锡基钙钛矿的研究进展及其在发光二极管中的应用

余毅; 安治东; 蔡晓艺; 郭明磊; 敬承斌; 李艳青

doi:10.7498/aps.70.20201284

摘要

卤化铅钙钛矿由于具有高吸收系数、高载流子迁移率、高缺陷容忍度和高光致发光效率等优越的光电子性能, 近年来引起了人们的广泛关注. 然而, 可能阻碍其商业应用的关键是铅元素的存在引起的毒性问题. 为了解决这一毒性问题, 谨慎而有策略地用其他无毒候选元素替代Pb²⁺是一个很有前途的方向. 锡具有和铅相似的结构和性质, 是目前最有希望替代铅的元素, 这也引起了研究者们广泛的兴趣及进一步的研究. 本文综述了近年来锡基钙钛矿的研究进展及其在发光二极管中的应用. 首先, 介绍了一些适合应用于发光二极管的锡基钙钛矿材料的合成方法. 然后, 分析了不同价态下锡基钙钛矿的晶体结构和光电性质. 在此基础上讨论了锡基钙钛矿材料在发光器件中的应用, 并总结了提高锡基钙钛矿性能的一些措施. 最后提出了锡基钙钛矿当前遇到的重大挑战, 并提出了可能的解决方案, 有助于实现高性能锡基卤化物钙钛矿发光二极管. 基于这篇综述, 以期对锡基卤化物材料及其在发光二极管中的应用有深入了解, 进而推动锡基钙钛矿发光二极管的发展.

关键词:

Abstract

Lead halide perovskites have aroused widespread interest in recent years due to their superior optoelectronic properties, such as high absorption coefficient, high charge carrier mobility, high defect tolerance and high photoluminescence (PL) efficiency. However, one critical problem which potentially hampers their commercial applications is the toxicity caused by lead. To address this toxicity problem, a careful and strategic replacement of Pb²⁺ with other nontoxic candidate elements represents a promising direction. Tin (Sn), currently the most promising alternative to lead due to its structure and properties, has received extensiveattention. In this review, some recent developments of Sn-based perovskites and their applications in light-emitting diodes are summarized. Firstly, some synthesis methods of Sn-based perovskite materials are introduced. Then, the crystal structures and photoelectric properties of Sn-perovskites in different valence states are analyzed. Then, the potential application of Sn-based perovskite materials in light-emitting devices is presented and some methods to improve the performance of Sn-based PeLEDs are also summarized. Finally, the significant challenges in these Sn-based PeLEDs are pointed out and their possible solutions are suggested. It is expected that this review can conduce to an in-depth understanding of Sn-based halide materials and their application in PeLEDs.

Keywords:

作者及机构信息

1.
华东师范大学物理与电子科学学院, 教育部纳米光电与先进仪器工程研究中心, 上海　200241

2.
苏州大学功能纳米与软物质研究院, 江苏省碳基功能材料与器件重点实验室, 苏州　215123

通信作者: 敬承斌, cbjing@ee.ecnu.edu.cn ; 李艳青, yqli@phy.ecnu.edu.cn

基金项目: 国家自然科学基金(批准号: 61520106012, 61722404, 51873138)资助的课题

Authors and contacts

1.
Ministry of Education Nanophotonics & Advanced Instrument Engineering Research Center, School of Physics and Electronics Science, East China Normal University, Shanghai 200241, China

2.
Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123, China

Corresponding author: Jing Cheng-Bin, cbjing@ee.ecnu.edu.cn ; Li Yan-Qing, yqli@phy.ecnu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 61520106012, 61722404, 51873138)

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施引文献

图 1 元素周期表中与铅相邻的元素^[30]

Fig. 1. Elements adjacent to lead in the periodic table^[30].

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图 2 (a) 二维锡基钙钛矿薄膜的制备过程示意图^[59]; (b) Cs₂SnCl₆ 纳米晶的形成和Mn²⁺离子掺杂机制示意图^[45]; (c) 控制合成条件制备1D和0D溴化锡钙钛矿示意图^[62]

Fig. 2. (a) Schematic illustration of the fabrication process for 2D tin-based perovskite thin films by solution method^[59]; (b) schematic illustration of the Cs₂SnCl₆ NC formation and Mn²⁺ ion doping mechanisms^[45]; (c) synthetic schemes for the preparations of 1D and 0D Sn bromide perovskites by carefully controlling synthetic conditions^[62].

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图 3 (a) ABX₃钙钛矿晶体的晶胞^[70]; (b) CsSnX₃ (X = Cl, Cl_0.5Br_0.5, Br, Br_0.5I_0.5, I)钙钛矿纳米晶的PXRD谱图^[60]; (c) 各种钙钛矿的容差因子(t); (d) 各种钙钛矿的八面体因子(μ)^[68]

Fig. 3. (a) Unit cell of ABX₃ perovskite crystal^[70]; (b) PXRD spectra of CsSnX₃ (X = Cl, Cl_0.5Br_0.5, Br, Br_0.5I_0.5, I) perovskite nanocrystals^[60]; (c) tolerance factor (t) of various perovskites; (d) octahedral factor (μ) of various perovskites^[68].

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图 4 (a) 概述MA(Pb_1–_xSn_x)I₃中带隙变化起源的示意图, 阴影区域代表价带和导带^[72]; (b) 卤化物钙钛矿太阳能电池的光学吸收原理图^[12]; (c) α-CsSnI₃, α-CsSnBr₃, and α-CsSnCl₃的QSGW带结构和部分态密度^[75]; (d) BZA₂SnI₄电子带结构的DFT计算; (e) BZA₂SnI₄总态密度和部分态密度的DFT计算^[76]

Fig. 4. (a) Schematic summarizing the origin of the band gap bowing in MA(Pb_1–_xSn_x)I₃, shaded regions represent the valence and conduction bands^[72]; (b) schematic optical absorption of halide perovskite solar cell absorber^[12]; (c) QSGW band structures and partial densities of states of α-CsSnI₃, α-CsSnBr₃, and α-CsSnCl₃^[75]; (d) DFT calculations of electronic band structures for BZA₂SnI₄; (e) DFT calculations of total and partial density of states (PDOS) for BZA₂SnI₄^[76].

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图 5 (a) 纯卤素和混合卤素的CsSnX₃薄膜的归一化吸收光谱和稳态荧光光谱^[65]; (b) 不同阳离子(CH₃NH₃⁺和Pb²⁺) ABI₃的光致发光光谱^[78]; (c) (PEA)₂SnX₄的钙钛矿薄膜的归一化吸收(实线)和荧光(虚线)光谱^[41]

Fig. 5. (a) Normalized absorption spectra and steady-state PL spectra of CsSnX₃ films containing pure and mixed halides^[65]; (b) photoluminescence spectra for ABI₃ with different cations (CH₃NH₃⁺ and Pb²⁺)^[78]; (c) normalized absorbance (solid lines) and PL (dashed lines) spectra of (PEA)₂SnX₄ perovskite thin films processed on glass^[41].

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图 6 (a) CsSnI₃电导率随温度变化关系图^[79]; (b) 由HI溶液(黑色)生长的和由EtOH溶液(红色)生长的单晶MASnI₃的电阻率与温度的关系^[80]

Fig. 6. (a) Temperature dependence of the electrical conductivity of CsSnI₃^[79]; (b) temperature dependence of the electrical resistivity of single-crystal MASnI₃ grown from the HI solution(black)and that grown from the EtOH solution (red)^[80].

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图 7 (a) MASnI₃和(b) FASnI₃的电阻率在不同RH时随时间的变化关系^[82]; 由溶液法获得的 (c) MASnI₃和(d) FASnI₃的单晶电阻率在5−330 K范围内随温度变化曲线^[36]

Fig. 7. Resistivity of (a) MASnI₃ and (b) FASnI₃ as a function of the aging time in air at 60% and 10% RH, respectively^[82]; single-crystal temperature-dependent resistivity plots of (c) MASnI₃ and (d) FASnI₃ in the 5−330 K temperature range. The specimens were obtained from the solution method^[36].

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图 8 (a) (RNH₂)₂SnBr₄的光致发光光谱(在316 nm光下激发)^[6]; (b) 由有机配体包围的0D Sn混合卤素钙钛矿(C₄N₂H₁₄Br)₄SnBr_xI_6–_x(x = 3)的单晶结构^[86]; (c) 室温下(C₄N₂H₁₄Br)₄SnBr_xI_6–_x钙钛矿晶体的激发(蓝线)和发射(红线)光谱^[86]; (d) 由积分球收集的(C₄N₂H₁₄Br)₄SnBr_xI_6–_x (x = 3)晶体的参照和发射光谱^[86]

Fig. 8. (a) Photoluminescence spectra of (RNH₂)₂SnBr₄ (excited by 316 nm)^[6]; (b) single-crystal structure of the 0D Sn mixed-halide perovskite (C₄N₂H₁₄Br)₄SnBr_xI_6–_x (x = 3) surrounded by organic ligands^[86]; (c) excitation (blue line) and emission (red line) spectra of bulk Sn mixed-halide perovskite crystals at room temperature^[86]; (d) excitation line of reference and emission spectrum of (C₄N₂H₁₄Br)₄SnBr_xI_6–_x (x = 3) crystals collected by an integrating sphere^[86].

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图 9 (a) Cs₂SnI₆的晶体结构^[22]; (b) A₂SnI₆的粉末X射线衍射图样和Rietveld细化; (c) Cs₂SnI₆, (CH₃NH₃)₂SnI₆和(CH(NH₂)₂)₂SnI₆的分离单元结构^[90]

Fig. 9. (a) Crystal structure of Cs₂SnI₆^[22]; (b) laboratory powder X-ray diffraction patterns and Rietveld refinements showing phase purity of the A₂SnI₆ series; (c) structures of Cs₂SnI₆, (CH₃NH₃)₂SnI₆, and (CH(NH₂)₂)₂SnI₆ showing the isolated octahedral units^[90].

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图 10 (a) 通过GGA功能计算的Cs₂SnI₆化合物的能带结构和(b) PDOS^[81]; 使HSE06+SOC计算的Rb₂SnI₆的(c) P4/mnc和(d) P2₁/n相的能带结构^[91]

Fig. 10. (a) Calculated band structure and (b) PDOS of the Cs₂SnI₆ compound via the GGA functional^[81]; band structures calculated using HSE06+SOC for the (c) P4/mnc and (d) P2₁/n phases of Rb₂SnI₆^[91].

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图 11 (a) A₂SnI₆系列每个成员的电阻率作为温度的函数^[90]; (b) 使用4探针配置收集的Rb₂SnI₆(IV)的温度依赖性电阻率数据^[91]; (c) A₂SnI₆空位有序双钙钛矿的实验和计算得出的Hellwarth(μ_e_H)电子迁移率与钙钛矿容差因子的函数关系图^[91]

Fig. 11. (a) Electrical resistivity as a function of temperature for each member of the A₂SnI₆ series^[90]; (b) temperature-dependent resistivity data of rubidium tin(IV) iodide collected using a 4-probe configuration with Pt wires and Ag paste^[91]; (c) experimentally and computationally derived Hellwarth (μ_eH) electron mobilities of the A₂SnI₆ vacancy-ordered double perovskites plotted as a function of perovskite tolerance factor^[91].

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图 12 (a) 裸露的CsSnI₃薄膜在大气环境条件下的照片; (b) 常温条件下封装器件的照片^[58]

Fig. 12. (a) Photographs of a bare CsSnI₃ film in ambient condition; (b) photographs of encapsulated devices put in ambient condition^[58].

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图 13 (a) (PEA)₂SnX₄钙钛矿的总体晶体示意图^[41]; (b) (PEA)₂SnX₄钙钛矿体系的归一化吸光度(实线)和PL(虚线)光谱^[41]; (c) 基于PEA₂SnI₄和TEA₂SnI₄的PeLED器件的电流密度与电压关系(J-V)曲线和亮度电压(L-V)特性^[59]

Fig. 13. (a) General crystal schematic of a (PEA)₂SnX₄ perovskite^[41]; (b) normalized absorbance (solid lines) and PL (dashed lines) spectra of (PEA)₂SnX₄^[41]; (c) current density versus voltage (J–V) and luminance versus voltage (L–V) characteristics for the PeLED devices based on PEA₂SnI₄ and TEA₂SnI₄^[59].

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图 14 (a) HPA将Sn⁴⁺还原为Sn²⁺的机制; (b) 在不同电压下工作的器件的EL光谱; (c) 没有HPA添加剂的高分辨率Sn 3 d内层电子的XPS能谱; (d) 有HPA添加剂的高分辨率Sn 3 d内层电子的XPS能谱; (e) EQE与电流密度的关系^[95]

Fig. 14. (a) Mechanism of HPA reduction of Sn⁴⁺ to Sn²⁺; (b) EL spectra of the device operating under different voltages; high-resolution Sn 3 d core level XPS spectra (c) without or (d) with HPA additive; (e) EQE versus current density^[95].

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表 1 部分锡基和铅基PeLEDs的总结

Table 1. Summaries of Sn-based PeLEDs and Pb-based PeLEDs.

年份	器件结构	优化方式	电致发光峰/nm	半峰宽/nm	最大亮度/ 辐射率	EQE/%	参考文献
2018	ITO/ZnO/PEI/(C₁₈H₃₅NH₃)₂SnBr₄/TCTA/MnO₃/Al	低维	621	162	350 cd/m²	0.1	[40]
2019	ITO/PVK/(PEA)_3.5Cs₅Sn_4.5I_17.5/TmPyPB/LiF/Al	低维	920	—	40 W/(sr·m²)	3.01	[42]
2020	ITO/PEDOT:PSS/TEA₂SnI₄/TPBi/LiF/Al	低维	638	28	322 cd/m²	0.62	[59]
2016	ITO/PEDOT:PSS/CsSnI₃/PBD/LiF/Al	—	950	—	40 W/(sr·m²)	3.8	[58]
2018	ITO/LiF/CsSnBr₃/LiF/ZnS/Al	封装层	672	—	172 cd/m²	0.34	[65]
2020	ITO/PEDOT:PSS/(PEA)₂SnI₄/TPBi/LiF/Al	还原剂	633	24	70 cd/m²	0.3	[88]
2020	ITO/PEDOT:PSS/(PEA)₂SnI₄/TPBi/LiF/Al	还原剂	632	—	132 cd/m²	0.72	[110]
2020	ITO/PEDOT:PSS/(PEA)₂SnI₄/TPBi/LiF/Al	还原剂	630	—	355 cd/m²	0.52	[39]
2018	ITO/PEDOT:PSS/CsPbBr₃/PMMA/B3 PYMPM/LiF/Al	—	525	20	14000 cd/m²	20.3	[2]
2018	ITO/ZnO-PEIE/FAPbI₃/TFB/MoOx/Au	—	800	—	390 W/(sr·m²)	20.7	[3]
2019	ITO/ZnO-PEIE/FAPbI₃/TFB/MoOx/Au	—	800	—	308 W/(sr·m²)	21.6	[5]
2019	ITO/poly-TPD/FA_0.33Cs_0.67Pb(I_0.7Br_0.3)₃/TPBi/LiF/Al	—	694	37	—	20.9	[37]

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