen bonds between —NH₂ and halide anions. Ultraviolet-visible absorption (UV-Vis) spectrum and X-ray diffraction (XRD) spectrum demonstrate that a new intermediate phase, PABA·Pb···Br(I), is formed between PABA molecules and the components of CsPbIBr₂ precursor. The formation of this intermediate phase slows down the crystallization rate of the perovskite, regulates the grain growth, and enables the preparation of dense perovskite films. XRD, UV-Vis, space charge limited current, and linear sweep voltammetry are used to characterize the film quality. After the addition of PABA, the film quality of CsPbIBr₂ perovskite is improved. Thus, the light absorption is enhanced. The defect density is reduced. And the conductivity is increased. The efficiency of the champion cell increases to 10.65% compared with that of the control cell (8.76%). Further, dark current-voltage curves, Mott-Schottky curves, electrochemical impedance spectra, and photoluminescence spectra are utilized to analyze the reasons for the improved photovoltaic performance. After the addition of PABA, the CsPbIBr₂ device exhibits reduced leakage current, enhanced built-in electric field, suppressed charge recombination, and improved charge extraction at the interface. In addition to the enhancement in photovoltaic efficiency, the PABA-regulated perovskite cells also exhibit high stability. After being stored in air for 1500 h, the average efficiency of the unencapsulated cells remains 80% of the initial value.

Keywords:
CsPbIBr₂ /

inorganic perovskite /

crystallization regulation /

perovskite solar cells
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图 1 (a) PABA分子的结构和静电势; (b) CsPbIBr₂, PABA和添加PABA后CsPbIBr₂样品的FTIR谱图; (c) CsPbIBr₂和添加PABA后CsPbIBr₂前驱体的UV-Vis谱图; (d) PbBr₂和添加PABA后PbBr₂的XRD谱图

Figure 1. (a) Molecular structure and electrostatic potential of PABA; (b) FTIR spectra of CsPbIBr₂, PABA and CsPbIBr₂ with PABA; (c) UV-Vis spectra of the precursor of CsPbIBr₂ and CsPbIBr₂ with PABA; (d) XRD patterns of PbBr₂ and PbBr₂ with PABA.

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图 2 (a)—(c) CsPbIBr₂钙钛矿和添加PABA后CsPbIBr₂钙钛矿结晶过程的颜色演变和XRD谱图; (d) PABA调控CsPbIBr₂钙钛矿结晶的示意图

Figure 2. (a)–(c) Color evolution and XRD patterns of the perovskite of CsPbIBr₂ and CsPbIBr₂ with PABA; (d) schematic of the crystallization of CsPbIBr₂ perovskite regulated by PABA.

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图 3 (a) PABA的热失重曲线; (b) 添加PABA后CsPbIBr₂钙钛矿的EDS图像; (c), (d) CsPbIBr₂和添加PABA后CsPbIBr₂钙钛矿薄膜的SEM图像

Figure 3. (a) Thermogravimetric analysis of PABA; (b) EDS mapping of CsPbIBr₂ with PABA; (c), (d) SEM images of CsPbIBr₂ and CsPbIBr₂ with PABA perovskite.

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图 4 CsPbIBr₂和添加PABA后CsPbIBr₂钙钛矿薄膜的性能分析　(a) XRD; (b) UV-Vis;

Figure 4. Properties analysis of the perovskite films of CsPbIBr₂ and CsPbIBr₂ with PABA: (a) XRD; (b) UV-Vis; (c) dark current-voltage curves of the electron-only devices; (d) linear sweep voltammetry curves.

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图 5 CsPbIBr₂和添加PABA的CsPbIBr₂两种钙钛矿所组装电池的光伏性能　(a) J-V特性曲线; (b) 不同波长的单色光照射下两种电池的光子-电子转化效率和积分电流密度曲线; (c) 最大功率点的稳定功率输出曲线; (d) 30块电池的PCE分布

Figure 5. Photovoltaic performance of the devices fabricated by CsPbIBr₂ and CsPbIBr₂ with PABA perovskite: (a) J-V curves; (b) the incident photon to current conversion efficiency and integrated current density curves; (c) stable power output curves at maximum power points; (d) PCE distribution of 30 cells

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图 6 CsPbIBr₂和添加PABA的CsPbIBr₂两种钙钛矿电池的电化学测试和光谱分析　(a) 暗电流-电压曲线; (b) Mott-Schottky曲线; (c) Nyquist图; (d) 玻璃/CsPbIBr₂/碳电极和玻璃/添加PABA的CsPbIBr₂/碳电极两种半电池的PL光谱

Figure 6. Electrochemical tests and spectral analysis of the devices fabricated by CsPbIBr₂ and CsPbIBr₂ with PABA perovskite: (a) Dark current-voltage curves; (b) Mott-Schottky curves; (c) Nyquist plots; (d) PL spectra of half-cells fabricated by glass/CsPbIBr₂/carbon electrode and glass/CsPbIBr₂ with PABA /carbon electrode.

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图 7 (a) 20—25 ℃, 20%—30% RH、空气环境中两种钙钛矿薄膜的颜色随时间变化的图像; (b)相同条件下未封装的电池PCE随时间的变化; (c) 在85 ℃、干燥的N₂手套箱中未封装的电池PCE随时间的变化; (d) 85% RH、空气条件下未封装的电池PCE随时间的变化

Figure 7. (a) Images of the color evolution of different perovskite films at 20–25 ℃, 20%–30% RH, and air atmosphere; (b) curves of the PCE evolution of unencapsulated cells at the same condition; (c) curves of the PCE evolution of unencapsulated cells at 85 ℃ and dry N₂ atmosphere; (d) curves of the PCE evolution of unencapsulated cells at 85% RH and air atmosphere.

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表 1 已报道的碳基CsPbIBr₂ PSCs的光伏参数

Table 1. Photovoltaic parameters of carbon-based CsPbIBr₂ PSCs reported previously.

电池结构	J_sc/(mA·cm^–2)	V_oc/V	FF/%	PCE/%	Ref.
ITO/TiO₂/CsPbIBr₂/Carbon	11.87	1.312	68.4	10.65	本研究
FTO/SnO₂/CsPbIBr₂/Carbon	9.23	1.08	0.60	5.95	[32]
ITO/TiO₂/CsPbIBr₂/CuSCN/Carbon	10.01	1.19	0.60	7.17	[33]
ITO/TiO₂/CsPbIBr₂/Ti₃C₂Cl_x/Carbon	11.56	1.29	69.93	10.43	[34]
FTO/TiO₂/CsPbIBr₂/GQDs/Carbon	11.93	1.25	65.4	9.8	[35]
ITO/TiO₂/CsPbIBr₂/Carbon	11.64	1.31	67	10.23	[36]
ITO/TiO₂/CsPbIBr₂/Carbon	11.69	1.29	66.97	10.10	[37]
FTO/TiO₂/CsPbIBr₂/Carbon	11.25	1.32	71.9	10.68	[38]
FTO/TiO₂/CsPbIBr₂/DES/Carbon	9.2	1.24	61.5	7.04	[39]
FTO/TiO₂/m-TiO₂/CsPbIBr₂/Carbon	11.67	1.24	70	10.13	[40]
FTO/TiO₂/ET/CsPbIBr₂/Carbon	11.63	1.325	72.23	11.13	[41]
FTO/TiO₂/PPC-CsPbIBr₂/Carbon	10.25	1.25	57.5	7.36	[42]
ITO/TiO₂/ODTC-CsPbIBr₂/Carbon	11.48	1.30	68	10.15	[13]
FTO/TiO₂/m-TiO₂/PTU-CsPbIBr₂/Carbon	11.28	1.26	71	10.09	[43]
FTO/Li: TiO₂/CsPbIBr₂/Carbon	10.01	1.26	64	8.09	[44]
FTO/TiO₂/CsPbIBr₂-SAM/Carbon	11.81	1.317	71.1	11.06	[45]
FTO/TiO₂/Cd- CsPbIBr₂/carbon	11.53	1.324	69.63	10.63	[46]
FTO/TiO₂/PMMA/CsPbIBr₂/carbon	11.36	1.307	62	9.21	[47]
FTO/TiO₂/MAAc/CsPbIBr₂/carbon	10.86	1.26	64.56	8.85	[48]
FTO/TiO₂/CsPbIBr₂/P3 HT:PC₆₁BM/Carbon	11.79	1.31	74.47	11.54	[49]
FTO/TiO₂/CsPbIBr₂/Carbon	10.88	1.08	64	7.52	[50]

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Enhancing crystallization and photovoltaic performance of CsPbIBr₂ perovskite through p-aminobenzoic acid

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Enhancing crystallization and photovoltaic performance of CsPbIBr2 perovskite through p-aminobenzoic acid

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Enhancing crystallization and photovoltaic performance of CsPbIBr₂ perovskite through p-aminobenzoic acid