CsPbX3纳米晶稳定性的研究进展

doi:10.15541/jim20190572

无机材料学报 ›› 2020, Vol. 35 ›› Issue (10): 1088-1098.DOI: 10.15541/jim20190572 CSTR: 32189.14.10.15541/jim20190572

所属专题：【虚拟专辑】钙钛矿材料(2020~2021)

CsPbX₃纳米晶稳定性的研究进展

杨丹丹(),李晓明(),孟翠芳,陈佳欣,曾海波

南京理工大学材料科学与工程学院, 新型显示材料与器件工信部重点实验室, 南京 210094

收稿日期:2019-11-09 修回日期:2020-02-04 出版日期:2020-10-20 网络出版日期:2020-09-23
作者简介:杨丹丹(1989-), 女, 博士研究生. E-mail:dandan.yang@njust.edu.cn.
基金资助:
中国科协“青年人才托举工程”(2018QNRC001);国家自然科学基金(61874054);国家自然科学基金(51902160);江苏省自然科学基金(BK20180489);中央高校基本科研专项资金(30918011208);国家杰出青年科学基金(61725402)

Research Progress on the Stability of CsPbX₃ Nanocrystals

YANG Dandan(),LI Xiaoming(),MENG Cuifang,CHEN Jiaxin,ZENG Haibo

MIIT Key Laboratory of Advanced Display Materials and Devices, School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China

Received:2019-11-09 Revised:2020-02-04 Published:2020-10-20 Online:2020-09-23
About author:YANG Dandan (1989-), female, PhD candidate. E-mail: dandan.yang@njust.edu.cn
Supported by:
Young Elite Scientists Sponsorship Program by CAST(2018QNRC001);National Natural Science Foundation of China(61874054);National Natural Science Foundation of China(51902160);Natural Science Foundation of Jiangsu Province(BK20180489);Fundamental Research Funds for the Central Universities(30918011208);The National Natural Science Funds for Distinguished Young Scholars(61725402)

摘要/Abstract

摘要：

全无机钙钛矿纳米晶具有窄发射、高量子效率及较高的载流子迁移率等优点, 在高清柔性显示器和太阳能电池等领域具有广泛的应用前景。然而, 钙钛矿纳米晶的表面配体处于高度动态结合的状态, 容易在分离和提纯等过程中造成大量配体缺失, 从而导致量子效率和稳定性下降。此外, 钙钛矿材料本身的离子晶体特性使其对极性溶剂非常敏感, 这些问题严重制约了钙钛矿纳米晶在光电器件中的实际应用。本文从钙钛矿纳米晶表面态出发, 结合国内外的研究工作, 分析了路易斯酸、路易斯碱及表面包覆策略对钙钛矿纳米晶光学性质和稳定性的影响, 并对进一步优化提升钙钛矿纳米晶的稳定性进行了展望。

关键词: 全无机钙钛矿纳米晶, 表面态, 表面钝化, 量子效率, 稳定性

Abstract:

All inorganic perovskite nanocrystals with narrow-emission, high quantum efficiency and high carrier mobility have been widely applied in the fields of light emitting diodes and solar cells. However, present surface ligands of the perovskite nanocrystals are in a dynamic bonding state, which easily fall off during separation and purification processes, resulting in the deterioration of quantum efficiency and stability. Besides, the ionic characteristic of halide perovskites makes it extremely sensitive to polar solvents. These disadvantages severely restrict the practical application of perovskite nanocrystals in optoelectronic devices. In this review, based on the surface state of perovskite nanocrystals, the effects of passivation strategies with Lewis acid, Lewis base and surface coating on optical properties, and stability of CsPbX₃ perovskite nanocrystals are analyzed in detail combined with the domestic and abroad research work. Further optimization and improvement of the stability of CsPbX₃ are prospected.

Key words: all inorganic perovskite nanocrystals, surface state, surface passivation, quantum yield, stability

中图分类号:

TQ174

杨丹丹, 李晓明, 孟翠芳, 陈佳欣, 曾海波. CsPbX₃纳米晶稳定性的研究进展[J]. 无机材料学报, 2020, 35(10): 1088-1098.

YANG Dandan, LI Xiaoming, MENG Cuifang, CHEN Jiaxin, ZENG Haibo. Research Progress on the Stability of CsPbX₃ Nanocrystals[J]. Journal of Inorganic Materials, 2020, 35(10): 1088-1098.

图/表 9

图1 不同配体钝化CsPbX3纳米晶策略的示意图

Fig. 1 Schematic diagram of passivation strategies for different ligands on the surface of CsPbX3 nanocrystals

图2 (a) CsPbX3晶体结构不稳定性机理的示意图; (b) CsPbX3纳米晶的团聚现象; (c) CsPbX3纳米晶的分解产物; CsPbX3纳米晶的(d)相转变(非钙钛矿相)和(e)相转变(钙钛矿相)示意图

Fig. 2 (a) Schematic diagram of instability mechanism of CsPbX3 nanocrystals, (b) agglomeration and (c) decomposing product of CsPbX3 nanocrystals, and schematic diagram of (d) phase transition (non-perovskite phase) and (e) phase transition (perovskite phase)

图3 (a)硬路易斯酸配体表面钝化策略(左)、高和低缺陷密度纳米晶的发光照片(激发波长365 nm, 中)和对应的荧光寿命曲线(右)[25]; (b)DETAI3表面钝化策略的原理图(左)、CsPbI3?xDETAI3薄膜和放置60 d后的紫外-可见吸收光谱图(中)、以及相应的XRD图谱(右)[29]

Fig. 3 (a) Passivation strategy based on hard Lewis acid ligands (left), images under 365 nm UV light (middle), and photoluminescence decay curves (right) of nanocrystals with high and low defect densities[25]; (b) Schematic diagram of DETAI3 surface passivation strategy (left), absorption curves (middle) and long-term phase stability (right) of CsPbI3?xDETAI3 thin films[29]

表1 路易斯酸型配体表面钝化策略

Table 1 Surface passivation strategies of Lewis acid ligands

Ligands	Treating agent	QY/%	Stability	Ref.
OA/OAm	DDDMAB	~100	21 d	[9]
OA/OAm	TOAB	95	-	[25]
OA/OAm	DDAB	96	-	[26,30]
OA/OAm	NH₄BF₄	(95±2)	-	[27]
OA/OAm	NH₄SCN	(99±2)	-	[28]
OA/OAm	Trimethylsilyl iodine	85	105 d	[31]
OA/OAm	Oxalic acid	89	-	[32]

图4 (a)路易斯碱表面钝化CsPbX3纳米晶的策略示意图; (b)理论计算单羧酸和双羧酸吸附在CsPbI3纳米晶表面的束缚能[34]; (c)OPA和OAm-CsPbX3纳米晶表面钝化策略的示意图和多次纯化后的发光照片[35]; (d)两性离子(磺酸甜菜碱, 磷酸胆碱和γ-氨基酸)表面钝化策略[36]

Fig. 4 (a) Schematic diagram of Lewis base surface passivation strategy for CsPbX3 nanocrystals; (b) Theoretical calculation of the binding energy of mono- and dicarboxylic acids on the surface of CsPbI3 nanocrystals[34]; (c) Schematic diagram of OPA and OAm-CsPbX3 surface passivation strategies and photos after multiple purifications[35]; (d) Surface passivation strategy with zwitterionic ligands (sulfobetaines, phosphocholines and γ-amino acids)[36]

图5 (a)不同配体(OAm, OA和DBSA)在CsPbBr3纳米晶表面的钝化策略和(b)对应的激子复合过程[37]; (c) OAm-CsPbBr3纳米晶表面富含PbBrx(左)和OAm/OA-CsPbBr3纳米晶表面富溴(右)的示意图[11]; (d) OAm/OA-CsPbBr3纳米晶(上)和OAm-CsPbBr3 纳米晶(下)在水溶液中保持稳定的发光照片[11]

Fig. 5 (a) Passivation strategies with different ligands (OAm, OA and DBSA) on the surface of CsPbBr3 nanocrystals and (b) the corresponding exciton recombination processes[37]; (c) Schematic diagram of PbBrx-rich surface of OAm-CsPbBr3 nanocrystals (left) and Br-rich surface of OAm/OA-CsPbBr3 nanocrystals (right)[11]; (d) Photographs showing the resistance of different samples against water treatment of OAm/OA-CsPbBr3 nanocrystals (above) and OAm-CsPbBr3 nanocrystals (below)[11]

表2 路易斯碱表面钝化策略

Table 2 Surface passivation strategies of Lewis base ligands

Ligands	QY/%	Stability	Ref.
OAm	~100 %	-	[11]
OA	70	-	[33]
IDA/OAm	95	40 d	[34]
OPA/TOPO	>90	-	[35]
Zwitterion	>90	28 d	[36]
DBSA	95	5 m	[37]
TMPPA/OAm	90	28 d	[38]
OA/TOPO	90	-	[39]
TDPA/OAm	68	-	[40]
DA	94.3	70 d	[41]

表3 不同钝化策略的特点及其优缺点

Table 3 Characteristics, advantages and disadvantages of different passivation strategies

Strategies		Characteristics	Advantages	Disadvantages	Ref.
Lewis acid ligands	Quaternary ammonium salt	Large steric hindrance	High QY^*	Instable	[9,25-26,30]
Lewis base ligands	Carboxylic acids	Hard base, weak acid	Simple synthesis	Instable, low QY	[32-33]
	Phosphoric acid	Soft alkali, moderately strong acid	High QY, stable	TOPO assisted dissolution	[35]
	Zwitterionic ligands	Surfactant	High QY, stable	Complex process	[36]
	Sulfonic acid	Soft alkali, strong acid	High QY, stable	High temperature	[37]
	Neutral ligands	Lone pair electrons	High QY, stable	Room temperature	[11]

图6 (a) CPB-DBAE@SiO2纳米复合材料的制备过程示意图[51]; (b) CsPbBr3@SiO2纳米晶的普通透射电镜照片(TEM)和高分辨透射电镜照片(HRTEM)以及水稳定性的实物照片[60]; (c) CsPbBr3/CdS纳米晶的示意图(左)、HRTEM照片(中)以及连续脉冲激光照射CsPbBr3/CdS纳米晶的稳定性曲线(右)[67]

Fig. 6 (a) Schematic diagram of CPB-DBAE@SiO2 preparation process[51]; (b) Transmission electron microscopy (TEM) and high resolution transmission electron microscopy (HRTEM) images of CsPbBr3@SiO2 nanocrystals and photographs of water stability[60]; (c) Schematic representation (left), HRTEM image (middle), and plot of emission intensity under continuous pulsed laser irradiation (right) of CsPbBr3/CdS nanocrystals[67]

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CsPbX₃纳米晶稳定性的研究进展

Research Progress on the Stability of CsPbX₃ Nanocrystals

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