Transition metal oxides as hole-transporting materials in organic semiconductor and hybrid perovskite based solar cells

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SCIENCE CHINA Chemistry
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SCIENCE CHINA Chemistry, Volume 60, Issue 4: 472-489(2017) https://doi.org/10.1007/s11426-016-9023-5

Transition metal oxides as hole-transporting materials in organic semiconductor and hybrid perovskite based solar cells

Pingli Qin1,2,4, Qin He3, Dan Ouyang5, Guojia Fang4, Wallace C.H. Choy5, Gang Li1,*
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  • ReceivedDec 16, 2016
  • AcceptedFeb 20, 2017
  • PublishedMar 14, 2017
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Abstract

Organic polymer solar cells (OSCs) and organic-inorganic hybrid perovskite solar cells (PSCs) have achieved notable progress over the past several years. A central topic in these fields is exploring electronically efficient, stable and effective hole-transporting layer (HTL) materials. The goal is to enhance hole-collection ability, reduce charge recombination, increase built-in voltage, and hence improve the performance as well as the device stability. Transition metal oxides (TMOs) semiconductors such as NiOx, CuOx, CrOx, MoOx, WO3, and V2O5, have been widely used as HTLs in OSCs. These TMOs are naturally adopted into PSC as HTLs and shows their importance. There are similarities, and also differences in applying TMOs in these two types of main solution processed solar cells. This concise review is on the recent developments of transition metal oxide HTL in OSCs and PSCs. The paper starts from the discussion of the cation valence and electronic structure of the transition metal oxide materials, followed by analyzing the structure-property relationships of these HTLs, which we attempt to give a systematic introduction about the influences of their cation valence, electronic structure, work function and film property on device performance.


Funded by

Natural Science Foundation of Hubei Province(2014CFB275)

Project of Strategic Importance provided by The Hong Kong Polytechnic University(1-ZE29)

National Natural Science Foundation of China(61376013)

Special(2016T90724)

National High Technology Research and Development Program(2015AA050601)


Acknowledgment

This work was supported by the Project of Strategic Importance provided by The Hong Kong Polytechnic University (1-ZE29), the Natural Science Foundation of Hubei Province (2014CFB275), the Special (2016T90724, 2014T70735) and General (2015M572187, 2013M531737) Postdoctoral Science Foundation of China, the National High Technology Research and Development Program (2015AA050601), and the National Natural Science Foundation of China (61376013, 91433203, 11674252).


Interest statement

The authors declare that they have no conflict of interest.


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    Figure 1

    (a) High resolution Ni 2P3/2 XPS acquisition for NiO. The spectrum shows three contributions: one from Ni2+ in the octahedral NiO configuration at low binding energy, one from hydroxylated or defective NiO at an intermediate binding energy, and one from a shake-up process in the NiO lattice at the highest binding energy. (b) High resolution O 1s XPS acquisition for NiO. The spectrum shows two contributions: one from O2? in the octahedral NiO configuration at low binding energy and one from hydroxylated or defective NiO at a higher binding energy [59].

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    Figure 2

    UPS and IPES measurements of the density of states near the valence band edge and conduction band and resulting band energies. (a) UPS spectra (He I) of the photoemission cut-off showing an increase in WF after O2-plasma treatment of the NiOx; (b) combined UPS and IPES spectra of the NiOx near the valence and conduction band edge; (c) energy level diagrams of NiOx before and after O2-plasma treatment [70].

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    Figure 3

    The Cu 2P3/2 core level peaks of (a) the as-deposited and (b) UVO-treated CuOx films (color online).

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    Figure 4

    UPS spectra of the as-deposited and UVO-treated CuOx films. The full UPS spectra using He I radiation (a), and the valence-band region (b) are included (color online).

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    Figure 5

    XPS spectra of (a) Cr 2p, (b) Mo 3d, (c) V 2p, and (d) W 4f core level peaks observed for molybdenum oxide thin ?lms [37,80–82] (color online).

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    Figure 6

    (a) UPS spectra of CrOx and Cu:CrOx films with UVO treatment. The full UPS spectra using He I radiation (left) and the valence-band region (right) are included. (b) UPS and IPES spectra of vacuum grown MoO3, V2O5 and WO3. The left panel shows the photoemission onset, the middle panel shows the density of filled states near the valence band (VB) edge, and the right panel shows the density of empty states near the conduction band (CB) edge. The reference is the Fermi level, measured separately on a metallic electrode. The tick marks denote the onset position, the top of the VB, and the bottom of the conduction band [37,58,91,93,110] (color online).

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    Figure 7

    CB minimum and VB maximum with respect to the vacuum level (EVL) for MoO3, V2O5 and WO3, deduced from the UPS and IPES measurements depicted in Figure 6. The ionization energy, work function and electron affinity are indicated in each case (color online).

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    Figure 8

    Schematic illustration of energy levels of each layer and charge transfer in (a) OSC and (b) inverted planar PSC (color online).

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    Figure 9

    Scanning electron microscope (SEM) images of (a) NiOx thin film and (b) NiO nanocrystal, (c) schematic and (d) the energy-level diagram of the device [124,125] (color online).

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    Figure 10

    (a) Photoluminescence and (b) TRPL data of CH3NH3PbI3 contacted with different interfaces; (c) overall device structure, consisting of glass; (d) energy band alignment of the metal-oxide-based perovskite solar cell [129] (color online).

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    Figure 11

    (a) Cell configuration and (b) the cell energy level (versus vacuum) diagram of the inverted PSC with the structure of FTO/NiO/meso-Al2O3/CH3NH3PbI3/PCBM/BCP/Ag [137] (color online).

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    Figure 12

    Structure and band alignments of the PSC. (a) Diagram of the cell configuration highlighting the doped charge carrier extraction layers. The right panels show the composition of Ti(Nb)Ox and the crystal structure of Li+-doped NixMg1?xO, denoted as NiMg(Li)O. (b) A high-resolution crosssectional SEM image of a complete solar cell. (c) Band alignments of the solar cell [134] (color online).

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    Figure 13

    (a) Schematic device structure; (b) energy band diagram of the full solar device; (c) UPS spectra with the secondary-electron cutoff region and zoom-in of the valence band edge of Cu:Ni(ac) and UVO-Cu:Ni(ac) on the ITO substrate; (d) energy level alignment for the ITO/HTL junction [133] (color online).

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    Figure 14

    (a) Device structure of the polymer solar cells; (b) the HOMO and LUMO energy levels of the materials involved in the OSCs [52] (color online).

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    Figure 15

    (a) Preparation process for Cu2O and CuO films; (b) device structure; (c) energy level diagram [76].

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    Figure 16

    (a) Molecular structures of PCDTBT and PC70BM; (b) UPS spectra of ITO and MoOx films on ITO; (c) energy level diagram of the component materials in PCDTBT:PC70BM solar cells fabricated with MoOx as HTL [115].

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    Figure 17

    Schematic energy level diagrams of devices components referenced to the vacuum level. (a) S-MoO3; (b) MoO3; (c) MoO3/MoS2 [54,55] (color online).

  • Table 1   Performance parameters of OSCs with TMO films as interface layers

    Structure of device a)

    HTL prepared method and annealing temperature

    Voc (V)

    Jsc (mA/cm2)

    FF (%)

    PCE (%)

    Ref.

    ITO/NiO (10 nm)/ P3HT:PC61BM/Ca/Al

    Pulsed-laser deposition

    0.638

    11.3

    69.3

    5.16

    [51]

    ITO/NiOx/PCDTBT:PC70BM/Ca/Al

    Solution deposition, 300 °C

    0.879

    11.5

    65.0

    6.7

    [70]

    ITO/NiO(5 nm)/pDTG-TPD:PC71BM/LiF/Al

    Sol-gel deposition, 275 °C

    0.82

    13.9

    68.4

    7.8

    [59]

    ITO/NiO/TQ1:PC71BM/Ca/Al

    Chemistry combustion, 175 °C

    0.87

    10.50

    70.0

    6.42

    [113]

    ITO/CuOx/PCDTBT:PC71BM/Ca/Al

    Sol-gel deposition, 60 °C

    0.89

    10.58

    68.4

    6.44

    [71]

    ITO/CuOx/PBDTTT-C:PC61BM/Ca/Al

    Solution deposition, 80 °C

    0.71

    16.86

    59.7

    7.14

    [52]

    ITO/CuOx/P3HT:ICBA/Ca/Al

    Solution deposition, 80 °C

    0.86

    10.27

    71.3

    6.29

    [52]

    ITO/CuOx/P3HT:PC61BM/Ca/Al

    Solution deposition, 80 °C

    0.59

    9.11

    68.9

    3.70

    [52]

    FTO/CrOx (10 nm)/P3HT:PC60BM/Al

    reactive sputtering, 200 °C

    0.54

    10.97

    55.6

    3.28

    [53]

    ITO/CrOx/P3HT:ICBA/Ca/Al

    UVO treat in situ, room temperature

    0.87

    10.74

    70.3

    6.55

    [114]

    ITO/MoOx/P3HT: PC61BM/Al

    Solution deposition, 70 °C

    0.59

    9.5

    68

    3.8

    [81]

    ITO/MoOx/PCDTBT:PC70BM/ TiOx/Al

    Thermal evaporation

    0.89

    10.88

    67.2

    6.50

    [115]

    ITO/S-MoOx/P3HT:PC61BM/Al

    Sputtering method, 150 °C

    0.630

    10.05

    58.3

    3.69

    [54]

    ITO/MoO3/MoS2/P3HT:PC61BM/Al

    UVO treat in situ, room temperature

    0.627

    9.90

    67.1

    4.15

    [55]

    ITO/WO3/Si-PCPDTBT:PC70BM/ Ca/Ag

    Solution deposition, 80 °C

    0.616

    12.8

    60.4

    4.8

    [116]

    ITO/ZnO/α-PTPTBT:PC61BM/ VOx/Ag

    Solution deposition, room temperature

    0.82

    11.6

    0.53

    5.0

    [117]

    a)P3HT: poly(3-hexylthiophene); PC71/70/61BM: [6,6]-phenyl C71/70/61/-butyric acid methyl ester; PCDTBT:poly(N-9'-heptadecanyl-2,7-carbazole-alt-5,5- (4′,7′-di-2-thienyl-2′,1′,3′-benzothidiazole); pDTG-TPD: poly-dithienogermole-thienopyrrolodione; TQ1: poly[2,3-bis-(3-octyloxyphenyl)quinoxaline-5,8-diyl-alt-thiophene-2,5-diyl]; PBDTTT-C:poly(4,8-bis-alkyloxybenzo (1,2-b:4,5-b′)dithiophene-2,6-diyl-alt-(alkyl thieno(3,4-b)thiophene-2-carboxylate)-2,6-diyl); ICBA: indene-C60-bisadduct; Si-PCPDTBT: poly[(4,4′-bis(2-ethylhexyl) dithieno[3,2-b:2′,3′-d]silole)-2,6-diyl-alt-(4,7-bis(2-thienyl)-2,1,3-benzothiadiazole)-5,50-diyl]; α-PTPTBT: poly(thiophene-phenylene-thiophene)-(2,1,3-benzothiadiazole).

  • Table 2   Performance parameters of PSCs with TMO films as interface layers

    Structure of device a)

    HTL prepared method and annealing temperature

    The active or mask area of the device

    Voc (V)

    Jsc (mA/cm2)

    FF (%)

    PCE (%)

    Ref.

    ITO/NiOx/MAPbI3/PCBM/ BCP/Al

    Solution deposition, 300 °C

    0.06 cm2

    0.92

    12.43

    68

    7.8

    [63]

    ITO/NiOx/MAPbI3/PCBM/ BCP/Ag

    Solution deposition

    0.10 cm2

    0.994

    20.4

    66.8

    13.6

    [126]

    ITO/NiOx/NiOnc/MAPbI3/ PCBM/BCP/Al

    sputtering deposition, 150 °C

    0.96

    19.8

    61.0

    11.6

    [125]

    ITO/NiOx/CH3NH3PbI3/ZnO/Al

    Solution deposition, 300 °C

    0.10 cm2

    1.01

    21.0

    76.0

    16.1

    [129]

    ITO/NiOx/CH3NH3PbI3/ PCBM/LiF/Al

    Pulsed laser, 200 °C

    0.09 cm2

    1.06

    20.2

    81.3

    17.3

    [130]

    ITO/Cu:NiOx/MAPbI3/ PCBM/C60/Ag

    Sol-gel deposition, 275 °C

    0.0314 cm2

    1.11

    19.17

    72.0

    15.40

    [131]

    ITO/ NiOx/MAPbI3/PCBM/ C60/Ag

    Sol-gel deposition, 275 °C

    0.0314 cm2

    1.08

    14.42

    58.0

    8.94

    [131]

    ITO/Cu:NiOx/MAPbI3/C60/ Bis-C60/Ag

    Combustion method, 150 °C

    0.0314 cm2

    1.05

    22.23

    76.0

    17.74

    [132]

    ITO/Cu:NiOx/MAPbI3/C60/ Bis-C60/Ag

    Conventional sol-gel, 500 °C

    0.0314 cm2

    1.05

    20.53

    72.0

    15.52

    [132]

    ITO/UVO-Cu:Ni(ac)/MAPbI3/PCBM/Al

    Solution deposition, 245 °C

    1.00

    16.1

    67.0

    12.2

    [133]

    FTO/NiOx(Li:Mg)/MAPbI3/ PCBM/Ti(Nb)Ox/Ag

    Spray pyrolysis, 500 °C

    >1 cm2

    1.09

    20.4

    83.0

    18.4

    [134]

    ITO/Cu2Ox/MAPbI3/ PCBM/Ca/A1

    Chemical reaction method in situ, 100 °C

    0.04 cm2

    1.07

    16.52

    75.51

    13.35

    [76]

    ITO/CuO/MAPbI3/PCBM//Ca/A1

    Annealing, 250 °C

    0.04 cm2

    1.06

    15.82

    72.54

    12.16

    [76]

    ITO/CuOx/MAPbI3/ PCBM/C60/BCP/Ag

    Solution deposition, 80 °C

    0.10 cm2

    1.01

    20.1

    70.6

    14.4

    [135]

    ITO/CuOx/MAPbI3?xClx/ PCBM/C60/BCP/Ag

    Solution deposition, 80 °C

    0.10 cm2

    1.11

    22.5

    75.8

    19.0

    [135]

    FTO/Cu:CrOx/MAPbI3/PCBM/Al

    Sputtering deposition, 200 °C

    0.09 cm2

    0.99

    16.33

    70.0

    11.48

    [37]

    ITO/WO3/MAPbI3/PCBM/Al

    Solvo-thermal method, 200 °C

    0.04 cm2

    0.92

    18.10

    64.0

    7.68

    [136]

    a)BCP: bathocuproine.

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