High-efficiency "green" quantum dot solar cells.

Semiconductor quantum dots (QDs) are extremely interesting materials for the development of photovoltaic devices, but currently the present the drawback is that the most efficient devices have been prepared with toxic heavy metals of Cd or Pb. Solar cells based on "green" QDs--totally free of Cd or Pb--present a modest efficiency of 2.52%. Herein we achieve effective surface passivation of the ternary CuInS2 (CIS) QDs that provides high photovoltaic quality core/shell CIS/ZnS (CIS-Z) QDs, leading to the development of high-efficiency green QD solar cells that surpass the performance of those based on the toxic cadmium and lead chalcogenides QDs. Using wide absorption range QDs, CIS-Z-based quantum dot sensitized solar cell (QDSC) configuration with high QD loading and with the benefit of the recombination reduction with type-I core/shell structure, we boost the power conversion efficiency of Cd- and Pb-free QDSC to a record of 7.04% (with certified efficiency of 6.66%) under AM 1.5G one sun irradiation. This efficiency is the best performance to date for QDSCs and also demonstrates that it is possible to obtain comparable or even better photovoltaic performance from green CIS QDs to the toxic cadmium and lead chalcogenides QDs.

[1]  J. Bisquert,et al.  Titanium dioxide nanomaterials for photovoltaic applications. , 2014, Chemical reviews.

[2]  Emilio Palomares,et al.  Quantum dot based molecular solar cells , 2014 .

[3]  X. Zhong,et al.  Electroplating Cuprous Sulfide Counter Electrode for High-Efficiency Long-Term Stability Quantum Dot Sensitized Solar Cells , 2014 .

[4]  Illan J. Kramer,et al.  The architecture of colloidal quantum dot solar cells: materials to devices. , 2014, Chemical reviews.

[5]  S. Bent,et al.  Interface Engineering in Inorganic-Absorber Nanostructured Solar Cells. , 2014, The journal of physical chemistry letters.

[6]  N. Makarov,et al.  An integrated approach to realizing high-performance liquid-junction quantum dot sensitized solar cells , 2013, Nature Communications.

[7]  Wen Chen,et al.  Efficiency enhancement of TiO2 nanodendrite array electrodes in CuInS2 quantum dot sensitized solar cells , 2013 .

[8]  Y. Rui,et al.  A facile in situ synthesis route for CuInS(2) quantum-dots/In(2)S(3) co-sensitized photoanodes with high photoelectric performance. , 2013, ACS applied materials & interfaces.

[9]  Cheng-Hsien Yang,et al.  Synthesis of eco-friendly CuInS2 quantum dot-sensitized solar cells by a combined ex situ/in situ growth approach. , 2013, ACS applied materials & interfaces.

[10]  J. Bisquert,et al.  Core/shell colloidal quantum dot exciplex states for the development of highly efficient quantum-dot-sensitized solar cells. , 2013, Journal of the American Chemical Society.

[11]  Jia-Yaw Chang,et al.  Improved performance of CuInS2 quantum dot-sensitized solar cells based on a multilayered architecture. , 2013, ACS applied materials & interfaces.

[12]  H. Momose,et al.  Huge suppression of charge recombination in P3HT-ZnO organic-inorganic hybrid solar cells by locating dyes at the ZnO/P3HT interfaces. , 2013, Physical chemistry chemical physics : PCCP.

[13]  Juan Bisquert,et al.  Mechanism of carrier accumulation in perovskite thin-absorber solar cells , 2013, Nature Communications.

[14]  Yongcai Qiu,et al.  A quasi-quantum well sensitized solar cell with accelerated charge separation and collection. , 2013, Journal of the American Chemical Society.

[15]  P. Reiss,et al.  Ternary and quaternary metal chalcogenide nanocrystals: synthesis, properties and applications , 2013 .

[16]  Ke Zhao,et al.  Near infrared absorption of CdSe(x)Te(1-x) alloyed quantum dot sensitized solar cells with more than 6% efficiency and high stability. , 2013, ACS nano.

[17]  Yanhong Luo,et al.  Highly efficient core-shell CuInS2-Mn doped CdS quantum dot sensitized solar cells. , 2013, Chemical communications.

[18]  O. Voznyy,et al.  Graded Doping for Enhanced Colloidal Quantum Dot Photovoltaics , 2013, Advanced materials.

[19]  P. Kamat.  Quantum Dot Solar Cells. The Next Big Thing in Photovoltaics. , 2013, The journal of physical chemistry letters.

[20]  Thomas E Mallouk,et al.  Design and development of photoanodes for water-splitting dye-sensitized photoelectrochemical cells. , 2013, Chemical Society reviews.

[21]  Pralay K. Santra,et al.  CuInS2-Sensitized Quantum Dot Solar Cell. Electrophoretic Deposition, Excited-State Dynamics, and Photovoltaic Performance. , 2013, The journal of physical chemistry letters.

[22]  H. Teng,et al.  Photoactive p-type PbS as a counter electrode for quantum dot-sensitized solar cells , 2013 .

[23]  N. Fuke,et al.  Engineered CuInSexS2-x Quantum Dots for Sensitized Solar Cells. , 2013, The journal of physical chemistry letters.

[24]  H. Zhang,et al.  Efficient CdSe quantum dot-sensitized solar cells prepared by a postsynthesis assembly approach. , 2012, Chemical communications.

[25]  Catherine J Murphy,et al.  Applications of colloidal inorganic nanoparticles: from medicine to energy. , 2012, Journal of the American Chemical Society.

[26]  Aram Amassian,et al.  Hybrid passivated colloidal quantum dot solids. , 2012, Nature nanotechnology.

[27]  Zhan'ao Tan,et al.  Highly Emissive and Color‐Tunable CuInS2‐Based Colloidal Semiconductor Nanocrystals: Off‐Stoichiometry Effects and Improved Electroluminescence Performance , 2012 .

[28]  S. Evans,et al.  Determining the Concentration of CuInS2 Quantum Dots from the Size-Dependent Molar Extinction Coefficient , 2012 .

[29]  J. Hua,et al.  Highly efficient inverted type-I CdS/CdSe core/shell structure QD-sensitized solar cells. , 2012, ACS nano.

[30]  Jia-Yaw Chang,et al.  Efficient "green" quantum dot-sensitized solar cells based on Cu2S-CuInS2-ZnSe architecture. , 2012, Chemical communications.

[31]  P. Kamat.  Boosting the efficiency of quantum dot sensitized solar cells through modulation of interfacial charge transfer. , 2012, Accounts of Chemical Research.

[32]  S. Paria,et al.  Core/shell nanoparticles: classes, properties, synthesis mechanisms, characterization, and applications. , 2012, Chemical reviews.

[33]  S. Hayase,et al.  Multiple electron injection dynamics in linearly-linked two dye co-sensitized nanocrystalline metal oxide electrodes for dye-sensitized solar cells. , 2012, Physical chemistry chemical physics : PCCP.

[34]  Guoping Xu,et al.  Effect of ZnS and CdS coating on the photovoltaic properties of CuInS2-sensitized photoelectrodes , 2012 .

[35]  H. Teng,et al.  High-performance quantum dot-sensitized solar cells based on sensitization with CuInS2 quantum dots/CdS heterostructure , 2012 .

[36]  J. Luther,et al.  Peak External Photocurrent Quantum Efficiency Exceeding 100% via MEG in a Quantum Dot Solar Cell , 2011, Science.

[37]  Xiaoming Huang,et al.  Aqueous colloidal CuInS2 for quantum dot sensitized solar cells , 2011 .

[38]  M. Grätzel,et al.  Toward interaction of sensitizer and functional moieties in hole-transporting materials for efficient semiconductor-sensitized solar cells. , 2011, Nano letters.

[39]  Aram Amassian,et al.  Colloidal-quantum-dot photovoltaics using atomic-ligand passivation. , 2011, Nature materials.

[40]  Prathik Roy,et al.  Quantum dot-sensitized solar cells incorporating nanomaterials. , 2011, Chemical communications.

[41]  Q. Shen,et al.  Uncovering the role of the ZnS treatment in the performance of quantum dot sensitized solar cells. , 2011, Physical chemistry chemical physics : PCCP.

[42]  F. Fabregat‐Santiago,et al.  Characterization of nanostructured hybrid and organic solar cells by impedance spectroscopy. , 2011, Physical chemistry chemical physics : PCCP.

[43]  X. Zhong,et al.  Facile synthesis of ZnS-CuInS2-alloyed nanocrystals for a color-tunable fluorchrome and photocatalyst. , 2011, Inorganic chemistry.

[44]  H. Teng,et al.  CuInS2 quantum dots coated with CdS as high-performance sensitizers for TiO2 electrodes in photoelectrochemical cells , 2011 .

[45]  Jaehyun Park,et al.  CuInS2/ZnS core/shell quantum dots by cation exchange and their blue-shifted photoluminescence , 2011 .

[46]  V. Klimov,et al.  Efficient synthesis of highly luminescent copper indium sulfide-based core/shell nanocrystals with surprisingly long-lived emission. , 2011, Journal of the American Chemical Society.

[47]  Q. Shen,et al.  Sensitization of Titanium Dioxide Photoanodes with Cadmium Selenide Quantum Dots Prepared by SILAR: Photoelectrochemical and Carrier Dynamics Studies , 2010 .

[48]  Prashant V Kamat,et al.  Beyond photovoltaics: semiconductor nanoarchitectures for liquid-junction solar cells. , 2010, Chemical reviews.

[49]  J. Luther,et al.  Semiconductor quantum dots and quantum dot arrays and applications of multiple exciton generation to third-generation photovoltaic solar cells. , 2010, Chemical reviews.

[50]  Juan Bisquert,et al.  Breakthroughs in the Development of Semiconductor-Sensitized Solar Cells , 2010 .

[51]  B. Parkinson,et al.  Multiple Exciton Collection in a Sensitized Photovoltaic System , 2010, Science.

[52]  J. Bisquert,et al.  Modeling high-efficiency quantum dot sensitized solar cells. , 2010, ACS nano.

[53]  T. Mirkovic,et al.  Noninjection gram-scale synthesis of monodisperse pyramidal CuInS2 nanocrystals and their size-dependent properties. , 2010, ACS nano.

[54]  Arie Zaban,et al.  Quantum-dot-sensitized solar cells. , 2010, Chemphyschem : a European journal of chemical physics and physical chemistry.

[55]  J. Bisquert,et al.  Design of injection and recombination in quantum dot sensitized solar cells. , 2010, Journal of the American Chemical Society.

[56]  Xuhong Guo,et al.  Bifunctional multidentate ligand modified highly stable water-soluble quantum dots. , 2010, Inorganic chemistry.

[57]  Justin B. Sambur,et al.  CdSe/ZnS core/shell quantum dot sensitization of low index TiO(2) single crystal surfaces. , 2010, Journal of the American Chemical Society.

[58]  F. Fabregat‐Santiago,et al.  Recombination in quantum dot sensitized solar cells. , 2009, Accounts of chemical research.

[59]  Xiaogang Peng,et al.  Formation of high-quality I-III-VI semiconductor nanocrystals by tuning relative reactivity of cationic precursors. , 2009, Journal of the American Chemical Society.

[60]  Prashant V. Kamat,et al.  Quantum Dot Solar Cells. Semiconductor Nanocrystals as Light Harvesters , 2008 .

[61]  Gary Hodes,et al.  Comparison of Dye-and Semiconductor-Sensitized Porous Nanocrystalline Liquid Junction Solar Cells , 2008 .

[62]  Yuliang Zhang,et al.  A facile route to violet- to orange-emitting CdxZn1−xSe alloy nanocrystals via cation exchange reaction , 2007 .

[63]  Q. Shen,et al.  High efficiency of CdSe quantum-dot-sensitized TiO2 inverse opal solar cells , 2007 .

[64]  Yadong Yin,et al.  Cation Exchange Reactions in Ionic Nanocrystals , 2004, Science.

[65]  B. Parkinson,et al.  The Adsorption Behavior of a Ruthenium‐Based Sensitizing Dye to Nanocrystalline TiO2 Coverage Effects on the External and Internal Sensitization Quantum Yields , 1999 .

[66]  M. Bawendi,et al.  (CdSe)ZnS Core-Shell Quantum Dots - Synthesis and Characterization of a Size Series of Highly Luminescent Nanocrystallites , 1997 .

[67]  A. Alivisatos.  Semiconductor Clusters, Nanocrystals, and Quantum Dots , 1996, Science.