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  • Retraction for Journal of Materials Chemistry A:

    In-situ formed ternary-based hybrid ink for the fabrication of Cu2ZnSn(S,Se)4 solar cell

    absorbers

    Kai Zong, Yuxiu Sun, Yongzheng Zhang, Hao Wang, Jingbing Liu and Hui Yan

    J. Mater. Chem. A, 2013, Accepted Manuscript (DOI: 10.1039/C3TA13157B). Retraction published

    2 nd

    December 2013.

    We, the named authors, hereby wholly retract this Journal of Materials Chemistry A article due to

    data fabrication in Figures 3 and 6. The Raman spectra reported as a CZTSe film in Figure 3b is

    identical to the Raman spectra reported as CZTSe nanocrystals in Figure 4 of “The synthesis of

    Cu2Zn(GexSn1-x)Se4 nanocrystals with tunable band gaps”, CrystEngComm, 2013, 15, 6942 [DOI:

    10.1039/c3ce40953h]. The UV-vis absorption spectra curves in Figure 6b of films of varying S/Se

    content are the same curve that has been copied, shifted and pasted within the figure: the purple curve

    is the copy of the blue curve. An investigation by Dr Yongping Lei (Professor and Chairman of

    College Council of the College of Materials Science and Engineering, Beijing University of

    Technology, China) determined that Kai Zong was responsible for these instances of data fabrication.

    Hao Wang, as his tutor and also corresponding author, is responsible for the duty of supervision and

    management. Other co-authors accept joint responsibility for the preparation of article. Please allow

    us to sincerely apologise to all readers and the Editorial Office.

    Signed: Kai Zong, Yuxiu Sun, Yongzheng Zhang, Hao Wang, Jingbing Liu and Hui Yan, November

    2013.

    Retraction endorsed by Liz Dunn, Managing Editor, Journal of Materials Chemistry A.

    Electronic Supplementary Material (ESI) for Journal of Materials Chemistry A This journal is © The Royal Society of Chemistry 2013

  • Registered Charity Number 207890

    Accepted Manuscript

    This is an Accepted Manuscript, which has been through the RSC Publishing peer review process and has been accepted for publication.

    Accepted Manuscripts are published online shortly after acceptance, which is prior to technical editing, formatting and proof reading. This free service from RSC Publishing allows authors to make their results available to the community, in citable form, before publication of the edited article. This Accepted Manuscript will be replaced by the edited and formatted Advance Article as soon as this is available.

    To cite this manuscript please use its permanent Digital Object Identifier (DOI®), which is identical for all formats of publication.

    More information about Accepted Manuscripts can be found in the Information for Authors.

    Please note that technical editing may introduce minor changes to the text and/or graphics contained in the manuscript submitted by the author(s) which may alter content, and that the standard Terms & Conditions and the ethical guidelines that apply to the journal are still applicable. In no event shall the RSC be held responsible for any errors or omissions in these Accepted Manuscript manuscripts or any consequences arising from the use of any information contained in them.

    www.rsc.org/materialsA

    0959-9428(2010)20:1;1-A

    ISSN 2050-7488

    Materials for energy and sustainability

    Journal of Materials Chemistry A www.rsc.org/MaterialsA Volume 1 | Number 1 | January 2013 | Pages 0000–0000

    Journal of Materials Chemistry A

    Electronic Supplementary Material (ESI) for Journal of Materials Chemistry A This journal is © The Royal Society of Chemistry 2013

  • 1

    In-situ Formed Ternary-based Hybrid Ink for the

    Fabrication of Cu2ZnSn(S,Se)4 Solar Cell Absorbers

    Kai Zong a , Yuxiu Sun *

    a,b , Yongzheng Zhang

    a,c , Hao Wang *

    a,c , Jingbing Liu

    a ,

    Hui Yan a,c

    a The College of Materials Science and Engineering, Beijing University of

    Technology, Beijing, 100124, P.R. China

    b Tianjin Key Laboratory of Structure and Performance for Functional Molecule,

    College of Chemistry, Tianjin Normal University, Tianjin, 300387, P.R. China

    c Chengdu Green Energy and Green Manufacturing Technology R&D Centre,

    Shuangliu, Chengdu 610207, P.R.China

    ABSTRACT Cu2ZnSn(S,Se)4 (CZTSSe) is a promising material for use as the low

    cost absorber for thin film solar cells, because it is only composed of abundant and

    economical elements. Herein we outline an alternative strategy to fabricate kesterite

    CZTSSe absorbers from an easily scalable hybrid ink based on propylmercaptan (PM)

    solution. The ink comprises a Zn-PM solution, with the in-situ formed readily

    dispersible particle-based Cu2SnS3 ternary precursor. The pre-formed Cu2SnS3

    precursor would simplify the reaction pathway for the synthesis of CZTSSe thin

    films, and reduce the formation of detrimental secondary phases. CZTSSe solar cells

    fabricated by this approach exhibit an average power conversion efficiency up to 7.4

    %.

    KEYWORDS: Cu2ZnSn(S,Se)4, ink, solar cells, thin films

    Page 1 of 19 Journal of Materials Chemistry A

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    Electronic Supplementary Material (ESI) for Journal of Materials Chemistry A This journal is © The Royal Society of Chemistry 2013

  • 2

    Corresponding Author: The College of Materials Science and Engineering, Beijing

    University of Technology, Beijing 100124, P.R. China. E-mail:

    haowang@bjut.edu.cn; Tel: +86-10-6739-2733

    Introduction

    Exploring a safe and scalable route to fabricate low-cost and high-efficiency

    photovoltaics is one of the most active research fields in the area of solar cells.

    Kesterite, copper zinc tin sulfide selenide (Cu2ZnSn(S,Se)4 or CZTSSe), is considered

    as a potential substitute to traditional Copper-based quaternary semiconductors,

    Cu(In,Ga)(S,Se)2 (CIGSe), due to its direct band gap energy (1.0-1.5 eV), relatively

    low toxicity, high optical absorption coefficient in the visible range (>104 cm−1), and

    earth abundant content of elements. 1-3 To date, Guha et al. reported the fabrication of

    CZTSSe thin film solar cells with 8.4 % power conversion efficiency (PCE) using a

    vacuum-based approach. 4 However, such process typically suffers from relatively

    high cost, low material utilization, difficulty in composition control and difficulties

    associated with large-scale production.5

    Recently, thin film processes using solution-based inks have attracted intense

    attentions, because the precursor film can be deposited on the substrate via a variety

    of facile techniques, such as dip-coating, slip casting, and screen printing etc., thereby

    enabling the development of low-cost, high-throughput roll-to-roll processes. 6, 7 Guo

    et al. 8 demonstrated the fabrication of CZTSSe solar cells with 7.2 % power

    conversion efficiency using copper zinc tin sulfide (CZTS) nanocrystal inks

    synthesized by hot injection method with the subsequent selenization. However, the

    quaternary nanocrystal-based synthetic routes do not offer a simple method by which

    the final film composition can be controlled. Furthermore, the synthesis of

    nanocrystals by this additional step with controlled size is not compatible with the

    large-scale production. 8-10 Mitzi et al. demonstrated the fabrication of CZTSSe thin

    film solar cells with higher efficiency over 9.6 %, which is further improved up to

    11.1 % by spin-casting precursor inks based on a hybrid solution-particle

    Page 2 of 19Journal of Materials Chemistry A

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    Electronic Supplementary Material (ESI) for Journal of Materials Chemistry A This journal is © The Royal Society of Chemistry 2013

  • 3

    hydrazine-based inks.11-13 However, the corrosivity, explosibility, and toxicity of

    hydrazine limit its further investigation and large-scale application in industry. 14, 15

    Furthermore, all processing for precursor solution and film preparations must be

    performed in the closed environment, such as glove box, due to the corrosivity nature

    of this solvent, and thus hydrazine would not be easily adaptable for large-scale solar

    cell fabrication. Therefore, a facile and easily scalable solution-based process for the

    fabrication of high quality CZTSSe absorber layers is still highly demanded.

    In this work, we demonstrate a facile strategy to process CZTSSe absorbers, which

    features the preparation of hybrid ink using propylmercaptan (PM) solution. The

    hybrid ink employed for deposition comprises a Zn-PM solution, with the in-situ

    formed readily dispersible particle-based Cu2SnS3 ternary precursors. The concept is

    similar to that of the hybrid hydrazine-based ink adopted by Mitzi et al, 11-13 however,

    which is composed of Cu–Sn chalcogenide (S or S–Se) solution and particle-based

    Zn-chalcogenide precursors, ZnSe(N2H4) or ZnS(N2H4). In th

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