高质量钙钛矿单晶CH3NH3PbI3研究进展

doi:10.15541/jim20180003

摘要/Abstract

摘要：

有机-无机钙钛矿材料因为具有光谱吸收范围宽、缺陷密度低、载流子复合率低等非常优良的光电性能吸引了广泛关注, 掀起了钙钛矿材料研究热潮。近年来杂化钙钛矿型太阳能电池发展迅速, 光电转化效率目前已达到22.1%, 展现出极大的应用潜力。与多晶薄膜相比, 单晶具有极低的缺陷密度和极少的界面缺陷。多个课题组成功培养出大尺寸钙钛矿单晶, 发现钙钛矿单晶材料具有比其他薄膜多晶材料更好的光响应特性, 是设计制备光伏器件的理想材料。在各类钙钛矿材料中, CH₃NH₃PbI₃是研究和应用最广泛的一类钙钛矿材料。本文主要针对近年来CH₃NH₃PbI₃单晶材料的研究制备进行综述, 介绍了CH₃NH₃PbI₃单晶材料的结构及性能, 重点总结了CH₃NH₃PbI₃单晶材料生长制备方法和应用, 并对其发展趋势进行了展望。

关键词: 钙钛矿, 单晶, CH₃NH₃PbI₃, 光电性能, 综述

Abstract:

Organic-inorganic hybrid halide perovskites have attracted a huge amount of research interest and arised new research upsurge due to its broad absorption range, low trap density, low carrier recombination, and other excellent optoelectronic properties. Perovskite solar cells have shown great potential for application with maximum power conversion efficiencies evolving from 3.8% to 22.1% in just a few years. Single crystal has extremely low defect density and minimal interface defect than polycrystalline materials. Several research groups successfully cultivated large-sized perovskite single crystals, finding that perovskite single crystal is an ideal material for design and fabrication of photovoltaic devices for better light-response than polycrystalline and thin-film materials. Among all kinds of perovskite materials, CH₃NH₃PbI₃ is one of the most widely studied and applied perovskite materials. This paper reviews the study of CH₃NH₃PbI₃ single crystal recently, introducing its structure and superior characteristics. Particularly, growth methods and applications of perovskite single crystals are highlighted. Finally, the development trend of perovskite single crystals is prospected.

Key words: hybrid halide perovskite, single crystal, CH₃NH₃PbI₃, optoelectronic property, review

中图分类号:

O782

楚增勇, 李高林, 蒋振华, 王春华. 高质量钙钛矿单晶CH₃NH₃PbI₃研究进展[J]. 无机材料学报, 2018, 33(10): 1035-1045.

CHU Zeng-Yong, LI Gao-Lin, JIANG Zhen-Hua, WANG Chun-Hua. Recent Progress in High-quality Perovskite CH₃NH₃PbI₃ Single Crystal[J]. Journal of Inorganic Materials, 2018, 33(10): 1035-1045.

图/表 9

图1 太阳能电池光电转化效率发展[3]

Fig. 1 The development of solar cells photoelectric conversion efficiency[3]

图2 钙钛矿晶体结构[5]

Fig. 2 Drawing of crystal structure of hybrid halide perovskite[5]

图3 CH3NH3PbI3单晶(a)反射光谱及(b)热重曲线[46]

Fig. 3 (a) Reflection spectrum and (b) TGA curve of CH3NH3PbI3 single crystal[46]

图4 降温法结晶 (a)~(c)底部籽晶法结晶过程及单晶实物照片[38, 42]; (d)~(e)顶部籽晶法结晶过程及单晶实物照片[40]

Fig. 4 Schematic diagram of solution temperature-lowering crystallization(STL) (a)-(c) Crystallization process of BSSG and images of as-prepared CH3NH3PbI3 single crystal[38, 42]; (d)-(e) Crystallization process of TSSG and image of as-prepared CH3NH3PbI3 single crystal[40]

图5 升温法结晶 (a)~(c)升温结晶法示意图及单晶实物照片[41, 43]; (d)升温结晶溶液中CH3NH3PbI3单晶随时间变化的照片[41]

Fig. 5 Schematic diagram of inverse temperature crystallization (ITC) (a)-(c) Crystallization process of ITC and images of as-prepared CH3NH3PbI3 single crystal[41, 43]; (d) CH3NH3PbI3 crystal growth at different time intervals by ITC[41]

图6 (a)~(c)空间限域制备CH3NH3PbI3单晶片示意图及实物照片; (d) CH3NH3PbI3单晶膜批量制备光电探测器[57]

Fig. 6 (a)-(c) Schematic diagram of thinness- and shape- controlled growth and images of as-prepared CH3NH3PbI3 single crystal wafer; (d) Mass photodetectors based on a piece of single CH3NH3PbI3 crystal wafer[57]

图7 溶剂辅助法结晶(a)~(b)二氯甲烷辅助结晶及晶体产物照片[39]; (c)~(d)CH3NH3PbI3在GBL/ACN混合溶剂溶解度曲线及单晶实物照片[44]; (e)~(f) CH3NH3PbI3在GBL/CB混合溶剂溶解度曲线及单晶实物照片[45]

Fig. 7 Schematic diagram of solvent assisted crystallization (SAC) (a)-(b) Crystallization process of DCM assisted and images of as-prepared CH3NH3PbI3 crystals[39]; (c)-(d) Solubility of CH3NH3PbI3 at different temperatures in mixed-solvent of GBL and ACN, and image of as-prepared CH3NH3PbI3 single crystal[44]; (e)-(f) Solubility of CH3NH3PbI3 at different temperatures in mixed-solvent of GBL and CB, and image of as-prepared CH3NH3PbI3 single crystal[45]

表1 目前各种方法制备的CH3NH3PbI3单晶性能比较

Table 1 A summary of properties of CH3NH3PbI3 single crystal by different methods

Growth method	Solvent	T/℃	Size/mm	Carrier mobility/ (cm²•V^-1•s^-1)	Trap density/cm^-3	Bandgap/eV	Crystal system	Ref.
STL	HI	65→40	10×10×8	—	—	1.48	Tetragonal	[38]
	HI	100→57	12×12×7	—	—	1.48	Tetragonal	[42]
	HI	105→40	20×18×6	167±35	(1.8±1.0)×10⁹	—	Tetragonal	[60]
	HI	75	10×3	164±25	3.6×10¹⁰	—	Tetragonal	[40]
ITC	GBL	60→110	5.8	67.2±7.3	(1.4±0.2)×10¹⁰	1.51	Tetragonal	[41]
	GBL	50→100	71×54×39	34	4.8×10¹⁰	1.53	Tetragonal	[43]
	GBL	—	113×58×52	41	2.1×10⁸	—	Tetragonal	[55]
	GBL	60→110	150 μm in thickness	39.6	6.0×10⁸	1.45	Tetragonal	[56]
SAC	GBL/DCM	Room temperature	Millimeters	2.5	(3.3±0.3)×10¹⁰	1.51	Tetragonal	[39]
	GBL/ACN	60→70	17	—	—	—	Tetragonal	[44]
	GBL/CB	30→60	15×15×10	—	—	—	Cubic	[45]

图8 钙钛矿单晶材料的器件应用[40, 42, 48, 56-57, 67, 71-72]

Fig. 8 Optoelectronic device applications of perovskite single crystals[40, 42, 48, 56-57, 67, 71-72]

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高质量钙钛矿单晶CH₃NH₃PbI₃研究进展

Recent Progress in High-quality Perovskite CH₃NH₃PbI₃ Single Crystal

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