锡铅混合钙钛矿太阳能电池垂直组分梯度的溶剂工程调控

doi:10.15541/jim20220710

无机材料学报 ›› 2023, Vol. 38 ›› Issue (9): 1089-1096.DOI: 10.15541/jim20220710

所属专题：【能源环境】钙钛矿(202310)；【能源环境】太阳能电池(202310)

锡铅混合钙钛矿太阳能电池垂直组分梯度的溶剂工程调控

代晓栋¹^,²(), 张露伟², 钱奕成², 任智鑫², 曹焕奇²(), 印寿根²

1.理学院, 天津理工大学, 天津 300384
2.材料科学与工程学院显示材料与光电器件教育部重点实验室, 天津市光电显示材料与器件重点实验室, 功能材料国家级实验教学示范中心, 天津理工大学, 天津 300384

收稿日期:2022-11-28 修回日期:2023-01-27 出版日期:2023-09-20 网络出版日期:2023-04-15
通讯作者: 曹焕奇, 教授. E-mail: caoh@tjut.edu.cn
作者简介:代晓栋(1996-), 男, 硕士研究生. E-mail: 1021385583@qq.com
基金资助:
国家重点研发计划(2022YFB4200701);国家自然科学基金(61974103);天津市教委基金(2018ZD09)

Controlling Vertical Composition Gradients in Sn-Pb Mixed Perovskite Solar Cells via Solvent Engineering

DAI Xiaodong¹^,²(), ZHANG Luwei², QIAN Yicheng², REN Zhixin², CAO Huanqi²(), YIN Shougen²

1. School of Science, Tianjin University of Technology, Tianjin 300384, China
2. Key Laboratory of Display Materials and Photoelectric Devices (Ministry of Education), Tianjin Key Laboratory for Photoelectric Materials and Devices, National Demonstration Center for Experimental Function Materials Education, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China

Received:2022-11-28 Revised:2023-01-27 Published:2023-09-20 Online:2023-04-15
Contact: CAO Huanqi, professor. E-mail: caoh@tjut.edu.cn
About author:DAI Xiaodong (1996-), male, Master candidate. E-mail: 1021385583@qq.com
Supported by:
National Key R&D Program of China(2022YFB4200701);National Natural Science Foundation of China(61974103);Scientific Developing Foundation of Tianjin Education Commission(2018ZD09)

摘要/Abstract

摘要：

带隙1.1~1.4 eV的锡铅混合卤化物钙钛矿是单结太阳能电池光电转换效率(PCE)接近Shockley-Queisser (S-Q)理论效率极限值的理想材料。钙钛矿薄膜垂直方向上的化学组分梯度会通过影响能带结构影响载流子的传输和分离, 因此对锡铅混合钙钛矿薄膜的结晶过程进行控制十分重要。本研究发现使用不同剂量的反溶剂制备锡铅混合钙钛矿会形成不同的垂直组分梯度, 并且随反溶剂用量增大薄膜表面铅含量增加。调整溶剂组分可以控制锡铅混合钙钛矿的垂直组分梯度, 增大溶剂中V(DMSO):V(DMF)可以形成底部富铅而表面富锡的垂直组分梯度。当铅基前驱液溶剂中V(DMSO):V(DMF)最优化为1 : 2时, 相比于1 : 4的对照组, 器件在标准光照条件下的开路电压从0.725 V提高到0.769 V, 短路电流密度从30.95 mA·cm^-2提高到31.65 mA·cm^-2, PCE从16.22%提升到接近18%。利用SCAPS软件数值模拟进一步证明了垂直组分梯度的必要性, 当钙钛矿薄膜底部富铅、顶部富锡时, 载流子在空穴传输层界面区域的复合有所减少, 因而电池性能得到提升。

关键词: 锡铅混合钙钛矿, 太阳能电池, 垂直组分梯度, 溶剂工程

Abstract:

With a bandgap of 1.1-1.4 eV, Sn/Pb mixed halide perovskites are ideal materials for single-junction solar cells to reach the power conversion efficiencies (PCEs) limit of Shockley-Queisser (S-Q) theory. Their chemical composition gradient in the vertical direction of the perovskite films affect the transport and separation of carriers by changing the energy band structures. Therefore, it is very important to control the crystallization process of tin-lead mixed perovskite thin films. In this work, it was found that different vertical composition gradients were formed when tin-lead mixed perovskites were prepared with different amounts of the anti-solvent. Larger amounts of anti-solvent was contributed to higher lead content on the film surface. The vertical composition gradient of tin-lead mixed perovskite could be regulated by adjusting the solvent composition, among which increasing V(DMSO):V(DMF) in the solvent could form a vertical composition gradient with a lead-rich bottom and a tin-rich surface. When V(DMSO):V(DMF) in lead-based precursor solutions was optimized to 1 : 2, compared with the control group of 1 : 4, open circuit voltage of the device under standard light conditions increased from 0.725 to 0.769 V, short circuit current density from 30.95 to 31.65 mA·cm^-2, and PCE from 16.22% to nearly 18%. Numerical simulations using SCAPS further proved the necessity of forming a vertical composition gradient. When the bottom of the perovskite film is rich in lead and the top is rich in tin, the recombination of carriers in the hole transport layer interface region is reduced, which can improve the device’s performance.

Key words: tin-lead mixed perovskite, solar cell, vertical component gradient, solvent engineering

中图分类号:

TQ174

代晓栋, 张露伟, 钱奕成, 任智鑫, 曹焕奇, 印寿根. 锡铅混合钙钛矿太阳能电池垂直组分梯度的溶剂工程调控[J]. 无机材料学报, 2023, 38(9): 1089-1096.

DAI Xiaodong, ZHANG Luwei, QIAN Yicheng, REN Zhixin, CAO Huanqi, YIN Shougen. Controlling Vertical Composition Gradients in Sn-Pb Mixed Perovskite Solar Cells via Solvent Engineering[J]. Journal of Inorganic Materials, 2023, 38(9): 1089-1096.

图/表 10

图1 不同反溶剂乙酸乙酯用量制备钙钛矿薄膜的晶体结构

Fig. 1 Crystal structures of perovskite films prepared with different amounts of antisolvent (a) XRD patterns of perovskite films prepared with different amounts of antisolvent; (b) Magnified XRD patterns of (100) lattice plane diffraction peaks; (c) Half-peak width of (100) lattice plane diffraction peaks of thin films at different antisolvent dosages; (d-f) Top-down SEM images of films prepared by 100, 300 and 500 μL antisolvents and statistics of grain sizes

图2 (a) PF-DMSO0.25正面和背面的PL谱图; (b) PF-DMSO0.25对应的PSCs的横截面SEM照片及EDS面扫分析区域; (c) PF-DMSO0.25或PF-DMSO0.50的SEM截面照片中不同深度区域的铅锡元素比

Fig. 2 (a) PL spectra from the front and back sides of PF-DMSO0.25; (b) Cross-sectional SEM images of PSCs of PF-DMSO0.25 and EDS scanning areas; (c) Lead/tin elemental ratios in different depth regions of the cross-sectional SEM images of PF-DMSO0.25 or PF-DMSO0.50; Colorful figures are available on website

图3 PF-DMSOx的物相结构和光电性能

Fig. 3 Phase structure and photoelectric properties of perovskites films PF-DMSOx (a) XRD patterns of films and (b) PCE statistics of devices; (c) Time-resolved photoluminescence spectra; (d) Tauc plots of ultraviolet-visible absorption spectra and (e) ultraviolet photoelectron spectra of PF-DMSO0.50 and PF-DMSO0.25; (f) Energy level relationship, (g) J-V curves, (h) external quantum efficiency and integrated current density, (i) Urbach band edge absorption obtained from EQE spectra and fitted electroluminescence spectra of devices fabricated with PF-DMSO0.50 and PF-DMSO0.25; Colorful figures are available on website

表1 钙钛矿太阳能电池各层结构主要模拟参数

Table 1 Main simulation parameters of perovskite solar cell structures

Ingredient	Thickness/μm	E_g/eV	χ/eV	ε_r	N_c/cm^-3	N_v/cm^-3	μ_n/(cm²∙ V^-1∙s^-1)	μ_p/(cm²∙ V^-1∙s^-1)	N_d/cm^-3	N_a/cm^-3	N_t/cm^-3	Ref.
PEDOT: PSS	0.03	2.2	3	3	2.2×10¹⁵	1.8×10¹⁸	0.02	0.0002	-	3.17×10¹⁴	1×10¹⁵	[35,39, 40-42]
Perovskite	0.6	1.25-1.23	4.15-4.2	100	1.0×10¹⁸	1.0×10¹⁸	2	2	-	1.0×10¹⁸	2.5×10¹⁶	[43-45]
PCBM	0.05	2.0	3.9	3.9	2.5×10²¹	2.5×10²⁰	0.2	0.2	2.93×10¹⁷	-	1×10¹⁵	[42, 46]
BCP	0.01	3.5	3.7	10	1.8×10¹⁸	2.2×10¹⁸	0.02	0.002	1×10²¹	1×10¹⁰	1×10	[42, 46]

图4 数值模拟顺梯度(NG)、无梯度(WO)和逆梯度(IG)异质结结构器件性能

Fig. 4 Numerical simulation of devices with NG, WO, IG heterojunctions (a) Schematic diagram of the solar cell structures with different vertical composition gradients; (b) Positions of the conduction band, valence band, electron and hole quasi-Fermi levels, (c) electron and hole carrier concentrations, (d) J-V curves and (e) EQE curves; (f) Hole deep-level defect trapping probabilities of normal or inverted gradient devices; Colorful figures are available on website

图S1 SnI2溶液旋涂制备薄膜的XRD图谱

Fig. S1 XRD pattern of thin films prepared by spin coating SnI2

图S2 (a~d) PF-DMSO0.50薄膜中, 区域1~4的EDS能谱图; (e~h) PF-DMSO0.25薄膜中, 区域1~4的EDS能谱图

Fig. S2 (a-d) EDS spectra of regions 1-4 of PF-DMSO0.50 film and (e-h) EDS spectra of regions 1-4 of PF-DMSO0.25 film

图S3 PF-DMSOx (x=0.20,0.25,0.33,0.50,1.00)对应器件的(a)开路电压, (b)填充因子和(c)短路电流密度统计图

Fig. S3 Statistical charts of (a) open-circuit voltage, (b) fill factor and (c) short-circuit current density for devices of PF-DMSOx (x=0.20,0.25,0.33,0.50,1.00)

图S4 PF-DMSO0.50和PF-DMSO0.25薄膜的紫外-可见吸收光谱

Fig. S4 UV-Vis absorption spectra of PF-DMSO0.50 and PF-DMSO0.25

图S5 实验中用到的ITO导电玻璃的透过率

Fig. S5 Transmittance spectrum of ITO conductive glass used in the experiments

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锡铅混合钙钛矿太阳能电池垂直组分梯度的溶剂工程调控

Controlling Vertical Composition Gradients in Sn-Pb Mixed Perovskite Solar Cells via Solvent Engineering

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