CN111403558B - 高效率柔性叠层薄膜太阳能电池及其制备方法 - Google Patents
高效率柔性叠层薄膜太阳能电池及其制备方法 Download PDFInfo
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- UIPVMGDJUWUZEI-UHFFFAOYSA-N copper;selanylideneindium Chemical compound [Cu].[In]=[Se] UIPVMGDJUWUZEI-UHFFFAOYSA-N 0.000 claims abstract description 28
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Abstract
本发明公开了一种高效率柔性叠层薄膜太阳能电池及其制备方法,叠层薄膜太阳能电池包括底电池和堆叠在所述底电池上的顶电池,所述底电池的P型半导体吸收层为铜铟硒吸收层,所述顶电池的带隙宽于所述底电池。本发明的底电池采用窄禁带铜铟硒太阳能电池,可以以各种柔性材料为衬底制备柔性电池,且将窄禁带铜铟硒太阳能电池与宽禁带太阳能电池结合生长在柔性衬底上,通过调整禁带宽度的方式形成叠层电池,太阳能电池被按带隙宽窄程度叠合而成,从而达到了覆盖不同吸收波长范围的目的,使得柔性可弯曲的叠层电池效率最优化,通过采用机械堆叠法,可灵活地选择禁带宽度来分配光吸收效果,而且不需电流匹配,制备过程更简单。
Description
技术领域
本发明涉及太阳能电池技术领域,尤其涉及一种高效率柔性叠层薄膜太阳能电池及其制备方法。
背景技术
目前单层电池效率接近理论极限效率,其提升空间较小,串联太阳能电池技术提供了一种提高太阳能电池效率的有效方法,通过结合两个或多个具有不同吸收波段的太阳能电池来获取更广泛波长的太阳辐射。
提高聚合物太阳能电池效率的有效方法也是采用串联结构,通过利用更宽的太阳辐射光谱,使光子能量的热化损失最小化。然而,针对聚合物太阳能电池,由于缺乏合适的低禁带聚合物,其串联器件的性能明显落后于单层太阳能电池。另外,目前普遍采用的以晶体硅制作的底电池的叠层电池的缺点是硅片较厚,不能弯曲,因此也限制了其应用范围。
发明内容
鉴于现有技术存在的不足,本发明提供了一种高效率柔性叠层薄膜太阳能电池及其制备方法,该叠层薄膜太阳能电池除了具有薄膜太阳能电池的各种优点以外,还能保证串联性能,提高电池效率,具有制备方法简单、成本较低、应用范围更加广泛等优点。
为了实现上述的目的,本发明采用了如下的技术方案:
一种高效率柔性叠层薄膜太阳能电池的制备方法,包括:
制备底电池,所述底电池的P型半导体吸收层为铜铟硒吸收层;
制备顶电池,所述顶电池的带隙宽于所述底电池;
采用机械堆叠法,将所述顶电池堆叠在所述底电池上。
作为其中一种实施方式,制备底电池的步骤包括:
提供一柔性的第一衬底;
在所述第一衬底上形成背电极;
在所述背电极上采用三步共蒸发法制备所述铜铟硒吸收层;
对所述铜铟硒吸收层进行碱金属后沉积处理,并在处理后的所述铜铟硒吸收层上方依次制备第一半导体缓冲层、第一窗口层、第一透明前电极。
作为其中一种实施方式,制备底电池的步骤包括:
在三步共蒸发法制备所述铜铟硒吸收层的第一阶段生长铟,在第二阶段生长铜,在第三阶段生长铟使之形成贫铜相;
其中,在第三阶段生长过程中添加氟化钠,在第三阶段生长完成后的碱金属后沉积处理过程中添加氟化铷。
作为其中一种实施方式,所述第一阶段的生长过程包括:在5.0×10-5Pa~1.0×10-4Pa的本底真空条件下,在所述背电极上同时蒸镀In、Se两种元素,In和Se的蒸发源温度分别为810-830℃和240-300℃,所述第一衬底的温度为350℃-400℃,沉积时间为25-40min;
所述第二阶段的生长过程包括:在1.0×10-2Pa~2.0×10-2Pa的真空条件下,在前一阶段的基础上同时蒸镀Cu和Se两种元素,Cu和Se两种元素的蒸发源温度分别为1150-1300℃和240-300℃,所述第一衬底的温度为500-600℃,沉积时间为15-25min;
所述第三阶段的生长过程包括:在2.0×10-2Pa~3.0×10-2Pa的真空条件下,在前两阶段形成的膜层上同时蒸镀In和Se,In和Se两种元素的蒸发源温度分别为730-770℃和240-300℃,所述第一衬底的温度为500℃-600℃,沉积时间15-30min。
作为其中一种实施方式,在第三阶段生长过程中添加氟化钠的过程为:在真空为2.0×10-2Pa~3.0×10-2Pa、所述第一衬底的温度达到380℃的条件下,在Se的环境下通入氟化钠源,沉积时间为8-15min;
碱金属后沉积处理过程中添加氟化铷的过程为:当所述第一衬底的温度达到320℃时,在Se环境下通入氟化铷源,沉积时间为15-20min。
本发明的另一目的在于提供一种高效率柔性叠层薄膜太阳能电池,包括底电池和堆叠在所述底电池上的顶电池,所述底电池的P型半导体吸收层为铜铟硒吸收层,所述顶电池的带隙宽于所述底电池。
作为其中一种实施方式,所述底电池的铜铟硒吸收层的朝向所述顶电池的上表面覆盖有碱金属化合物沉积层。
作为其中一种实施方式,所述碱金属化合物沉积层由氟化钠和氟化铷沉积形成。
作为其中一种实施方式,所述底电池包括铜铟硒吸收层、设于所述铜铟硒吸收层下方的背电极以及自下而上依次层叠地设于所述铜铟硒吸收层上的所述碱金属化合物沉积层、第一半导体缓冲层、第一窗口层、第一透明前电极。
作为其中一种实施方式,所述顶电池的半导体吸收层为铜镓硒吸收层(20)、钙钛矿吸收层或CdTe。
本发明的底电池采用窄禁带铜铟硒太阳能电池,可以以各种柔性材料为衬底制备柔性电池,且将窄禁带铜铟硒太阳能电池与宽禁带太阳能电池结合生长在柔性衬底上,通过调整禁带宽度的方式形成叠层电池,太阳能电池被按带隙宽窄程度叠合而成,从而达到了覆盖不同吸收波长范围的目的,使得柔性可弯曲的叠层电池效率最优化,通过采用机械堆叠法,可灵活地选择禁带宽度来分配光吸收效果,而且不需电流匹配,制备过程更简单。
另外,本发明通过在窄禁带铜铟硒太阳能电池的吸收层中利用碱金属后沉积处理法提高空穴浓度,进而提高开路电压,从而明显提高了窄禁带铜铟硒太阳能电池的效率。
附图说明
图1为本发明实施例1的一种高效率柔性叠层薄膜太阳能电池的结构原理示意图;
图2为本发明实施例1的一种高效率柔性叠层薄膜太阳能电池的制备方法流程图;
图3为本发明实施例1的一种制备铜铟硒底电池的方法流程图;
图4为本发明实施例2的顶电池的结构示意图;
图中标号说明如下:
1-底电池;
1a-背电极;
10-铜铟硒吸收层;
11-碱金属化合物沉积层;
12-第一半导体缓冲层;
13-第一窗口层;
14-第一透明前电极;
2-顶电池;
2a-透明电极;
20-铜镓硒吸收层;
21-第二半导体缓冲层;
22-第二窗口层;
23-第二透明前电极;
201-光阳极;
202-电子传输层;
203-钙钛矿吸收层;
204-空穴传输层;
205-背电极;
A-第一衬底;
B-第二衬底。
具体实施方式
为了使本发明的目的、技术方案及优点更加清楚明白,以下结合附图及实施例,对本发明进一步详细说明。应当理解,此处所描述的具体实施例仅仅用以解释本发明,并不用于限定本发明。
实施例1
结合图1和图2所示,本发明提供了一种高效率柔性叠层薄膜太阳能电池及其制备方法,该制备方法包括:
S01、制备底电池1,底电池1的P型半导体吸收层为铜铟硒吸收层10;
S02、制备顶电池2,顶电池2的带隙宽于底电池1;
S03、采用机械堆叠法,将顶电池2堆叠在底电池1上。
本实施例中,窄带隙底电池1、宽带隙的顶电池2可以分别独立地制作,然后采用机械堆叠法按4端堆叠结构形成,不仅可以灵活地选择禁带宽度来分配光吸收,而且不需电流匹配,更容易制备。在将顶电池2堆叠在底电池1上后,在顶电池2上制备顶端欧姆接触电极用作收集电极,即可完成叠层薄膜太阳能电池的制备。顶端欧姆接触电极可以采用电子束蒸发、丝网印刷法制备。
本实施例根据两个子电池带隙的不同,吸收光谱范围的不同,利用吸收光谱互补、扩大光谱利用率从而提高了电池效率。由于铜铟硒(CuInSe2,简称CIS)是一种直接带隙材料,光吸收率高达105量级,制作的电池厚度可以做到2~3μm,非常适于太阳电池薄膜化,因此降低了昂贵材料的消耗,其可以以不锈钢或耐高温聚合物为衬底,制备而成的柔性电池可适合于建筑物曲面屋顶等处使用,还可以做成折叠式电源,方便携带,也可以供给小型仪器计算机及军事通信GPS等领域的移动设备使用,可极大的拓展其应用领域。
如图1所示,底电池1包括柔性的第一衬底A和自下而上依次层叠在第一衬底A上的背电极1a、铜铟硒吸收层10、碱金属化合物沉积层11、第一半导体缓冲层12、第一窗口层13、第一透明前电极14。
如图3所示,本实施例中,制备底电池1的步骤主要包括:
S011、提供一柔性的第一衬底A,第一衬底A优选采用柔性不锈钢材料。
首先,用温热去离子水和碱性清洗剂清洗10*10的柔性不锈钢,并在超声机内用无水乙醇清洗15分钟,控制低速用氮气***吹掉表面多余水分,然后放入烘箱中烘干。
然后,将第一衬底A置于真空室中,置于衬底固定器中预定的中心位置。
S012、在第一衬底A上形成背电极1a。
背电极1a的材料优选采用钼(Mo),在第一衬底A上通过蒸发Mo的方式形成背电极1a。蒸发Mo用到的参数为第一层2.0Pa、350W、20次;第二层为0.3Pa、1000w、10次,背电极1a的厚度大约1.1μm;XRF(X Ray Fluorescence,即X射线荧光光谱分析)计数为1044。
S013、在背电极1a上采用三步共蒸发法制备铜铟硒吸收层10。
其中,在三步共蒸发法制备铜铟硒吸收层10的第一阶段生长铟,在第二阶段生长铜,在第三阶段生长铟使之形成贫铜相,在第三阶段生长过程中添加氟化钠。在第三阶段生长过程中添加氟化钠,充分考虑到其在第三阶段的掺入对薄膜表面的结晶度影响较小的前提下又可以提高开路电压和填充因子,因此,相应的太阳能电池可以表现出更好的性能。
具体地,三步共蒸发法的第一阶段的生长过程包括:将背电极1a放入5.0×10-5Pa~1.0×10-4Pa的本底真空条件的腔体内,在本底真空条件下,在背电极1a上同时蒸镀In、Se两种元素,In和Se的蒸发源温度分别为810-830℃和240-300℃,第一衬底A的温度为350℃-400℃,沉积时间为25-40min;
第二阶段的生长过程包括:在1.0×10-2Pa~2.0×10-2Pa的真空条件下,在前一阶段的基础上同时蒸镀Cu和Se两种元素,Cu和Se两种元素的蒸发源温度分别为1150-1300℃和240-300℃,第一衬底A的温度为500-600℃,沉积时间为15-25min;
第三阶段的生长过程包括:在2.0×10-2Pa~3.0×10-2Pa的真空条件下,在前两阶段形成的膜层上同时蒸镀In和Se,In和Se两种元素的蒸发源温度分别为730-770℃和240-300℃,第一衬底A的温度为500℃-600℃,沉积时间15-30min。
在第三阶段生长过程中添加氟化钠的过程为:在真空为2.0×10-2Pa~3.0×10- 2Pa、第一衬底A的温度达到380℃的条件下,在Se的环境下通入氟化钠(NaF)源,沉积时间为8-15min。
S014、对铜铟硒吸收层10进行碱金属后沉积处理,在此过程中,需要添加氟化铷。
由于本实施例在吸收层生长完成后才添加氟化铷,使得更重的碱金属在晶界处形成RbInSe2的二次相,从而起到钝化缺陷的作用。
碱金属后沉积处理过程中添加氟化铷的过程具体为:当第一衬底A的温度达到320℃时,在Se环境下通入氟化铷源,沉积时间为15-20min。
S015、在处理后的铜铟硒吸收层10上方依次制备第一半导体缓冲层12、第一窗口层13、第一透明前电极14。
N型的第一半导体缓冲层12材料可以是:硫化镉、硫化锌、掺杂镉硫化锌、锌镁氧、锌硫氧、硒化铟中的任意一种,厚度为50nm-80nm。这里,优选采用硫化镉(CdS)。第一半导体缓冲层12可以采用化学水浴、磁控溅射或者原子层沉积方法制备。
第一半导体缓冲层12优选采用化学水浴法制得,具体是:将0.184g的硫酸镉溶于60ml去离子水中,5.694g的硫脲溶于150ml的去离子水中,用去离子水冲洗铜铟硒吸收层10表面然后放入大烧杯中,将45ml的浓氨水(28-30%)与上述硫酸镉溶液混合倒入大烧杯中,将硫脲溶液也倒入大烧杯中,然后将大烧杯放入69℃水浴锅内,用磁力搅拌器匀速搅拌9min,取出用去离子水冲洗然后用高纯氮气吹干迅速放入160℃烘箱退火2min。
铜铟硒吸收层10的厚度为2-3μm,硫化镉的第一半导体缓冲层12的厚度为50nm,栅型收集电极(欧姆接触电极)为镍/铝/镍(Ni/Al/Ni)三层叠层或铬/镍/金(Cr/Ni/Au),镍/铝/镍(或铬/镍/金)厚度分别为100nm/8000nm/100nm,可以依次通过电子束蒸发法蒸镀叠加。用电子束热蒸发法制备Ni/Al/Ni栅型收集电极时,最上层Ni可以防止第二层的Al与空气反应被氧化,最下层的Ni可以使电极不易脱落。
第一窗口层13优选采用氧化锌(ZnO),氧化锌厚度为100nm。第一透明前电极14优选掺铝氧化锌,铝掺杂比例为0.2%,厚度200nm-400nm,透过率>85%,电导率<6×10-4Ω.cm2。
第一窗口层13、第一透明前电极14均可采用磁控溅射的方式形成,例如,第一窗口层13制作时,氩气流量为20sccm,氧气流量为2.0sccm,在溅射功率120W的条件下溅射4次,随后将功率调整到220W溅射16次。溅射第一透明前电极14时,将第一衬底A温度加热至90℃,氩气流量为20sccm,氢气流量为2.5sccm,在溅射功率750W的条件下溅射12次。
本实施例的顶电池2为铜镓硒(CGS)太阳能电池,其半导体吸收层为铜镓硒吸收层20,由三种原料铜、镓、硒制得,所得吸收层厚度为2-3μm。顶电池2主要包括第二衬底B和自下而上依次层叠在第二衬底B上的透明电极2a、铜镓硒吸收层20、第二半导体缓冲层21、第二窗口层22、第二透明前电极23。
透明电极2a可以是全透明或半透明的ITO,光透过率≥85%,所用材料为氧化锌掺杂铝透明导电膜,厚度为150nm。第二衬底B、第二半导体缓冲层21、第二窗口层22、第二透明前电极23的材料和厚度以及工艺可以与底电池1中的第一衬底A、第一半导体缓冲层12、第一窗口层13、第一透明前电极14相同。
铜镓硒吸收层20采用铜、镓、硒元素三步共蒸发法制得,并通过衬底背后的热偶探测到衬底温度,在第一步的衬底温度为450℃,在第二步的衬底温度为600℃,第三步的衬底温度为600℃,Ga的沉积速率为4A°/s,Cu的沉积速率为3A°/s,Se的沉积速率在三步中都稳定保持在30A°/s。其衬底温度下降2℃在第二步末尾形成富铜相,在第三步衬底温度上升2℃,添加Ga,使其形成贫铜相。由于热偶与衬底间有一定距离,所以热偶所探测到的衬底温度比实际衬底表面的温度低30-50℃。
本发明的另一目的在于提供一种高效率柔性叠层薄膜太阳能电池,包括底电池1和堆叠在底电池1上的顶电池2,底电池1的P型半导体吸收层为铜铟硒吸收层10,顶电池2的带隙宽于底电池1。
与之相应的,底电池1的铜铟硒吸收层10的朝向顶电池2的上表面覆盖有碱金属化合物沉积层11。碱金属化合物沉积层11由氟化钠和氟化铷沉积形成。
实施例2
与实施例1不同,本实施例的叠层薄膜太阳能电池的顶电池2可以是钙钛矿(perovskite)电池或者碲化镉(CdTe)电池,顶电池2对应的半导体吸收层为钙钛矿吸收层或CdTe。以禁带宽度为1.0eV左右的CIS柔性电池为底电池1,与禁带宽度为1.7eV左右的宽禁带柔性钙钛矿和碲化镉薄膜太阳能前电池结合,可形成效率高达30%以上的双节叠层柔性太阳能电池。
如图4所示,为钙钛矿顶电池的结构示意图。
钙钛矿顶电池2主要由光阳极201、电子传输层(ETL)202、钙钛矿吸收层203、空穴传输层(HTL)204、背电极205组成。其中光阳极201一般为掺氟氧化物(FTO),背电极205一般为金(Au)或银(Ag)电极。
钙钛矿吸收层203的制备方法选用工艺简单且无需真空的溶液法,具体涉及两步法。首先将金属卤化物(通常为碘化铅PbI2)沉积在薄膜上,然后通过气相或液相方法,使金属卤化物与阳离子卤化物(MAI、FAI等)反应生成钙钛矿吸收层203。
具体实施方法为:首先,制备碘化钾胺(MAI)粉末,将氢碘酸水溶液和甲胺甲醇溶液混合后,沐浴条件下搅拌两小时,随后在50℃条件下旋蒸一小时,用***清洗3次后进行真空干燥得到MAI粉末。然后按1.2M浓度将PbI2溶于极性溶剂DMF中搅拌至完全溶解,将40μL的PbI2溶液滴到TiO2膜上停留30s后,以2000rpm转速旋涂60s。旋涂完成后,将膜置于90℃热台上加热5min以去除膜中剩余的溶剂。冷却至室温后将膜浸入10mg/mL浓度的MAI溶液中(溶于异丙醇),在PbI2转化为MAPbI3后,用异丙醇清洗并在90℃热台上退火40min即得MAPbI3钙钛矿吸收层203。
将制得的钙钛矿电池作为叠层电池的顶电池,与制备的CIS底电池按4端堆叠结构,将钙钛矿电池直接堆叠在CIS电池上,即得钙钛矿/铜铟硒的叠层太阳能电池。
综上,本发明的底电池采用窄禁带铜铟硒太阳能电池,可以以各种柔性材料为衬底制备柔性电池,且将窄禁带铜铟硒太阳能电池与宽禁带太阳能电池结合生长在柔性衬底上,通过调整禁带宽度的方式形成叠层电池,太阳能电池被按带隙宽窄程度叠合而成,从而达到了覆盖不同吸收波长范围的目的,使得柔性可弯曲的叠层电池效率最优化,通过采用机械堆叠法,可灵活地选择禁带宽度来分配光吸收效果,而且不需电流匹配,制备过程更简单。而且,本发明通过在窄禁带铜铟硒太阳能电池的吸收层中利用碱金属后沉积处理法提高空穴浓度,进而提高开路电压,从而明显提高了窄禁带铜铟硒太阳能电池的效率,该叠层电池具备低成本、柔性可弯曲、高效率等优势,具有广阔的应用前景。
以上所述仅是本申请的具体实施方式,应当指出,对于本技术领域的普通技术人员来说,在不脱离本申请原理的前提下,还可以做出若干改进和润饰,这些改进和润饰也应视为本申请的保护范围。
Claims (7)
1.一种高效率柔性叠层薄膜太阳能电池的制备方法,其特征在于,包括:
制备底电池(1),所述底电池(1)的P型半导体吸收层为铜铟硒吸收层(10);
制备顶电池(2),所述顶电池(2)的带隙宽于所述底电池(1);
采用机械堆叠法,将所述顶电池(2)堆叠在所述底电池(1)上;
其中,制备底电池(1)的步骤包括:
提供一柔性的第一衬底(A);
在所述第一衬底(A)上形成背电极(1a);
在所述背电极(1a)上采用三步共蒸发法制备所述铜铟硒吸收层(10);
对所述铜铟硒吸收层(10)进行碱金属后沉积处理,并在处理后的所述铜铟硒吸收层(10)上方依次制备第一半导体缓冲层(12)、第一窗口层(13)、第一透明前电极(14);
其中,制备底电池(1)的步骤包括:
在三步共蒸发法制备所述铜铟硒吸收层(10)的第一阶段生长铟,在第二阶段生长铜,在第三阶段生长铟使之形成贫铜相;其中,在第三阶段生长过程中添加氟化钠,在第三阶段生长完成后的碱金属后沉积处理过程中添加氟化铷;
其中,所述第一阶段的生长过程包括:在5.0×10-5Pa~1.0×10-4Pa的本底真空条件下,在所述背电极(1a)上同时蒸镀In、Se两种元素,In和Se的蒸发源温度分别为810-830℃和240-300℃,所述第一衬底(A)的温度为350℃-400℃,沉积时间为25-40min;
所述第二阶段的生长过程包括:在1.0×10-2Pa~2.0×10-2Pa的真空条件下,在前一阶段的基础上同时蒸镀Cu和Se两种元素,Cu和Se两种元素的蒸发源温度分别为1150-1300℃和240-300℃,所述第一衬底(A)的温度为500-600℃,沉积时间为15-25min;
所述第三阶段的生长过程包括:在2.0×10-2Pa~3.0×10-2Pa的真空条件下,在前两阶段形成的膜层上同时蒸镀In和Se,In和Se两种元素的蒸发源温度分别为730-770℃和240-300℃,所述第一衬底(A)的温度为500℃-600℃,沉积时间15-30min。
2.根据权利要求1所述的高效率柔性叠层薄膜太阳能电池的制备方法,其特征在于,
在第三阶段生长过程中添加氟化钠的过程为:在真空为2.0×10-2Pa~3.0×10-2Pa、所述第一衬底(A)的温度达到380℃的条件下,在Se的环境下通入氟化钠源,沉积时间为8-15min;
碱金属后沉积处理过程中添加氟化铷的过程为:当所述第一衬底(A)的温度达到320℃时,在Se环境下通入氟化铷源,沉积时间为15-20min。
3.一种高效率柔性叠层薄膜太阳能电池,其特征在于,所述高效率柔性叠层薄膜太阳能电池由权利要求1或2所述的制备方法制备形成,所述高效率柔性叠层薄膜太阳能电池包括底电池(1)和堆叠在所述底电池(1)上的顶电池(2),所述底电池(1)的P型半导体吸收层为铜铟硒吸收层(10),所述顶电池(2)的带隙宽于所述底电池(1),所述铜铟硒吸收层(10)由三步共蒸发法制备形成。
4.根据权利要求3所述的高效率柔性叠层薄膜太阳能电池,其特征在于,所述底电池(1)的铜铟硒吸收层(10)的朝向所述顶电池(2)的上表面覆盖有碱金属化合物沉积层(11)。
5.根据权利要求4所述的高效率柔性叠层薄膜太阳能电池,其特征在于,所述碱金属化合物沉积层(11)由氟化钠和氟化铷沉积形成。
6.根据权利要求4所述的高效率柔性叠层薄膜太阳能电池,其特征在于,所述底电池(1)包括铜铟硒吸收层(10)、设于所述铜铟硒吸收层(10)下方的背电极(1a)以及自下而上依次层叠地设于所述铜铟硒吸收层(10)上的所述碱金属化合物沉积层(11)、第一半导体缓冲层(12)、第一窗口层(13)、第一透明前电极(14)。
7.根据权利要求3~6任一所述的高效率柔性叠层薄膜太阳能电池,其特征在于,所述顶电池(2)的半导体吸收层为铜镓硒吸收层(20)、钙钛矿吸收层或CdTe。
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