基于对氯苄胺的2D/3D钙钛矿太阳能电池

doi:10.15541/jim20210199

无机材料学报 ›› 2022, Vol. 37 ›› Issue (1): 72-78.DOI: 10.15541/jim20210199

所属专题：【信息功能】Max层状材料、MXene及其他二维材料；【能源环境】钙钛矿；【能源环境】太阳能电池

基于对氯苄胺的2D/3D钙钛矿太阳能电池

杨新月(), 董庆顺, 赵伟冬, 史彦涛()

大连理工大学化工学院化学系, 精细化工国家重点实验室, 大连 116024

收稿日期:2021-03-25 修回日期:2021-05-27 出版日期:2022-01-20 网络出版日期:2021-06-10
通讯作者: 史彦涛, 教授. E-mail: shiyantao@dlut.edu.cn
作者简介:杨新月(1996-), 女, 硕士研究生. E-mail: yangxinyue@mail.dlut.edu.cn
基金资助:
国家自然科学基金(51773025)

4-Chlorobenzylamine-based 2D/3D Perovskite Solar Cells

YANG Xinyue(), DONG Qingshun, ZHAO Weidong, SHI Yantao()

State Key Laboratory of Fine Chemicals, Department of Chemistry, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China

Received:2021-03-25 Revised:2021-05-27 Published:2022-01-20 Online:2021-06-10
Contact: SHI Yantao, professor. E-mail: shiyantao@dlut.edu.cn
About author:YANG Xinyue(1996-), female, Master candidate. E-mail: yangxinyue@mail.dlut.edu.cn
Supported by:
National Natural Science Foundation of China(51773025)

摘要/Abstract

摘要：

三维(3D)有机-无机金属卤化物钙钛矿薄膜的表面和晶界处存在大量缺陷, 容易导致载流子的非辐射复合并加快3D钙钛矿分解, 进而影响钙钛矿太阳能电池(PSCs)能量转换效率(PCE)及稳定性。本研究通过引入对氯苄胺阳离子, 与3D钙钛矿薄膜及其表面过剩的碘化铅反应后原位形成了二维(2D)钙钛矿, 实现了对3D钙钛矿薄膜表面和晶界处的缺陷钝化并改善了表面疏水性。基于该策略, 成功制备出具有更高PCE和更好稳定性的2D/3D-PSCs。本工作系统研究了钙钛矿薄膜的结构、形貌和器件的光电特性及稳定性。研究结果表明, 2D/3D-PSCs的PCE高达20.88%, 高于3D-PSCs的18.70%。另外, 2D/3D-PSCs连续工作200 h后(1个太阳光, N₂氛围), PCE保持初始值的82%, 展现出优异的稳定性。

关键词: 钙钛矿太阳能电池, 缺陷钝化, 2D钙钛矿, 3D钙钛矿, 稳定性

Abstract:

Defects at the surface and grain boundary of the three-dimensional (3D) organic-inorganic metal halide perovskite film incline to cause non-radiative recombination of charge carriers and accelerate decomposition of 3D perovskite, in turn deteriorating the power conversion efficiency (PCE) and stability of the perovskite solar cells (PSCs). In this study, the organic 4-chlorobenzylamine cation was applied to react with 3D perovskite and the residual PbI₂ to in-situ form a two-dimensional (2D) perovskite top layer, which can passivate the surface and grain boundary defects of the 3D perovskite film, and improve the surface hydrophobicity. Based on this strategy, 2D/3D-PSCs with higher PCE and better stability were successfully obtained. Their structure, morphology photoelectric propery and stability of PSCs were systematically studied. All results show that 2D/3D-PSCs achieve PCEs up to 20.88%, much higher than that of 18.70% for the 3D-PSCs. In addition, 2D/3D-PSCs can maintain 82% of the initial PCE after 200 h continuous operation under 1-sun illumination in N₂ atmosphere, exhibiting excellent stability.

Key words: perovskite solar cells, defect passivation, 2D perovskite, 3D perovskite, stability

中图分类号:

TQ174

杨新月, 董庆顺, 赵伟冬, 史彦涛. 基于对氯苄胺的2D/3D钙钛矿太阳能电池[J]. 无机材料学报, 2022, 37(1): 72-78.

YANG Xinyue, DONG Qingshun, ZHAO Weidong, SHI Yantao. 4-Chlorobenzylamine-based 2D/3D Perovskite Solar Cells[J]. Journal of Inorganic Materials, 2022, 37(1): 72-78.

图/表 13

图1 (a) 3D钙钛矿薄膜和2D/3D钙钛矿薄膜的XRD图谱, (b) 2D钙钛矿薄膜的XRD图谱

Fig. 1 (a) XRD patterns of 3D and 2D/3D perovskite films, and (b) XRD pattern of 2D perovskite film

图2 入射角度为(a, b)0.1°和(c, d)1°时, (a, c)3D钙钛矿薄膜和(b, d) 2D/3D钙钛矿薄膜的GIWAXS图谱

Fig. 2 GIWAXS patterns of (a, c) 3D and (b, d) 2D/3D perovskite films with incident angles of (a, b) 0.1° and (c, d)1°

图3 (a) 3D钙钛矿薄膜和(b) 2D/3D钙钛矿薄膜的俯视SEM照片, (c) 3D-PSCs和(d) 2D/3D-PSCs的横截面SEM照片

Fig. 3 Top-view SEM images of (a) 3D and (b) 2D/3D perovskite films, cross-sectional SEM images of (c) 3D-PSCs and (d) 2D/3D-PSCs

图4 3D钙钛矿薄膜和2D/3D钙钛矿薄膜的(a)紫外-可见吸收光谱、PL光谱和(b) TRPL衰减曲线

Fig. 4 (a) UV-Vis absorption, PL spectra and (b) TRPL decay curves of 3D and 2D/3D perovskite films

表1 3D及2D/3D钙钛矿薄膜TRPL拟合结果

Table 1 TRPL fitting results of 3D and 2D/3D perovskite films

Sample	τ₁/ns	A₁	τ₂/ns	A₂	τ_ave/ns
3D	2.55	0.71	17.26	0.30	13.49
2D/3D	4.75	0.53	24.86	0.43	21.02

图5 (a) 2D/3D-PSCs器件结构示意图, 3D-PSCs和2D/3D-PSCs (b)在反向和正向扫描时的J-V曲线, (c) EQE光谱图及相应积分电流密度, (d)在最大功率点处的稳态PCE曲线

Fig. 5 (a) Schematic diagram of 2D/3D-PSCs structure, (b) J-V curves (reverse and forward scans), (c) EQE spectra with the corresponding integrated current densities, and (d) stabilized PCE curves at the maximum power point for 3D-PSCs and 2D/3D-PSCs

表2 3D-PSCs及2D/3D-PSCs的光电性能参数

Table 2 Detailed photovoltaic parameters of 3D-PSCs and 2D/3D-PSCs

Sample	Scan method	V_OC/V	J_SC/(mA·cm^-2)	FF/%	PCE/%
3D	Reverse	1.11	23.17	72.74	18.70
3D	Forward	1.08	23.18	71.85	18.06
2D/3D	Reverse	1.17	23.45	76.39	20.88
2D/3D	Forward	1.16	23.44	75.07	20.41

图6 (a) 3D-PSCs和2D/3D-PSCs的热稳定性测试(温度85 ℃, 空气相对湿度为40%~70%), (b) 3D-PSCs和2D/3D-PSCs的光稳定性测试(1个太阳光, N2氛围)

Fig. 6 (a) Thermal stability of 3D-PSCs and 2D/3D-PSCs under 85 ℃ in air (relative humidity: 40%-70%), and (b) light stability of 3D-PSCs and 2D/3D-PSCs under continuous 1 sun illumination in N2 All devices are unencapsulated

图S1 (a) 3D钙钛矿薄膜和(b) 2D/3D钙钛矿薄膜的水接触角测试

Fig. S1 Water contact angle measurements of (a) 3D and (b) 2D/3D perovskite films

图S2 钙钛矿薄膜的Tauc图, 光学带隙为1.62 eV

Fig. S2 Tauc plots of the perovskite films, the optical bandgap is 1.62 eV

图S3 不同浓度4-CBAI溶液处理时(0, 0.5, 1.0和1.5 mg·mL-1), PSCs的PCE统计图

Fig. S3 Statistics of the PCE for PSCs, processed by 4-CBAI treatment with various concentrations of 0, 0.5, 1.0, and 1.5 mg·mL-1

图S4 2D/3D柔性PSCs的J-V曲线

Fig. S4 J-V curve of flexible PSCs based on 2D/3D perovskite

图S5 2D/3D柔性PSCs最大功率点处的稳态PCE和光电流密度曲线

Fig. S5 Stabilized PCE and photocurrent density curves at the maximum power point for the flexible PSCs based on 2D/3D perovskite

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基于对氯苄胺的2D/3D钙钛矿太阳能电池

4-Chlorobenzylamine-based 2D/3D Perovskite Solar Cells

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