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发光铅卤钙钛矿纳米晶稳定性的研究进展

樊钦华 祖延清 李璐 代锦飞 吴朝新

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发光铅卤钙钛矿纳米晶稳定性的研究进展

樊钦华, 祖延清, 李璐, 代锦飞, 吴朝新

Research progress of stability of luminous lead halide perovskite nanocrystals

Fan Qin-Hua, Zu Yan-Qing, Li Lu, Dai Jin-Fei, Wu Zhao-Xin
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  • 相比传统的II-VI或III-V族半导体纳米晶(NCs), 铅卤钙钛矿NCs具有窄发射线宽、高光致发光量子产率、可调光谱和易制备等优异特性, 因此被当作是一种更理想的发光材料. 然而, 当钙钛矿NCs在遇到光、热和极性溶剂等条件时, 将会发生快速且不可逆的降解, 从而表现出差的稳定性. 因此, 提高钙钛矿NCs的稳定性是目前该研究方向亟待解决的关键问题. 本文详细总结了近年来关于提高钙钛矿NCs稳定性的常见方法, 并展望了未来的研究方向.
    The lead halide perovskite nanocrystals (NCs) have become more ideal luminescent materials due to the excellent properties such as narrow emission linewidth, photoluminescence quantum yield (PLQY), adjustable spectrum and facile preparation in comparison with traditional II-VI or III-V group semiconductor NCs. Until now, the external quantum efficiency (EQE) of light-emitting diode (LED) devices using perovskite NCs as emitting layers, has reached > 20%. This optical performance is close to that of the commercially available organic LED, which shows their great potential applications in solid state lighting and panel displaying. However, when perovskite NCs suffer light, heat and polar solvent, they exhibit the poor stability owing to the intrinsic ion properties of perovskite, and highly dynamic interface between NCs and ligands as well as the abundant defects on the surface of NCs. Therefore, how to elevate their stability is a key and urgent problem. In this review, three methods to improve the stability of NCs are summarized: 1) In situ surface passivation with tight-binding or protonation-free sole ligands such as oleic acid (OA), oleamine (OAM), dodecyl benzene sulfonic acid, octylphosphonic acid, sulfobetaines, lecithin and two ligands such as 2-hexyldecanoic acid/OAM, bis-(2,2,4-trimethylpentyl)phosphinic acid/OAM as well as three ligands such as OA/OAM/Al(NO3)3·9H2O, OA/OAM/tris(diethylamino)phosphine); the postsynthetic ligand exchange or passivation with 1-tetradecyl-3-methylimidazolium bromide, 2-aminoethanethiol, silver-trioctylphosphine complex and n-dodecylammonium thiocyanate; 2) the doping of Cs+ by FA+, Na+ and the doping of Pb2+ by Zn2+, Mn2+, Cd2+, Sr2+, Sb3+ in perovskite NCs; 3) the surface coating with inorganic oxides (SiO2, ZrO2, Al2O3, NiOx), inorganic salts (NaNO3, NH4Br, PbSO4, NaBr, RbBr, PbBr(OH)), porous materials (mesoporous silica, zeolite-Y, lead-based metal-organic frameworks), polymer materials (polystyrene, poly(styrene-ethylene-butylene-styrene, poly(laurylmethacrylate), poly(maleic anhydride-alt-1-octadecene), polyimide, poly(n-butyl methacrylate-co-2-(methacryloyloxy)ethyl-sulfobetaine)). Besides, we make some suggestions to further improve the stability of NCs as follows: 1) Developing the surface ligands with good dispersity and multi-coordination groups; 2) theoretically studying the influence of ion doping on the structure and stability; 3) realizing the stable and conductive metal oxides shell for uniform and compact encapsulation of NCs core. In a word, these conventional methods can enhance the stability of NCs to a certain extent, which fail to meet the requirements for practical application, so more efforts will be needed in the future.
      通信作者: 吴朝新, zhaoxinwu@mail.xjtu.edu.cn
    • 基金项目: 国家级-国家重点研发计划(批准号: 2016YFA0200503) 资助的课题(2016YFB0400702)
      Corresponding author: Wu Zhao-Xin, zhaoxinwu@mail.xjtu.edu.cn
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  • 图 1  胶体铅卤钙钛矿NCs (a) APbX3钙钛矿结构, 具有三维共角八面体, 左侧为立方结构(MAPbX3, FAPbX3; 显示了两个晶胞), 右侧为正交结构(CsPbX3); (b)单个立方形CsPbX3 NCs大角度环形暗场扫描透射电子显微照片, 边缘长度为15 nm; (c)高发光胶体NCs的照片, 从左至右, CsPbBr3的发射峰为520 nm, CsPb(Cl/Br)3的发射峰为450 nm, FAPb(Br/I)3的发射峰为640 nm[15]

    Fig. 1.  Colloidal lead halide perovskite NCs: (a) The APbX3 perovskite structure with 3D-corner-sharing octahedra. (Cubic (MAPbX3, FAPbX3; two unit cells shown) on the left and orthorhombic (CsPbX3) on the right); (b) high-angle annular dark-field scanning transmission electron micrograph (HAADF-STEM) of a single, cube-shaped CsPbBr3 NCs, with 15 nm edge length; (c) photograph of highly luminescent colloidal NCs, from left to right, CsPbBr3 with emission peak at 520 nm, CsPb(Cl/Br)3 emitting at 450 nm and FAPb(Br/I)3 emitting at 640 nm)[15].

    图 2  磺酸基团的理论钝化效应 (a) CsPbBr3存在VBr 的价带最大值和导带最小值的电子DOS曲线; (b)CsPbBr3存在VBr 的电子离域结果; (c)磺酸基团钝化CsPbBr3VBr后的价带最大值和导带最小值的电子DOS曲线价带最大值和导带最小值的电子DOS曲线; (d) 磺酸基团钝化CsPbBr3VBr后的电子离域结果[34]

    Fig. 2.  Theoretical sulfonate passivation effect: (a) Electronic DOS curves of valence band maximum (VBM) and conduction band minimum (CBM) of CsPbBr3 with VBr; (b) electron localization function results of CsPbBr3 with VBr; (c) electronic DOS curves of valence band maximum (VBM) and conduction band minimum (CBM) of CsPbBr3 with VBr passivated by the sulfonate group; (d) electron localization function results of CsPbBr3 with VBr passivated by the sulfonate group[34].

    图 3  CsPbCl3 NCs中Pb2+被Cd2+取代的示意图[50]

    Fig. 3.  Representative scheme for exchange of Pb2+ by Cd2+ in CsPbCl3 NCs[50].

    图 4  CsPbBr3 NCs被嵌于SiO2的示意图[56]

    Fig. 4.  The schematic diagram of synthesis CsPbBr3 NCs into SiO2[56].

    图 5  水辅助使CsPbBr3/Cs4PbBr6复合NCs向CsPbBr3/CsPb2Br5复合NCs转化过程的示意图[62]

    Fig. 5.  Schematic illustration of the water-assisted transformation process from CsPbBr3/Cs4PbBr6 composite NCs to CsPbBr3/CsPb2Br5 composite NCs[62].

    图 6  MAPbBr3形貌变化的示意图[67]

    Fig. 6.  Schematic illustration of the morphology evolution of MAPbBr3[67].

    图 7  厚PMAO聚合物层包覆钙钛矿NCs的后合成处理示意图[69]

    Fig. 7.  Schematic illustration of postsynthetic treatment for obtaining perovskite NCs with a thick PMAO polymer coating layer[69].

    图 8  CsPbX3/介孔二氧化硅复合物的制备过程示意图[73]

    Fig. 8.  The synthesis process of CsPbX3/mesoporous silica nanocomposite[73].

    图 9  分别以星形P4 VP-b-PtBA-b-PS和P4 VP-b-PtBA-b-PEO为纳米反应器逐步合成PS包覆MAPbBr3/SiO2核/壳NCs和PEO包覆MAPbBr3/SiO2核/壳NCs的路线. CD表示环糊精; BMP表示2-溴–2-甲基丙酸盐; TOABr表示四辛基溴化铵[77]

    Fig. 9.  Stepwise representation of the synthetic route to PS-capped MAPbBr3/SiO2 core/shell NCs and PEO-capped MAPbBr3/SiO2 core/shell NCs by exploiting star-like P4 VP-b-PtBA-b-PS and P4 VP-b-PtBA-b-PEO as nanoreactors, respectively. CD, cyclodextrin; BMP, 2-bromo-2-methylpropionate; and TOABr, tetraoctylammonium bromide[77].

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    Ni Z Y, Bao C X, Liu Y, Jiang Q, Wu W Q, Chen S S, Dai X Z, Chen B, Hartweg B, Yu Z S, Holman Z, Huang J S 2020 Science 367 1352Google Scholar

    [2]

    Quan L, Rand B, Friend R, Mhaisalkar S, Lee T, Sargent E 2019 Chem. Rev. 119 7444Google Scholar

    [3]

    Levchuk I, Osvet A, Tang X, Brandl M, Perea J, Hoegl F, Matt G, Hock R, Batentschuk M, Brabec C 2017 Nano Lett. 17 2765Google Scholar

    [4]

    Lee T 2019 Adv. Mater. 31 1905077Google Scholar

    [5]

    Smock S, Williams T, Brutchey R 2018 Angew. Chem. Int. Ed. 57 11711Google Scholar

    [6]

    Møller C 1958 Nature 182 1436

    [7]

    Weber D 1978 Zeitschrift fur Naturforschung B 33 862Google Scholar

    [8]

    瞿子涵, 储泽马, 张兴旺, 游经碧 2019 物理学报 68 158504Google Scholar

    Qu Z H, Chu Z M, Zhang X W, You J B 2019 Acta Phys. Sin. 68 158504Google Scholar

    [9]

    Pu C, Dai X, Shu Y, Zhu M, Deng Y, Jin Y, Peng X 2020 Nat. Commun. 11 937Google Scholar

    [10]

    Reiss P, Carriere M, Lincheneau C, Vaure L, Tamang S 2016 Chem. Rev. 116 10731Google Scholar

    [11]

    Kumar S, Jagielski J, Kallikounis N, Kim Y, Wolf C, Jenny F, Tian T, Hofer C, Chiu Y, Stark W, Lee T, Shih C 2017 Nano Lett. 17 5277Google Scholar

    [12]

    He J, Chen H, Chen H, Wang Y, Wu S, Dong Y 2017 Opt. Express 25 12915Google Scholar

    [13]

    Won Y, Cho O, Kim T, Chung D, Kim T, Chung H, Jang H, Lee J, Kim D, Jang E 2019 Science 575 634

    [14]

    Yu D, Cao F, Gao Y, Xiong Y, Zeng H 2018 Adv. Funct. Mater. 28 1800248Google Scholar

    [15]

    Akkerman Q, Raino G, Kovalenko M, Manna L 2018 Nat. Mater. 17 394Google Scholar

    [16]

    Zu Y, Dai J, Li L, Yuan F, Chen X, Feng Z, Li K, Song X, Yun F, Yu Y, Jiao B, Dong H, Hou X, Ju M, Wu Z 2019 J. Mater. Chem. A 7 26116Google Scholar

    [17]

    Lv W, Li L, Xu M, Hong J, Tang X, Xu L, Wu Y, Zhu R, Chen R, Huang W 2019 Adv. Mater. 31 1900682Google Scholar

    [18]

    段聪聪, 程露, 殷垚, 朱琳 2019 物理学报 68 158503Google Scholar

    Duan C C, Cheng L, Yin Y, Zhu L 2019 Acta Phys. Sin. 68 158503Google Scholar

    [19]

    韦祎, 陈叶青, 程子泳, 林君 2018 中国科学: 化学 48 771Google Scholar

    Wei Y, Chen Y Q, Cheng Z R, Lin J 2018 Sci. Sin. Chim. 48 771Google Scholar

    [20]

    Niu G, Guo X, Wang L 2015 J. Mater. Chem. A 3 8970Google Scholar

    [21]

    谢启飞, 王新中, 李玥, 马艳红 2018 深圳信息职业技术学院学报 16 56Google Scholar

    Xie Q F, Wang X Z, Li Y, Ma Y H 2018 Journal of Shenzhen Institute of information tecnology 16 56Google Scholar

    [22]

    王恩胜, 余丽萍, 廉世勋, 周文理 2019 材料导报 33 777Google Scholar

    Wang E S, Yu L P, Lian S X, Zhou W L 2019 Materials Reports 33 777Google Scholar

    [23]

    徐妍, 曹蒙蒙, 夏超, 李会利 2019 聊城大学学报 32 69

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出版历程
  • 收稿日期:  2019-11-20
  • 修回日期:  2020-03-09
  • 刊出日期:  2020-06-05

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