Gram-scale synthesis of catalytic Co9S8 nanocrystal ink as a cathode material for spray-deposited, large-area dye-sensitized solar cells.

We report the development of Co9S8 nanocrystals as a cost-effective cathode material that can be readily combined with spraying techniques to fabricate large-area dye-sensitized solar cell (DSSC) devices and can be further connected with series or parallel cell architectures to obtain a relatively high output voltage or current. A gram-scale synthesis of Co9S8 nanocrystal is carried out via a noninjection reaction by mixing anhydrous CoCl2 with trioctylphosphine (TOP), dodecanethiol and oleylamine (OLA) at 250 °C. The Co9S8 nanocrystals possess excellent catalytic ability with respect to I(-)/I3(-) redox reactions. The Co9S8 nanocrystals are prepared as nanoinks to fabricate uniform, crack-free Co9S8 thin films on different substrates by using a spray deposition technique. These Co9S8 films are used as counter electrodes assembled with dye-adsorbed TiO2 photoanodes to fabricate DSSC devices having a working area of 2 cm(2) and an average power conversion efficiency (PCE) of 7.02 ± 0.18% under AM 1.5 solar illumination, which is comparable with the PCE of 7.2 ± 0.12% obtained using a Pt cathode. Furthermore, six 2 cm(2)-sized DSSC devices connected in series output an open-circuit voltage of 4.2 V that can power a wide range of electronic devices such as LED arrays and can charge commercial lithium ion batteries.

[1]  K. Ho,et al.  FeS2 nanocrystal ink as a catalytic electrode for dye-sensitized solar cells. , 2013, Angewandte Chemie.

[2]  Qiao Liu,et al.  A general and controllable synthesis of ComSn (Co9S8, Co3S4, and Co1−xS) hierarchical microspheres with homogeneous phases , 2013 .

[3]  Pralay K. Santra,et al.  Earth-Abundant Cobalt Pyrite (CoS2) Thin Film on Glass as a Robust, High-Performance Counter Electrode for Quantum Dot-Sensitized Solar Cells. , 2013, The journal of physical chemistry letters.

[4]  Haijun Zhang,et al.  Synthesis and Catalytic Properties of Sb2S3 Nanowire Bundles as Counter Electrodes for Dye-Sensitized Solar Cells , 2013 .

[5]  John Watt,et al.  How to control the shape of metal nanostructures in organic solution phase synthesis for plasmonics and catalysis , 2013 .

[6]  Zhong‐Sheng Wang,et al.  NiS2/Reduced Graphene Oxide Nanocomposites for Efficient Dye-Sensitized Solar Cells , 2013 .

[7]  Xiaohe Liu,et al.  Shape evolution and electrochemical properties of cobalt sulfide via a biomolecule-assisted solvothermal route , 2013 .

[8]  K. Ryan,et al.  Systematic Study into the Synthesis and Shape Development in Colloidal CuInxGa1–xS2 Nanocrystals , 2013 .

[9]  Yi Xie,et al.  In-plane coassembly route to atomically thick inorganic-organic hybrid nanosheets. , 2013, ACS nano.

[10]  Song Jin,et al.  Synthesis, characterization, and variable range hopping transport of pyrite (FeS₂) nanorods, nanobelts, and nanoplates. , 2013, ACS nano.

[11]  N. Kotov,et al.  Universal Synthesis of Single-Phase Pyrite FeS2 Nanoparticles, Nanowires, and Nanosheets , 2013 .

[12]  Shery L. Y. Chang,et al.  Shape control from thermodynamic growth conditions: the case of hcp ruthenium hourglass nanocrystals. , 2013, Journal of the American Chemical Society.

[13]  M. Ikegami,et al.  Nickel Oxide Hybridized Carbon Film as an Efficient Mesoscopic Cathode for Dye-Sensitized Solar Cells , 2013 .

[14]  Justin T. Harris,et al.  Pyrite Nanocrystal Solar Cells: Promising, or Fool's Gold? , 2012, The journal of physical chemistry letters.

[15]  K. Ryan,et al.  Assembly of CuIn(1-x)Ga(x)S2 nanorods into highly ordered 2D and 3D superstructures. , 2012, ACS nano.

[16]  Kuo-Chuan Ho,et al.  CoS acicular nanorod arrays for the counter electrode of an efficient dye-sensitized solar cell. , 2012, ACS nano.

[17]  Xin Xu,et al.  In situ growth of Co(0.85)Se and Ni(0.85)Se on conductive substrates as high-performance counter electrodes for dye-sensitized solar cells. , 2012, Journal of the American Chemical Society.

[18]  Alagesan Subramanian,et al.  Effects of boron doping in TiO2 nanotubes and the performance of dye-sensitized solar cells , 2012 .

[19]  Ming He,et al.  Low‐Cost Copper Zinc Tin Sulfide Counter Electrodes for High‐Efficiency Dye‐Sensitized Solar Cells. , 2012 .

[20]  Sen Li,et al.  Synthesis of CdS, ZnS, and CdS/ZnS Core/Shell Nanocrystals Using Dodecanethiol , 2012 .

[21]  Wei Guo,et al.  Economical Pt-free catalysts for counter electrodes of dye-sensitized solar cells. , 2012, Journal of the American Chemical Society.

[22]  K. Ryan,et al.  Colloidal synthesis of wurtzite Cu2ZnSnS4 nanorods and their perpendicular assembly. , 2012, Journal of the American Chemical Society.

[23]  G. Calogero,et al.  A new type of transparent and low cost counter-electrode based on platinum nanoparticles for dye-sensitized solar cells , 2011 .

[24]  Xueping Gao,et al.  Highly Pt-like electrocatalytic activity of transition metal nitrides for dye-sensitized solar cells , 2011 .

[25]  P. Etchegoin,et al.  Synthesis and Comparison of the Magnetic Properties of Iron Sulfide Spinel and Iron Oxide Spinel Nanocrystals , 2011 .

[26]  N. Alonso‐Vante 5 Structure and Reactivity of Transition Metal Chalcogenides toward the Molecular Oxygen Reduction Reaction , 2011 .

[27]  Shuhong Yu,et al.  Hierarchical hollow Co9S8 microspheres: solvothermal synthesis, magnetic, electrochemical, and electrocatalytic properties. , 2010, Chemistry.

[28]  T. Hanrath,et al.  SnSe nanocrystals: synthesis, structure, optical properties, and surface chemistry. , 2010, Journal of the American Chemical Society.

[29]  Zhenghua Wang,et al.  Co9S8 nanotubes synthesized on the basis of nanoscale Kirkendall effect and their magnetic and electrochemical properties , 2010 .

[30]  Chen Xu,et al.  Planar waveguide-nanowire integrated three-dimensional dye-sensitized solar cells. , 2010, Nano letters.

[31]  Xueping Gao,et al.  Carbon nanotubes with titanium nitride as a low-cost counter-electrode material for dye-sensitized solar cells. , 2010, Angewandte Chemie.

[32]  F. Kong,et al.  Influence of Different Electrolytes on the Reaction Mechanism of a Triiodide/Iodide Redox Couple on the Platinized FTO Glass Electrode in Dye-Sensitized Solar Cells , 2010 .

[33]  Yaguang Wei,et al.  Optical fiber/nanowire hybrid structures for efficient three-dimensional dye-sensitized solar cells. , 2009, Angewandte Chemie.

[34]  Xueping Gao,et al.  Highly ordered TiN nanotube arrays as counter electrodes for dye-sensitized solar cells. , 2009, Chemical communications.

[35]  M. Grätzel,et al.  CoS supersedes Pt as efficient electrocatalyst for triiodide reduction in dye-sensitized solar cells. , 2009, Journal of the American Chemical Society.

[36]  Yanhong Luo,et al.  A flexible carbon counter electrode for dye-sensitized solar cells , 2009 .

[37]  Byung-Ryool Hyun,et al.  PbSe nanocrystal excitonic solar cells. , 2009, Nano letters.

[38]  Jaesung Song,et al.  Efficient dye-sensitized solar cells with catalytic multiwall carbon nanotube counter electrodes. , 2009, ACS applied materials & interfaces.

[39]  Kuo-Chuan Ho,et al.  EIS analysis on low temperature fabrication of TiO2 porous films for dye-sensitized solar cells , 2008 .

[40]  Zhang Lan,et al.  High-performance polypyrrole nanoparticles counter electrode for dye-sensitized solar cells , 2008 .

[41]  Miaoliang Huang,et al.  Improvement of performance of dye-sensitized solar cells based on electrodeposited-platinum counter electrode , 2008 .

[42]  K. Sumiyama,et al.  Low polydispersed copper-sulfide nanocrystals derived from various Cu-alkyl amine complexes. , 2008, Journal of colloid and interface science.

[43]  Won-Seok Chae,et al.  Enhanced performance of a dye-sensitized solar cell with an electrodeposited-platinum counter electrode , 2008 .

[44]  Takurou N. Murakami,et al.  Counter electrodes for DSC: Application of functional materials as catalysts , 2008 .

[45]  Jaesung Song,et al.  Nanocarbon counterelectrode for dye sensitized solar cells , 2007 .

[46]  A. Alivisatos,et al.  Colloidal Synthesis of Hollow Cobalt Sulfide Nanocrystals , 2006 .

[47]  Tobias Schmidt,et al.  Development of a generalized parameter window for cold spray deposition , 2006 .

[48]  A. Anderson,et al.  Co9S8 as a catalyst for electroreduction of O2: quantum chemistry predictions. , 2006, The journal of physical chemistry. B.

[49]  B. Korgel,et al.  Nickel sulfide and copper sulfide nanocrystal synthesis and polymorphism. , 2005, Langmuir : the ACS journal of surfaces and colloids.

[50]  H. Wenk,et al.  Minerals: Their Constitution and Origin , 2004 .

[51]  I. Chorkendorff,et al.  A combined X-Ray photoelectron and Mössbauer emission spectroscopy study of the state of cobalt in sulfided, supported, and unsupported CoMo catalysts , 1982 .

[52]  C. Rao,et al.  Transition metal sulfides , 1976 .

[53]  S. Geller Refinement of the crystal structure of Co9S8 , 1962 .

[54]  A. I. Popov,et al.  Studies on the Chemistry of Halogen and of Polyhalides. XIII. Voltammetry of Iodine Species in Acetonitrile , 1958 .