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Progress in Chemistry 2019, Vol. 31 Issue (9): 1238-1250 DOI: 10.7536/PC190211 Previous Articles   Next Articles

From Preparation to Lighting and Display Applications of Ⅰ-Ⅲ-Ⅵ Quantum Dots

Yanqiao Xu1, Ting Chen1,2,**(), Lianjun Wang2,3,**(), Weihui Jiang1,2, Wan Jiang2,3, Zhixiang Xie1   

  1. 1. School of Material Science and Engineering, Jingdezhen Ceramic Institute, Jingdezhen 333001, China
    2. National Engineering Research Center for Domestic & Building Ceramics, Jingdezhen 333001, China;
    3. College of Materials Science and Engineering, Donghua University, Shanghai 201620, China
  • Received: Online: Published:
  • Contact: Ting Chen, Lianjun Wang
  • About author:
    ** E-mail: (Ting Chen);
    (Lianjun Wang)
  • Supported by:
    The National Natural Science Foundation of China(No.51402135); The National Natural Science Foundation of China(No.51432004); The National Natural Science Foundation of China(No.51774096); The Fund for Distinguished Young Scholars of Jiangxi Province(No.20171BCB23071); The Natural Science Foundation of Jiangxi Province(No.20181BAB216009); The Natural Science Foundation of Jiangxi Province(No.20171BAB216008); The Science Foundation of Jiangxi Provincial Department of Education(No.GJJ180708); The Science Foundation of Jiangxi Provincial Department of Education(No.GJJ180707)
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Semiconductor quantum dots(QDs) present great potential in applications of light emitting diodes, solar cells and bio-labeling fields owing to their unique optical and electronic properties. Although the traditional Ⅱ-Ⅵ and Ⅲ-Ⅴ type QDs possess appealing emission properties, the intrinsic toxicity of heavy metal elements, such as cadmium and lead, severely sheds doubt on their large-scale commercial applications. As a new kind of fluorescent material that has emerged in recent years, Ⅰ-Ⅲ-Ⅵ multiple QDs are considered as promising alternatives to the traditional binary QDs due to their low toxicity, tunable bandgaps, large Stokes shifts and long photoluminescence lifetime, which have been receiving considerable attention of researchers. In this review, we highlight the current research progress on theⅠ-Ⅲ-Ⅵ QDs. Firstly, the regulation mechanism of the luminescent properties is illuminated on the basis of their structure and composition. Moreover, the emphasis is focused on the current research of the organic and aqueous preparation pathways in recent years. Simultaneously, their primary applications in the lighting and display fields are summarized, and the comparison of the latest research progress of devices betweenⅠ-Ⅲ-Ⅵ QDs and other QDs is made. Finally, we outline the challenges concerning the development of the luminescentⅠ-Ⅲ-Ⅵ QDs and conclude the main future research directions.

Key words: quantum dots, I-III-VI type, preparation approach, optical property, lighting and display
Fig. 1 Unit cell of the(a) chalcopyrite structure, (b) zinc blende structure, and(c) wurtzite structure[46]. Copyright 2013, Royal Society of Chemistry
Fig. 2 Emission mechanism of CuInS2 quantum dots[63]. Copyright 2015, Elsevier
Table 1 Organic preparation methods forⅠ-Ⅲ-Ⅵ type quantum dots
Materials Precursors, ligands, solvents Methods Conditions Emission
peak/nm		 Size/nm QY/% ref
Cu-Fe-S/CdS Cu(Ac)2, FeCl2, S, DDT, OA, ODE Hot injection 180 ℃, Ar 520~1000 3~15 87 15
Cu-In-S/ZnS Cu(Ac)2, In(Ac)3, S, TOP, DDT, OA, SA, ODE Hot injection 180 ℃ 500~950 2~20 30 18
Cu-Zn-In-S CuAc, In(Ac)3, Zn(Ac)2, S, DDT, OA, ODE Hot injection 230 ℃, Ar 620~750 2~7 70 21
Zn-Ag-In-S/Zn-In-S/ZnS AgNO3, In(acac)3, HZAD, S, OLA, OA, OTT, ODE Hot injection 180 ℃, N2 511~590 3.3~3.9 87 26
Cu-In-S/ZnS CuI, In(Ac)3, Zn(Ac)2, S, OTT, OA, ODE Hot injection 230 ℃, N2 577~602 1.9~7.1 89 27
Zn-Cu-In-S CuI, InI3, S, DECZn, TOP, OLA, ODE Heating up 160~280 ℃,
N2		 570~800 3~6 5 13
Cu-In/Ga-S/ZnS CuI, GaI3, In(Ac)3, Zn(Ac)2, S, DDT, OA, OLA, ODE Heating up 240 ℃, N2 495~536 4.8~6.3 85 16
Cu-In-Zn-S CuI, In(Ac)3, Zn(St)2, DDT, TOP, ODE Heating up 230 ℃ 590~640 2.7 80 19
Cu-Zn-In-S/ZnS Cu(Ac)2, In(Ac)3, Zn(Ac)2, S, DDT, OAm, ODE Heating up 220 ℃ 450~810 2.4~3.9 85 22
Cu-In-S/ZnS CuI, In(Ac)3, Zn(St)2, DDT, ODE Heating up 230 ℃, Ar 665~717 2~4 78 23
Zn-Cu-In-S/ZnS CuI, In(Ac)3, Zn(SA)2, DDT, OA, ODE Heating up 240 ℃, Ar 600~815 3.2~6.2 50 28
Zn-Ag-In-S AgNO3, In(Ac)3, Zn(St)2, S, DDT, TOP, OA, ODE Heating up 120~210 ℃,
N2		 520~680 5~7.4 41 29
Cu-In-Zn-S Cu(Ac)2, In(Ac)3, Zn(Ac)2, DDT, OLA, ODE Heating up 230 ℃, Ar 520~700 2.5 76 57
Cu-In-S/ZnS
Cu-In-S/CdS		 CuI, In(Ac)3, Zn(St)2, Cd-OA, S, DDT Heating up 230 ℃, Ar 630~780 2.2~3.3 86 62
Cu-In-S/ZnS CuI, In(Ac)3, Zn(Ac)2, DDT, ODE Solvothermal 180 ℃ 545~614 1.4~3.6 65 55
Cu-In-S/ZnS CuI, In(Ac)3, Zn(Ac)2, S, OA, OAm, DDT, ODE Microwave 190~240 ℃ 610~712 2.7~3.2 56 75
Cu-In-S (PPh3)2CuIn(Set)4, C6H14S, TOPO, DOP Thermal decomposition 200 ℃, Ar 700 2~4 4.4 17
Ag-In-S AgNO3, In(NO3)3, NaS2CN(C2H5)2, OCA, OLA Thermal decomposition 180 ℃ 650~830 3.8~4.3 70 76
Table 2 Aqueous preparation methods forⅠ-Ⅲ-Ⅵ type quantum dots
Materials Precursors, ligands Methods Conditions Emission
peak/nm		 Size/nm QY/% ref
Cu-In-S/ZnS CuCl2·2H2O, InCl3, Zn(Ac)2·2H2O, Na2S·2H2O, SC, GSH Heating up 95 ℃ 543~625 2.1~3.8 38 31
Zn-Ag-In-S AgNO3, Zn(Ac)2, In(Ac)3, Na2S2O3, Thiourea, Na2S·9H2O, GSH Heating up 100 ℃ 525~625 2.0~2.5 30 37
Zn-Ag-In-Se AgNO3, Zn(Ac)2, In(Ac)3, Na2SeSO3, GSH Heating up 100 ℃ 450~760 3.5~4.0 30 38
Ag-In-S/ZnS AgNO3, InCl3, Na2S·9H2O, Zn(Ac)2, MAA Heating up 90~
95 ℃		 580~770 2.0~3.5 47 39
Cu-In-Zn-S CuCl2·2H2O, InCl3·4H2O, Zn(Ac)2·2H2O, Na2S, SC, GSH Heating up 95 ℃ 588~668 3.5~3.9 5.95 40
Ag-In-S-ZnS AgNO3, In(NO3)3, Zn(NO3)2, Na2S, GSH, PAA, MAA Heating up 100 ℃ 525~640 3.0 20 59
Zn-Cu-In-S CuCl2, InCl3·4H2O, Zn(Ac)2, Na2S·xH2O, MPA Heating up 100 ℃ 600~700 4.0~7.0 4.7 61
Ag-In-S/ZnS AgNO3, In(OH)3, TGA, Gelatin, (NH4)2S, ZnCl2 Electric pressure cooker 120 ℃ 535~607 2.4~2.9 39.1 32
Cu-In-Se/ZnS
Ag-In-Se/ZnS		 CuCl2·2H2O, AgNO3, In(OH)3, ZnO, TGA, Se, NaBH4, Gelatin Electric pressure cooker 120 ℃ 582~686 3.6, 3.9 23.3 33
Ag-In-S/ZnS AgNO3, In(OH)3, ZnCl2, (NH4)2S, TGA, Gelatin Electric pressure cooker 120 ℃ 570~615 3.0 57 34
Ag-In-S/ZnS AgNO3, In(OH)3, Zn(NO3)2·6H2O, (NH4)2S, TGA, Gelatin, PVA Electric pressure cooker 120 ℃ 560~575 2.5~3.4 64 35
Ag-In-S AgNO3, InCl3, PEI, Na2S·9H2O Electric pressure cooker 120 ℃ 550~560 3.1 32 36
Cu-In-S/ZnS CuCl2, InCl3, Na2S, SC, TGA Electric pressure cooker 120 ℃ 545~610 3.5~5.1 40 65
Cu-In-S/ZnS CuCl2·2H2O, InCl3, Zn(Ac)2·2H2O, Thiourea, SC, GSH Microwave 95 ℃ 543~700 3.2~4.8 43 58
Ag-In-S/ZnS AgNO3, In(NO3)3·4H2O, Zn(Ac)2·2H2O, Na2S, GSH Microwave 100 ℃ 553~570 2.5 40 66
Zn-Ag-In-S AgAc, In(Ac)3, Zn(Ac)2, Na2S, GSH One-step 95 ℃ 560~660 3.0~4.0 15 77
Cu-Zn-In-S CuCl2·2H2O, InCl3, Zn(Ac)2·2H2O, Na2S, Thiourea, SC, GSH Hydrothermal 150 ℃ 465~700 4.6~5.5 25~35 78
Fig. 3 (a) Absorption spectra, (b) normalized PL spectra, (c) the digital photograph under UV lamp and(d) schematic energy level diagram of CZIS QDs[78]. Copyright 2015, Royal Society of Chemistry
Fig. 4 (a) Schematic for the large-scale preparation process of CISe/ZnS and AISe/ZnS core/shell QDs, (b) the digital photographs of a commercial electric pressure cooker and(c) the crude dispersion of the as-prepared core/shell QDs[33]. Copyright 2015, Royal Society of Chemistry
Table 3 Parameters of pc-LED by usingⅠ-Ⅲ-Ⅵ quantum dots
Materials CRI CCT(K) LE(lm/W) Current(mA) LED Chips(nm) Ref
Cu-In-S/ZnS 73 6140 80.3 20 450 9
Cu-In-S/ZnS+Cu-Ga-S/ZnS 94~97 5654 68.8 20 455 16
Cu-In-S/ZnS 72 4447 63.4 20 455 23
Cu-In-Se/ZnS+YAG:Ce 78 3818 - 20 460 33
Ag-In-S/ZnS 90.2 3698 - 20 460 35
Cu-In-S/ZnS+YAG:Ce+Greenphosphor(G2762) 92 3800~5400 45~60 20 455 84
Cu-In-Zn-S/ZnS 95 4694 69.4 20 460 85
Cu-In-S+AlOH 94.3 5301 23.5 20 405 87
(Mn, Cu):Zn-In-S 95 5092 73.2 20 450 88
Cu-In-S/ZnS+Ba2SiO4:Eu2+ 90 6552 36.7 20 455 89
Fig. 5 (a) EL spectra, (b) operating images, (c) variations of CRI, CCT, luminous efficacy and(d) CIE color coordinates of LEDs fabricated with different weight ratios between CGS and CIS QDs[16]. Copyright 2017, Royal Society of Chemistry
Table 4 Parameters of electroluminescent devices by usingⅠ-Ⅲ-Ⅵ quantum dots
Materials Device structure Luminance(cd/m2) Current efficiency(cd/A) EQE(%) ref
Cu:Zn-In-S ITO/PEDOT:PSS/poly-TPD/QDs/TPBI/LiF/Al 220 2.45 - 22
Cu-In-S/ZnS ITO/PEDOT:PSS/TFB/QDs/ZnO/Al 8464 18.2 7.3 27
Cu-In-S/ZnS ITO/PEDOT:PSS/PVK/QDs/ZnO/Al 1564 2.52 1.1 94
Cu-In-S/ZnS ITO/ZnO/QDs/CBP/TCTA/MoO3/Al 8735 9.43 3.22 95
Cu-In-Ga-S ITO/PEDOT:PSS/PVK/QDs/ZnO/Al 1673 4.15 1.54 99
Cu-In-S/ZnS ITO/PEDOT:PSS/PVK/QDs/ZnO/Ag 2354 0.41 0.63 100
Cu-Ga-S/ZnS ITO/PEDOT:PSS/PVK/QDs/ZnO/Al 1007 3.6 1.9 101
Ag-In-S/ZnS ITO/ZnO/PEI/QDs/CBP/MoOx/Au 232 2.3 1.52 96
Ag-In-Zn-S ITO/ZnO/QDs/HTL/MoO3/Al 2034 2.1 - 102
Zn-Cu-In-S/ZnSe/ZnS ITO/PEDOT:PSS/poly-TPD/QDs/Alq3/Ca/Al 1600 0.62 - 93
Fig. 6 (a) Structure, (b) current efficiency and external quantum efficiency as a function of luminance, (c) corresponding energy level diagram, and(d) EL spectra with increasing driving voltage of EL devices[27]. Copyright 2016, American Chemical Society
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