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二价阳离子掺杂措施优化铜锌锡硫(硒)薄膜太阳能电池性能的研究进展

赵鑫,  杨艳春,  崔国楠,  刘艳青,  任俊婷,  田晓,  朱成军

文章导航 > 复合材料学报  > 2023 > 优先出版
赵鑫, 杨艳春, 崔国楠, 等. 二价阳离子掺杂措施优化铜锌锡硫(硒)薄膜太阳能电池性能的研究进展[J]. 复合材料学报, 2023, 41(0): 1-14
引用本文: 赵鑫, 杨艳春, 崔国楠, 等. 二价阳离子掺杂措施优化铜锌锡硫(硒)薄膜太阳能电池性能的研究进展[J]. 复合材料学报, 2023, 41(0): 1-14
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Xin ZHAO, Yanchun YANG, Guonan CUI, Yanqing LIU, Junting REN, Xiao TIAN, Chengjun ZHU. Research progress on optimizing performance of Cu2ZnSnS4(Cu2ZnSn(S,Se)4) thin-film solar cells by bivalent cations doping[J]. Acta Materiae Compositae Sinica.
Citation: Xin ZHAO, Yanchun YANG, Guonan CUI, Yanqing LIU, Junting REN, Xiao TIAN, Chengjun ZHU. Research progress on optimizing performance of Cu2ZnSnS4(Cu2ZnSn(S,Se)4) thin-film solar cells by bivalent cations doping[J]. Acta Materiae Compositae Sinica.
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二价阳离子掺杂措施优化铜锌锡硫(硒)薄膜太阳能电池性能的研究进展

  • 1.

    内蒙古师范大学　物理与电子信息学院, 呼和浩特 010022

  • 2.

    内蒙古大学　物理科学与技术学院, 呼和浩特010021

基金项目: 国家自然科学基金(62164010，62064010);中央引导地方科技发展资金(2020ZY0009); 中国博士后科学基金(2019M653806XB); 内蒙古师范大学校级研究生科研创新基金发展资金(CXJJS22105)
详细信息
    通讯作者:

    杨艳春，博士，副教授，硕士生导师，研究方向为光伏材料制备及性能研究工作，包括铜锌锡硫硒、有机-无机钙钛矿材料的光伏性能、发光性能的研究　E-mail: 20170020@imnu.edu.cn

    朱成军，博士，教授，博士生导师，研究方向为新能源材料与器件：薄膜太阳能电池材料与器件、低温固体氧化物燃料电池材料与器件　E-mail: ndcjzhu@126.com

  • 中图分类号: TM914.4+2

Research progress on optimizing performance of Cu2ZnSnS4(Cu2ZnSn(S,Se)4) thin-film solar cells by bivalent cations doping

  • 1.

    School of Physics and Electronic Information, Inner Mongolia Normal University, Hohhot 010022, China

  • 2.

    School of Physics Science and Technology, Inner Mongolia University, Hohhot 010021, China

Funds: This work was financially supported by the Natural Science Foundation of China (62164010, 62064010); The central government guides local funds for science and technology development(2020ZY0009); China Postdoctoral Science Foundation(2019M653806XB); Inner Mongolia Normal University graduate research and Innovation Fund development fund (CXJJS22105)

    摘要
  • 摘要:   背景  太阳能电池作为开发和利用清洁能源的技术之一，顺应当今社会可持续发展的理念，成为一个十分热门的研究方向，也产生很多分支。其中铜锌锡硫硒(CuZnSn(S,Se)，简称CZTSSe)薄膜太阳能电池因其无毒和低成本的优势，越来越受研究者们的青睐。而CZTSSe所面临的开路电压低、缺陷密度大、带尾态严重等问题则限制了其电池器件的效率，所以解决开路电压亏损等问题就成为提高电池光电转化效率的重中之重。经过多年的研究探索，阳离子掺杂措施被认为是缓解这些问题的一种有效方法，其中一价和四价的金属阳离子可选择性相对较少，因此，本论文详细介绍了二价阳离子掺杂在优化铜锌锡硫(硒)(CZTS(Se))薄膜太阳能电池性能方面的研究进展。  方法  本论文通过文献调研法、归纳法和对比分析法从二价阳离子取代和额外添加两个方面详细介绍了二价阳离子掺杂措施在优化CZTS(Se)薄膜太阳能电池性能方面的研究进展。主要内容：本文以掺杂的二价阳离子是否进入CZTSSe内部占据晶格位点为标准，将掺杂的二价阳离子进入CZTS(Se)晶格内并占据Zn格位点和未进入晶格内分类为：二价阳离子的取代和二价阳离子的额外添加。根据目前的研究进展，二价阳离子掺杂措施在优化此类电池性能方面的主要作用有：(1)改善吸收层的结晶性，减少Cu-Zn反位缺陷，改善带尾态效应，例如Mg、Ba、Ca，但是此类元素掺杂量的最佳范围较窄，一旦超过这个最佳范围会造成吸收层晶格膨胀，或产生杂相；(2)调节吸收层和缓冲层的能带偏移，例如Cd、Ni、Co、Mn。其中，Cd的掺杂的效果最为明显，可以使CZTS器件效率达到12%以上，但是Cd元素的毒性却是限制其发展的重要因素。除此之外，Cr取代Zn，则是在吸收层中间插入一个中间带，扩大光子的跃迁路径，增强光子的吸收，有助于电池器件性能的提高，但其未实施在优化电池器件性能上，所以，未来可以进行更深入的探索，争取应用在优化电池器件性能上；Co和Mn元素不仅可以与Zn发生取代，还可以通过额外添加的方式，促进晶粒的生长，改善薄膜电学性能，但该类措施也没有应用在优化电池器件性能上，却为以后的电池器件性能优化提供新的途径。  结论  本文从二价阳离子的取代和额外添加两个部分分别介绍了二价阳离子掺杂措施在优化CZTS(Se)薄膜太阳能电池性能的研究进展。二价阳离子取代措施，如：Cd取代Zn等，主要是可以有效降低CZTS(Se)薄膜太阳能电池吸收层的缺陷密度，提高结晶质量，解决吸收层和缓冲层之间界面能带偏移值较大的问题，从而减少电池器件的开路电压亏损，提高器件效率；二价阳离子的额外添加，如：Co、Mn的额外添加，主要是优化薄膜的结晶性、帮助载流子的输运，提高吸收层薄膜的电学性能。最后，也总结两类阳离子掺杂措施的优缺点以及应用前景。

     

    Abstract: Cations doping measures are considered as one of the effective measures to optimize the performance of Cu2ZnSn(S,Se)4 (CZTSSe) thin film solar cells, and divalent cations doping measures are the most studied and widely applied in all cations doping measures. Here, the research progress of divalent cation measures in optimizing the performance of CZTS(Se) thin film solar cells is introduced from two aspects: cations substitution and extra cations addition. Divalent cations substitution measures, such as, substitution of Zn2+ with Cd2+, mainly reduce the defect density of the absorber layer of CZTS(Se) thin film solar cells, improve the crystalline quality, and solve the problem of large interface energy band offset between the absorber layer and buffer layer, which reduce the open voltage circuit loss of the device and improving its efficiency; the extra addition of divalent cations, such as, the extra addition of Co2+/Mn2+, optimize the crystallinity of the film, help the carrier transport, and improve the electrical properties of the absorber layer; finally, their advantages, disadvantages, and the application prospects are also summarized.

     

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  • 图  1  二价阳离子掺杂措施总结示意图

    Figure  1.  Summary diagram of divalent cationic doping measures

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    图  2  CZTS和CZMTS吸收层XRD图(a)和Raman图(b). 插图为(112)衍射峰放大图[49]

    Figure  2.  X-ray diffraction patterns (a) and Raman scattering spectra (b) of CZTS and CZMTS absorber．The inset is the enlarged view of the (112) diffraction peak[49]

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    图  3  CZTS和CZMTS吸收层横截面FESEM图像[49]

    Figure  3.  FESEM cross-sectional images of the CZTS and CZMTS absorber[49]

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    图  4  Cu2Zn1-xBaxSn(S,Se)4薄膜表面SEM图像[52]

    Figure  4.  Surface SEM images of the Cu2Zn1-xBaxSn(S,Se)4 thin films[52]

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    图  5  CBTSe中本征缺陷在化学势点处的形成焓与费米能级的关系：(a) Cu-poor and Se-intermediate; (b) Cu-rich and Se-poor; (c) (Cu-poor and Se-rich)[53]

    Figure  5.  Calculated formation enthalpies of intrinsic defects in CBTSe as a function of Fermi level (EF) at the chemical potential points (a) (Cu-poor and Se-intermediate), (b) (Cu-rich and Se-poor), and (c) (Cu-poor and Se-rich)[53]

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    图  6  器件参数(PCE,VOC, JSC and FF)与微量Ca掺杂Cu2CaxZn1-xSn(S,Se)4即：Ca/(Ca+Zn)%的关系[55]

    Figure  6.  Relationship of the detail device parameters (PCE, VOC, JSC and FF) with trace Ca-doped Cu2CaxZn1-xSn(S,Se)4 i.e. Ca/(Ca+Zn)%devices[55]

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    图  7  在不同μCu下Cu2ZnSnS4在(μZn, μSn)面的稳定化学势区域(黑色区域)和在(μCu，μZn，μSn)化学势[28]

    Figure  7.  The calculated stable chemical potential region (black area) of Cu2ZnSnS4 in (μZn,μSn) planes with different μCu in the (μCu, μZn, μSn) chemical potential spaces[28]

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    图  8  根据PL和HR-XPS 研究，CZNTS中带隙, VBO, CBO随Ni浓度变化图[63]

    Figure  8.  Plot of variation of band gaps, VBO and CBO versus Ni composition in CZNTS, according to PL and HR-XPS investigations[63]

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    图  9  Cu2NixZn1-xSn(S,Se)4(0≤x≤0.1)薄膜SEM图像[61]

    Figure  9.  SEM images of the Cu2NixZn1-xSn(S,Se)4 (0≤x≤0.1)films with the various x values[61]

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    图  10  CZTS和Cu2(Zn0.96Cr0.04)SnS4薄膜能带图及价带(Ev)中间带(Ei)费米能级(EF)和导带(Ec)相对于真空能级(Evac)的位置[65]

    Figure  10.  Calculated band diagram of CZTS and Cu2(Zn0.96Cr0.04)SnS4 films and position of valence band (Ev), intermediate band states (Ei), fermi level (EF) and conduction band (Ec) with respect to vacuum level (Evac)[65]

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    图  11  以Cu2Zn1-xCrxSnS4为吸收层的电池性能参数随x变化的函数[65]

    Figure  11.  Output parameters of the cells with Cu2Zn1-xCrxSnS4 absorber layers as the functions of x[65]

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    图  12  Cu2MnxZn1-xSn(S,Se)4薄膜表面和截面SEM图[71]

    Figure  12.  Surface and cross-sectional SEM images of Cu2MnxZn1-xSn(S,Se)4 thin films[71]

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    图  13  (a)不同Co掺杂比(0, 1, 3, 5 mol%) CZTSSe XRD图. (b) (112)衍射峰的放大图[82]

    Figure  13.  (a) XRD patterns of CZTSSe samples with different trace Co incorporation ratio (0, 1, 3, and 5 mol%)． (b) The enlarged view of (112) peaks[82]

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    图  14  不同Mn掺杂比CZTSSe薄膜的AFM形貌和c-AFM表面电流图像:a-b:0; c-d:1 mol%; e-f:3 mol%;g-h:5 mol%; i-j:7 mol%[83]

    Figure  14.  AFM topography and c-AFM surface current images of CZTSSe thin films with the different Mn-doping ratios: a-b:0; c-d:1 mol%; e-f:3 mol%; g-h:5 mol%; i-j:7 mol%[83]

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    表  1  不同二价阳离子掺杂措施所取得的最高铜锌锡硫硒薄膜(CZTS(Se))薄膜太阳能电池参数

    Table  1.   The paramaters of the hightest Cu2ZnSn(S,Se)4 CZTS(Se) thin-film solar cell by different divalent cation doping measures

    Battery device nameVOC/mVJSC/mA·cm−2FF/%η/%Ref
    Cu2Mg0.0357Zn0.9643Sn(S,Se)4400.1533.4557.937.76[50]
    Cu2Ba0.01Zn0.9Sn(S,Se)442432.366.89.14[52]
    Cu2Ca0.02Zn0.8Sn(S,Se)441735.84588.73[54]
    Cu2Zn0.6Cd0.4SnS464027.87112.6[18]
    Cu2Ni0.05Zn0.95Sn(S,Se)435133.6245.055.32[60]
    Cu2Zn0.96Cr0.04SnS45681449.83.96[64]
    Cu2Mn0.05Zn0.95Sn(S,Se)441833.763.38.9[70]
    Cu2Co0.03Zn0.97Sn(S,Se)434026.8543.33.95[71]
    Notes：VOC: open circuit voltage; JSC: short-circuit current density; FF: fill factor; η: light-to-electricity conversion efficiency
    下载: 导出CSV

    表  2  CZTS和CZCTS 样品的电性能[58]

    Table  2.   Electrical characteristics of the CZTS and CZCTS samples[58]

    absorberOptical Eg/eVPL Peak/eVΔ(Eg- PL Peak)/mVEUrbach/meV
    CZTS1.541.37~17065
    CZCTS1.381.31~7045
    Notes: Optical Eg: optical band gap; PL Peak: photoluminescence peak; Δ(Eg - PL Peak): the difference between the optical band gap and PL peak, correlated with the extent of band tailing; EUrbach: Urbach tail energy, is used to account for sub-band gap photon absorption and the characterized band tailing.
    下载: 导出CSV
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