Pyrolysis preparation of WO<sub>3</sub> thin films using ammonium metatungstate DMF/water solution for efficient compact layers in planar perovskite solar cells

Abstract: The tungsten trioxide(WO₃) thin films were firstly prepared by spin-coating-pyrolysis methods using the ammonium metatungstate((NH₄)₆H₂W₁₂O₄₀) DMF/water solution, and successfully applied as the efficient compact layers for the planar perovskite solar cells. The influence of the WO₃ film thickness and the rinsing treatment of CH₃NH₃PbI₃ thin film with isopropanol on the photovoltaic performance of the corresponding perovskite solar cells was systematically investigated. The results revealed that the perovskite solar cell with a 62 nm thick WO₃ compact layer achieved a photoelectric conversion efficiency of 5.72%, with a short circuit photocurrent density of 17.39 mA/cm², an open circuit voltage of 0.58 V and a fill factor of 0.57. The photoelectric conversion efficiency was improved from 5.72% to 7.04% by the isopropanol rinsing treatment.

Key words: WO₃ thin film, ammonium metatungstate DMF/water solution, pyrolysis, compact layer, perovskite solar cell

References:

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[28]	Bertus L M, Enesca A, Duta A. Influence of spray pyrolysis deposition parameters on the optoelectronic properties of WO₃ thin films[J]. Thin Solid Films, 2012, 520: 4282.
[29]	Sun Y P, Murphy C J, Reyes-Gil K R. Photoelectrochemical and structural characterization of carbon-doped WO₃ films prepared via spray pyrolysis[J]. Int J Hydrogen Energy, 2009, 34: 8476.
[30]	Sivakumar R, Moses Ezhil Raj A, Subramanian B. Preparation and characterization of spray deposited n-type WO₃ thin films for electrochromic devices[J]. Mater Res Bull, 2004, 39: 1479.
[31]	Chen Q, Zhou H, Hong Z. Planar heterojunction perovskite solar cells via vapor-assisted solution process[J]. J Am Chem Soc, 2014, 136: 622.

[1]	Eperon G E, Stranks S D, Menelaou C. Formamidinium lead trihalide:a broadly tunable perovskite for efficient planar heterojunction solar cells[J]. Energy Environ Sci, 2014, 7: 982.
[2]	Green M A, Emery K, Hishikawa Y. Solar cell efficiency tables(Version 45)[J]. Prog Photovolt:Res Appl, 2015, 23: 1.
[3]	Minemoto T, Murata M. Theoretical analysis on effect of band offsets in perovskite solar cells[J]. Sol Energ Mater Sol Cells, 2015, 133: 8.
[4]	Jeon N J, Noh J H, Kim Y C. Solvent engineering for high-performance inorganic-organic hybrid perovskite solar cells[J]. Nat Mater, 2014, 13: 897.
[5]	Zhou H, Chen Q, Li G. Interface engineering of highly efficient perovskite solar cells[J]. Science, 2014, 345: 542.
[6]	Xing G, Mathews N, Sun S. Long-range balanced electron and hole-transport lengths in organic-inorganic CH₃NH₃PbI₃[J]. Science, 2013, 342: 344.
[7]	Stranks S D, Eperon G E, Grancini G. Electron-hole diffusion lengths exceeding 1 micrometer in an organometal trihalide perovskite absorber[J]. Science, 2013, 342: 341.
[8]	Im J H, Lee C R, Lee J W. 6.5% efficient perovskite quantum-dot-sensitized solar cell. Nanoscale[J]. , 2011, 3: 4088.
[9]	Jeng J Y, Chen K C, Chiang T Y. Nickel oxide electrode interlayer in CH₃NH₃PbI₃ perovskite/PCBM planar-heterojunction hybrid solar cells[J]. Adv Mater, 2014, 26: 4107.
[10]	Etgar L, Gao P, Xue Z. Mesoscopic CH₃NH₃PbI₃/TiO₂ hetero-junction solar cells[J]. J Am Chem Soc, 2012, 134: 17396.
[11]	Heo J H, Im S H, Noh J H. Efficient inorganic-organic hybrid heterojunction solar cells containing perovskite compound and polymeric hole conductors[J]. Nat Photonics, 2013, 7: 486.
[12]	He M, Zheng D, Wang M. High efficiency perovskite solar cells:from complex nanostructure to planar heterojunction[J]. J Mater Chem, 2014, 2: 5994.
[13]	Yong S M, Nikolay T, Ahn B T. One-dimensional WO₃ nanorods as photoelectrodes for dye-sensitized solar cells[J]. J Alloys Compd, 2013, 547: 113.
[14]	Zheng H D, Tachibana Y, Kalantar-zadeh K. Dye-sensitized solar cells based on WO₃[J]. Langmuir, 2010, 26: 19148.
[15]	Xiao M W, Wang L S, Huang X J. Synthesis and characterization of WO₃/titanate nanotubes nanocomposite with enhanced photocatalytic properties[J]. J Alloys Compd, 2009, 470: 486.
[16]	Yang H, Shi R, Zhang K. Synthesis of WO₃/TiO₂ nanocomposites via sol-gel method[J]. J Alloys Compd, 2005, 398: 200.
[17]	Yan F, Chen D, Li W. The ternary system Na₂O-ZnO-WO₃:compounds and phase relationships[J]. J Alloys Compd, 2008, 458: 138.
[18]	Mahmood K, Swain B S, Kirmania A R. Highly efficient perovskite solar cells based on a nanostructured WO₃-TiO₂ core-shell electron transporting material[J]. J Mater Chem, 2015, 3: 9051.
[19]	Jayatissa A H, Cheng S T, Gupta T. Annealing effect on the formation of nanocrystals in thermally evaporated tungsten oxide thin films[J]. Mater Sci Eng, 2004, 109: 269.
[20]	Stankova M, Vilanova X, Llobet E. Influence of the annealing and operating temperatures on the gas-sensing properties of RF sputtered WO₃ thin-film sensors[J]. Sens Actuators B:Chem, 2005, 105: 271.
[21]	Vijayalakshmi R, Jayachandran M, Sanjeeviraja C. Structural, electrochromic and FT-IR studies on electrodeposited tungsten trioxide films[J]. Curr Appl Phys, 2003, 3: 171.
[22]	Krasnov Y S, Kolbasov G Y. Electrochromism and reversible changes in the position of fundamental absorption edge in cathodically deposited amorphous WO₃[J]. Electrochim Acta, 2004, 49: 2425.
[23]	Subrahmanyam A, Karuppasamy A. Optical and electrochromic properties of oxygen sputtered tungsten oxide(WO₃) thin films[J]. Sol Energy Mater Sol Cells, 2007, 91: 266.
[24]	Tanner R E, Szekeres A, Gogova D. Study of the surface roughness of CVD-tungsten oxide thin films[J]. Appl Surf Sci, 2003, 218: 163.
[25]	Gesheva K A, Popkirov G, Ganchev M. Electrochromic properties of atmospheric CVD MoO₃ and MoO₃-WO₃ films and their application in electrochromic devices[J]. Mater Sci Eng, 2005, 119: 232.
[26]	Deepa M, Saxena T K, Singh D P. Spin coated versus dip coated electrochromic tungsten oxide films:structure, morphology, optical and electrochemical properties[J]. Electrochim Acta, 2006, 51: 1974.
[27]	Patra A, Auddy K, Ganguli D. Sol-gel electrochromic WO₃ coatings on glass[J]. Mater Lett, 2004, 58: 1059.
[28]	Bertus L M, Enesca A, Duta A. Influence of spray pyrolysis deposition parameters on the optoelectronic properties of WO₃ thin films[J]. Thin Solid Films, 2012, 520: 4282.
[29]	Sun Y P, Murphy C J, Reyes-Gil K R. Photoelectrochemical and structural characterization of carbon-doped WO₃ films prepared via spray pyrolysis[J]. Int J Hydrogen Energy, 2009, 34: 8476.
[30]	Sivakumar R, Moses Ezhil Raj A, Subramanian B. Preparation and characterization of spray deposited n-type WO₃ thin films for electrochromic devices[J]. Mater Res Bull, 2004, 39: 1479.
[31]	Chen Q, Zhou H, Hong Z. Planar heterojunction perovskite solar cells via vapor-assisted solution process[J]. J Am Chem Soc, 2014, 136: 622.

Pyrolysis preparation of WO₃ thin films using ammonium metatungstate DMF/water solution for efficient compact layers in planar perovskite solar cells

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