Novel seed-assisted synthesis of indium tin oxide submicro-cubes and their resistivity

Abstract

Indium tin oxide films, an important n-type semiconductor oxide, show great prospects in optoelectronic device applications. Consequently, as a key raw material of targets for sputtering films, it is important to prepare low-resistivity indium tin oxide powders. Herein, low-resistivity indium tin oxide submicro-cubes are synthesized by a seed-assisted coprecipitation method. The effects of seed content, In³⁺ concentration, aging time, reaction temperature and calcination temperature on resistivity were investigated by single factor and orthogonal experiments. To ensure reliability and reproducibility of data, each experiment was repeated three times and resistivity of each sample was measured three times to obtain average value. The results indicated that optimal sample was matched with cubic phase In₂O₃. The single-crystal indium tin oxide particles exhibited a regular cubic shape with a size of nearly 500 nm and low resistivity of 0.814 Ω·cm. Compared with particles prepared by the conventional coprecipitation method, indium tin oxide submicro-cubes showed good dispersion. The presence of seed particles provided nucleation sites with lower energy barriers and promoted formation of submicro-cubes. The face-to-face contact among particles and good dispersion contributed to electron transfer, resulting in lower resistivity. The seed-assisted synthesis provides a novel way to prepare low-resistivity indium tin oxide submicro-cubes.

Graphical abstract

Keywords

indium tin oxide / submicro-cubes / resistivity / seed-assisted coprecipitation method / orthogonal experiment

References

[1] Medvedovski E, Alvarez N A, Szepesi C J, Yankov O, Lippens P. Advanced indium tin oxide ceramic sputtering targets (rotary and planar) for transparent conductive nanosized films. Advances in Applied Ceramics, 2013, 112(5): 243–256

[2] Ma Y, Zhai X, Liu J. Synthesis of hexagonal-phase indium tin oxide nanoparticles by deionized water and glycerol binary solvothermal method and their resistivity. Journal of Materials Science, 2020, 55(9): 3860–3870

[3] Mei F, Yuan T, Li R, Qin K, Zhou L, Wang W. Micro-structure of ITO ceramics sintered at different temperatures and its effect on the properties of deposited ITO films. Journal of the European Ceramic Society, 2018, 38(2): 521–533

[4] Song X, Dong G, Gao F, Xiao Y, Liu Q, Diao X. Properties of NiO_x and its influence upon all-thin-film ITO/NiO_x/LiTaO₃/WO₃/ITO electrochromic devices prepared by magnetron sputtering. Vacuum, 2015, 111: 48–54

[5] Sun C, Cheng C H, Zhang B L, Li R X, Wang Y, Liu W F, Luo Y M, Du G T, Cong S L. Green and low-cost approach to modify the indium tin oxide anodes in organic light-emitting diodes by electrochemical treatment in NaCl aqueous solution. Applied Surface Science, 2017, 422: 125–129

[6] Li L, Wang M, Fang Y, Qiao S. Investigation of electrochemical degradation and application of e-paper dyes in organic solvents. Frontiers of Chemical Science and Engineering, 2009, 3(2): 182–185

[7] Canhola P, Martins N, Raniero L, Pereira S, Fortunato E, Ferreira I, Martins R. Role of annealing environment on the performances of large area ITO films produced by rf magnetron sputtering. Thin Solid Films, 2005, 487(1–2): 271–276

[8] Baía I, Quintela M, Mendes L, Nunes P, Martins R. Performances exhibited by large area ITO layers produced by r.f. magnetron sputtering. Thin Solid Films, 1999, 337(1–2): 171–175

[9] Chen Y, Zhai X, Liu J. One-step solvothermal synthesis of cubic ITO nanopowders. Rare Metal Materials and Engineering, 2019, 48(7): 2358–2363 (in Chinese)

[10] Saito Y, Matsuno T, Guo Q, Mori T, Kashiwagi M, Shimojima A, Wada H, Kuroda K. Preparation of ordered nanoporous indium tin oxides with large crystallites and individual control over their thermal and electrical conductivities. ACS Applied Materials & Interfaces, 2021, 13(13): 15373–15382

[11] Zhai X, Chen Y, Ma Y, Liu Y, Liu J. Fabrication of monodisperse ITO submicro-spheres using L-Histidine-assisted one-step solvothermal method. Ceramics International, 2019, 45(14): 17562–17566

[12] Liu T, Zhai X, Liu J. Optimum preparation of low-resistivity indium tin oxide nanopowders via polyacrylamide gel route using orthogonal experiment. Journal of Materials Science Materials in Electronics, 2021, 32(17): 22232–22244

[13] Aziz M A, Zahir M H, Shaikh M N, Al-Betar A R, Oyama M, Sulaiman K O. Hydrothermal synthesis of tin-doped indium oxide nanoparticles using pamoic acid as an organic additive and their photoluminescence properties. Journal of Materials Science Materials in Electronics, 2017, 28(4): 3226–3233

[14] Pan K Y, Lin L D, Chang L W, Shih H C. Studies on the optoelectronic properties of the thermally evaporated tin-doped indium oxide nanostructures. Applied Surface Science, 2013, 273: 12–18

[15] Li L, Chen S, Kim J, Xu C, Zhao Y, Ziegler K J. Controlled synthesis of tin-doped indium oxide (ITO) nanowires. Journal of Crystal Growth, 2015, 413: 31–36

[16] Patel N G, Patel P D, Vaishnav V S. Indium tin oxide (ITO) thin film gas sensor for detection of methanol at room temperature. Sensors and Actuators B: Chemical, 2003, 96(1–2): 180–189

[17] Ayeshamariam A, Kashif M, Bououdina M, Hashim U, Jayachandran M, Ali M E. Morphological, structural, and gas-sensing characterization of tin-doped indium oxide nanoparticles. Ceramics International, 2014, 40(1): 1321–1328

[18] Wang H W, Xu G D, Zhang J R, Yin X. Hydrothermal synthesis of indium tin oxide nanoparticles without chlorine contamination. Bulletin of the Korean Chemical Society, 2014, 35(7): 1999–2003

[19] Sasaki T, Endo Y, Nakaya M, Kanie K, Nagatomi A, Tanoue K, Nakamura R, Muramatsu A. One-step solvothermal synthesis of cubic-shaped ITO nanoparticles precisely controlled in size and shape and their electrical resistivity. Journal of Materials Chemistry, 2010, 20(37): 8153–8157

[20] Bouzidi A, Omri K, Mir L E, Guermazi H. Prepration, structural and optical investigations of ITO nanopowder and ITO/epoxy nanocomposites. Materials Science in Semiconductor Processing, 2015, 39: 536–543

[21] Jiang Z, Liu T, Zhai X, Liu J. Optimization preparation of indium tin oxide nanoparticles via microemulsion method using orthogonal experiment. Crystals, 2021, 11(11): 1387

[22] Seo K H, Lee J H, Kim J J, Bertoni M I, Ingram B J, Mason T O. Synthesis and electrical characterization of the polymorphic indium tin oxide nanocrystalline powders. Journal of the American Ceramic Society, 2006, 89(11): 3431–3436

[23] Jafari A, Ganjkhanlou Y, Kazemzad M, Ghorbani H. Effect of surfactants on the size, color, photoluminescence and resistivity of indium tin oxide nanoparticles prepared by co-precipitation method. Surface Review and Letters, 2012, 19(5): 1250054

[24] Senthilkumar V, Senthil K, Vickraman P. Microstructural, electrical and optical properties of indium tin oxide (ITO) nanoparticles synthesized by co-precipitation method. Materials Research Bulletin, 2012, 47(4): 1051–1056

[25] Ahmed N M, Sabah F A, Abdulgafour H I, Alsadig A, Sulieman A, Alkhoaryef M. The effect of post annealing temperature on grain size of indium-tin-oxide for optical and electrical properties improvement. Results in Physics, 2019, 13: 102159

[26] Lee J H, Kim Y H, Ahn S J, Ha T H, Kim H S. Grain-size effect on the electrical properties of nanocrystalline indium tin oxide thin films. Materials Science and Engineering B, 2015, 199: 37–41

[27] Boehme M, Charton C. Properties of ITO on PET film in dependence on the coating conditions and thermal processing. Surface and Coatings Technology, 2005, 200(1–4): 932–935

[28] Kobayashi Y, Mabuchi Y, Hama M, Inoue K, Yasuda Y, Morita T. Seeding technique for lowering temperature during synthesis of α-alumina. Journal of Asian Ceramic Societies, 2015, 3(1): 139–143

[29] Ma Y, Liang F, Liu Y, Zhai X, Liu J. Effect of dispersion on visible light transmittance and resistivity of indium tin oxide nanoparticles prepared by cetyltrimethylammonium bromide-assisted coprecipitation method. Journal of Materials Science Materials in Electronics, 2019, 30(19): 17963–17971

[30] Jalilpour M, Fathalilou M. Effect of aging time and calcination temperature on the cerium oxide nanoparticles synthesis via reverse co-precipitation method. International Journal of Physical Sciences, 2012, 7(6): 944–948

[31] Li X, Wei K, Liang X. Study on preparing nanosized ITO powder by chemical liquid phase coprecipitation process. Metal Mine, 2008, 38(9): 73–77 (in Chinese)

[32] Guo Y, Yang B, Xu B, Liu D, Feng T. Study on reagents and effecting factors in preparation process of indium tin oxide nano-powders. Materials Reports, 2007, 21: 156–158 (in Chinese)

[33] Huang J, Chen C, Huang Z, Fu J, Chen S, Jiang Y, Lu L, Xia Y, Zhao X. Preparation and growth mechanism of the flower-like whiskers of γ-, θ-, and α-Al₂O₃ phases by homogeneous precipitation/calcination method. Ceramics International, 2021, 47(12): 16943–16949

[34] Zhang Y, Liu J. Hydrothermal preparation of cubic ITO powder and its photoelectric performance. Chemical Journal of Chinese Universities, 2017, 38(7): 1110–1116 (in Chinese)

[35] Wang H, Xu X, Li X, Zhang J, Li C. Synthesis and sintering of indium tin oxide nanoparticles by citrate-nitrate combustion method. Rare Metals, 2010, 29(4): 355–360

[36] Shan W, Wu L, Tao N, Chen Y, Guo D. Optimization method for green SrAl₂O₄:Eu²⁺, Dy³⁺ phosphors synthesized via co-precipitation route assisted by microwave irradiation using orthogonal experimental design. Ceramics International, 2015, 41(10): 15034–15040

[37] Zhu J, Chew D A S, Lv S, Wu W. Optimization method for building envelope design to minimize carbon emissions of building operational energy consumption using orthogonal experimental design (OED). Habitat International, 2013, 37: 148–154

[38] Tan Y, Luo X, Mao M, Shu D, Shan W, Li G, Guo D. Optimization red emission of SrMoO₄:Eu³⁺ via hydro-thermal co-precipitation synthesis using orthogonal experiment. Current Applied Physics, 2018, 18(11): 1403–1409

[39] Hu X, Yang H, Guo T, Shu D, Shan W, Li G, Guo D. Preparation and properties of Eu and Dy co-doped strontium aluminate long afterglow nanomaterials. Ceramics International, 2018, 44(7): 7535–7544

[40] Duan Y, Ye R, Yan X, Dai C, Tan J, Xu G. Effects of pH value and calcining temperature on indium tin oxide nanopowder synthesized by co-precipitation. Materials Science and Engineering of Powder Metallurgy, 2014, 19(3): 413–420 (in Chinese)

[41] Kim S M, Seo K H, Lee J H, Kim J J, Lee H Y, Lee J S. Preparation and sintering of nanocrystalline ITO powders with different SnO₂ content. Journal of the European Ceramic Society, 2006, 26(1–2): 73–80

[42] Tang A, Li X, Zhou Z, Ouyang J, Yang H. Mechanochemical synthesis of Ni(OH)₂ and the decomposition to NiO nanoparticles: thermodynamic and optical spectra. Journal of Alloys and Compounds, 2014, 600: 204–209

[43] Rakhshani M, Kamrannejad M M, Babaluo A A, Rezaei M, Aghjeh M R. Thermal degradation behavior and kinetic studies of polyacrylamide gel in TiO₂ nanoparticles synthesis. Iranian Polymer Journal, 2012, 21(12): 821–828

[44] Li S Y, Lee C Y, Lin P, Tseng T Y. Low temperature synthesized Sn doped indium oxide nanowires. Nanotechnology, 2005, 16(4): 451–457

[45] Jung J, Kim D H. Growth evolution of self-catalytic tin-doped indium oxide nanowires. Journal of Alloys and Compounds, 2020, 823: 153648

[46] Lu J, Minami K, Takami S, Shibata M, Kaneko Y, Adschiri T. Supercritical hydrothermal synthesis and in situ organic modification of indium tin oxide nanoparticles using continuous-flow reaction system. ACS Applied Materials & Interfaces, 2012, 4(1): 351–354

[47] Nguyen A K Q, Huynh T T, Ho V T T. Preparation and characterization of indium doped tin oxide (ITO) via a non-aqueous sol−gel. Molecular Crystals and Liquid Crystals, 2016, 635(1): 32–39

[48] Kim K Y, Park S B. Preparation and property control of nano-sized indium tin oxide particle. Materials Chemistry and Physics, 2004, 86(1): 210–221

[49] Ray S, Banerjee R, Basu N, Batabyal A K, Barua A K. Properties of tin doped indium oxide thin films prepared by magnetron sputtering. Journal of Applied Physics, 1983, 54(6): 3497–3501

[50] Fang X, Bando Y, Shen G, Ye C, Gautam U K, Costa P M F J, Zhi C, Tang C, Golberg D. Ultrafine ZnS nanobelts as field emitters. Advanced Materials, 2007, 19(18): 2593–2596

[51] Walsh A, Da Silva J L F, Wei S H, Körber C, Klein A, Piper L F J, DeMasi A, Smith K E, Panaccione G, Torelli P, Payne D J, Bourlange A, Egdell R G. Nature of the band gap of In₂O₃ revealed by first-principles calculations and X-ray spectroscopy. Physical Review Letters, 2008, 100(16): 167402

[52] Cuya Huaman J L, Tanoue K, Miyamura H, Matsumoto T, Jeyadevan B. Large-scale synthesis of ITO nanoparticles in an alcohol system assisted by acids. New Journal of Chemistry, 2014, 38(8): 3421–3428

[53] Amin M, Ehsani N, Mozafarinia R. Effect of seeding and carbon content on the formation and microstructure of Ca-α-SiAlON. International Journal of Refractory & Hard Metals, 2019, 82: 208–214

[54] Zhou S, Wang H, Zhong L, Li G. Synthesis and luminescence properties of cubic-shaped Ca_1–xTiO₃:Eu³⁺ particles. Luminescence, 2018, 33(2): 443–449

[55] Li S, Qiao X, Chen J, Wang H, Jia F, Qiu X. Effects of temperature on indium tin oxide particles synthesized by co-precipitation. Journal of Crystal Growth, 2006, 289(1): 151–156

RIGHTS & PERMISSIONS

Higher Education Press