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Frontiers of Optoelectronics

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Front. Optoelectron.    2015, Vol. 8 Issue (3) : 252-268    https://doi.org/10.1007/s12200-015-0539-2
REVIEW ARTICLE
Cu2ZnSn(S,Se)4 thin film solar cells fabricated with benign solvents
Cheng ZHANG1,2,Jie ZHONG1,2,*(),Jiang TANG2,*()
1. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
2. Wuhan National Laboratory for Optoelectronics, Huazhong Univesity of Science and Technology, Wuhan 430074, China
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Abstract

Cu2ZnSn(S,Se)4 (CZTSSe) is considered as the promising absorbing layer materials for solar cells due to its earth-abundant constituents and excellent semiconductor properties. Through solution-processing, such as various printing methods, the fabrication of high performance CZTSSe solar cell could be applied to mass production with extremely low manufacturing cost and high yield speed. To better fulfill this goal, environmental-friendly inks/solutions are optimum for further reducing the capital investment on instrument, personnel and environmental safety. In this review, we summarized the recent development of CZTSSe thin films solar cells fabricated with benign solvents, such as water and ethanol. The disperse system can be classified to the true solution (consisting of molecules) and the colloidal suspension (consisting of nanoparticles).Three strategies for stabilization (i.e., physical method, chemical capping and self-stabilization) are proposed to prepare homogeneous and stable colloidal nanoinks. The one-pot self-stabilization method stands as an optimum route for preparing benign inks for its low impurity involvement and simple procedure. As-prepared CZTSSe inks would be deposited onto substrates to form thin films through spin-coating, spraying, electrodeposition or successive ionic layer adsorption and reaction (SILAR) method, followed by annealing in a chalcogen (S- or Se-containing) atmosphere to fabricate absorber. The efficiency of CZTSSe solar cell fabricated with benign solvents can also be enhanced by constituent adjustments, doping, surface treatments and blocking layers modifications, etc., and the deeper research will promise it a comparable performance to the non-benign CZTSSe systems.
Keywords Cu2ZnSn(S      Se)4 (CZTSSe)      solar cell      benign solvents      metal chalcogenide complexes (MCCs)      solution processing     
Corresponding Author(s): Jie ZHONG,Jiang TANG   
Just Accepted Date: 17 August 2015   Online First Date: 08 September 2015    Issue Date: 18 September 2015
 Cite this article:   
Cheng ZHANG,Jie ZHONG,Jiang TANG. Cu2ZnSn(S,Se)4 thin film solar cells fabricated with benign solvents[J]. Front. Optoelectron., 2015, 8(3): 252-268.
 URL:  
https://academic.hep.com.cn/foe/EN/10.1007/s12200-015-0539-2
https://academic.hep.com.cn/foe/EN/Y2015/V8/I3/252
Fig.1  Main processing steps of CZTS thin film synthesis using benign solvents
metal source sulfur source solvent additive reference
metal chlorides thiourea water – [5]
metal chlorides thiourea water HCl [6,7]
metal chlorides thiourea water-ethanol (30 vol% ethanol) – [8–10]
metal oxides ammonium thioglycolate water – [11]
metal chlorides, zinc acetate thiourea water – [12]
Tab.1  Constituents of solutions in papers
factor
influence additive [26] sulfur source [28] reaction duration [24] reaction temperature [24]
what phase phase purity purity
how ethylenediamine (EN) increases orthorhombic CZTS different sulfur sources produce different phases longer time promotes the formation of pure CZTS higher purity at higher reaction temperature
why EN reduces the surface energy of CZTS crystals reaction rate of Zn2+ and sulfur sources determines CZTS crystal structure complete the reaction higher temperature provides more energy
Tab.2  Factors influencing products of hydrothermally prepared CZTS NCs
Fig.2  TEM images of CZTS NCs prepared by hydrothermal process: (a) low resolution TEM image; (b) high resolution TEM image; (c) SAED pattern; and (d) picture of well-dispersed CZTS/ethanol ‘ink’ [22]
Fig.3  Schematic diagram of the preparation of CZTS solution using metal sulfides with cetyltrimethyl ammonium bromide (CTAB) as the capping ligand. A typical illustration of carbon-chained ligands capping on the NCs [17]
Fig.4  Schematic diagram of the self-stabilized ink [13]
Fig.5  CZTS nanoinks preparation and characterization. (a) Photos of CZTS nanoinks processed by one-pot mixing of aqueous Sn-MCC and Cu/Zn sources; (b) Raman spectrum of aqueous Sn-MCC solution; (c) FTIR spectra of CZTS inks vacuum-dried (dried ink) and the precipitation from centrifugation (centri-powder); (d) TEM morphology of the dispersed NCs with the SAD pattern; (e) high-resolution TEM image of a few NCs with measured lattice distance of 0.31nm corresponding to the (111) lattice distance of Cu/ZnS; (f) EDS analysis of as-made CZTS NCs. A Mo grid with carbon support film was used to manifest that the Cu signal is from NCs; (g) DLS characterization of the CZTS nanoink; (h) Zeta-potential curve of aqueous nanoink associated with MCC capping [13]
Fig.6  Dark-field STEM image and corresponding EDX-STEM mapping for Cu, Zn, and Sn elements in a slice of a Mo/CZTS (Se)/CdS/ZnO/ITO device (Cu: red, Zn: blue, Sn: green) with a CZTS (Se) film made by non-pyrolytic spray [15,16]
Fig.7  Schematic diagram of SILAR technique for the deposition of CZTS: beaker 1 contains cationic precursors, beaker 3 contains anionic precursor and beakers 2 and 4 contain double distilled water (DDW) [48]
techniques time-consuming simplicity large-scale production solution/ suspension quality of film highest efficiency
spincoating [11] no yes no both general 6.62%
spray [16] no yes yes both general 8.60%
electrodeposition [41] no no yes solution good 3.40%
SILAR [46] yes yes yes solution general 1.85%
Tab.3  Comparison of different deposition techniques with highest efficiencies
components solution/ suspension deposition technique temperature/°C time/min atmosphere reaction
Cu2S+ metal elements [14] suspension spin-coating 400-530 30 N2 + H2S (5%) liquid phase sintering
metal sulfides [52] solution SILAR 200-500 120 N2 + S solid state reaction
metal oxides [18] suspension doctor-blading 250-600 30 S sulfuration
metastable CZTS [28] suspension doctor-blading 550-600 30 S phase transformation (to kesterite)
kesterite CZTS [25] suspension spin-coating 450 60 N2 growth
metal sulfides [13] suspension spin-coating 540-600 10-15 N2 + Se solid state reaction
Tab.4  Comparison of annealing conditions for CZTS film deposited using different techniques
Fig.8  XRD patterns of CZTS thin films as a function of annealing temperatures [8]
Fig.9  Characterization of CZTSSe film. (a) Raman curves of the CZTSSe film produced by annealing the CZTS film in an atmosphere containing different amounts of Se and S, indicating a fully tunable composition and consequently a band gap; (b) XRD pattern of the CZTSSe absorber film. Peaks indexed to Mo and MoSe2 (from substrate) as well as the standard diffraction patterns for CZTS (JSPDS 26-0575) and CZTSe (JSPDS 52-0868) are included for reference; (c) cross-sectional and (d) top-view SEM images of the CZTSSe absorber film [13]
Fig.10  (a) J-V curve and (b) EQE spectrum of the CZTSSe device fabricated from aqueous CZTS nanoink [13]
samples Cu/(Zn+ Sn) Zn/Sn
As-deposited (from stoichiometry solution) 0.96 0.79
annealing with S (550°C) (from stoichiometry solution) 1.01 0.98
annealing with S (550°C) + KCN (from stoichiometry solution) 0.58 0.90
annealing with S+ Sn (550°C) (from stoichiometry solution) 0.99 0.92
annealing with S+ Sn (550°C) + KCN (from stoichiometry solution) 0.52 0.94
As-deposited (from nonstoichiometry solution) (-20% Cu and+20% Zn) 1.00 1.13
annealing with S+ Sn (550°C) (from nonstoichiometry solution) (-20% Cu and+20% Zn) 0.80 1.37
Tab.5  Compositional ratios of the precursor elements for as-deposited, annealed, and annealed and chemically treated samples. The as-deposited samples were deposited from stoichiometry and nonstoichiometry solutions [7]
Fig.11  (a) SEM image of typical solar cell based on CZTS:Na nanocrystals. Electrical characterization of the CZTS:Na- and CZTS- based devices; (b) current-voltage (J -V) characteristics under air mass 1.5 illumination, 100 mW/cm2; (c) EQE spectrum of the device without any applied bias; (d) TRPL of the device under low injection; (e) capacitance-voltage measurement, with the measurement frequency of 11 kHz, the DC bias ranging from 0 to - 0.5 V, and the temperature at 300 K [68]
Fig.12  Electronic characterization for CZTSSe devices S2 and S3. Admittance spectroscopy (AS) of S2 (a) and S3 (b) with temperature range of 180 to 300 K; (c) the trap conductance spectra (Gm-Gd)/w; and equivalent circuit model; (d) Arrhenius plots of S3 and S2 derived from AS patterns. The estimated energetic depths of the defect (Ea) for S3 and S2 are 101 and 156 meV, respectively [71]
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