CN102414827A - 具有基于聚硅氮烷的包封层的太阳能电池 - Google Patents
具有基于聚硅氮烷的包封层的太阳能电池 Download PDFInfo
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Abstract
薄膜太阳能电池(10)，包括由金属或玻璃构成的基材(1)、铜-铟-硫化物(CIS)或铜-铟-镓-硒化物(CIGSe)型光伏层状结构(4)和基于聚硅氮烷的包封层(5)。
Description
本发明涉及黄铜矿太阳能电池，包括基材和光伏层状结构。特别是涉及具有铜-铟-硫化物(CIS)或铜-铟-镓-硒化物(CIGSe)型光伏层状结构的薄膜太阳能电池。
此外，本发明涉及制备黄铜矿基太阳能电池的方法。在该方法的范畴内，所述太阳能电池设置有包封层，其通过使聚硅氮烷和添加剂的溶液在20-1000℃，特别是80-200℃范围内的温度下硬化而产生。
鉴于缺乏化石资源，光伏技术作为可更新并且有利环境的能源具有重大意义。太阳能电池将阳光转化为电流。在太阳能电池中晶体硅或非晶硅大多用作光吸收半导体材料。硅的使用带来巨大的成本。与之相反，可以用低得多的成本制备具有由黄铜矿材料，如铜-铟-硫化物(CIS)或铜-铟-镓-硒化物(CIGSe)构成的吸收体的薄膜太阳能电池。
为了迅速推广光伏技术，通常需要改善光伏发电的费效比。为此值得期待的是，提高太阳能电池的效率和使用寿命。太阳能电池的效率被定义为电功率(即电压和光电流之积)与入射光功率之比。此外，效率与渗入吸收层并有助于产生电子-空穴对的光子的数量成正比。在太阳能电池表面反射的光子对光电流没有贡献。相应地，可以通过减少太阳能电池表面的光反射来提高效率。太阳能电池的使用寿命可以通过改善对于由气候造成的降解过程的保护而得到延长。通过渗入的水或水蒸气，使降解过程加速。因此，为了将太阳能电池与水蒸气隔离，现有技术中使用由层复合体组成的包封，该层复合体包括玻璃和EVA以及任选的PVA和其他聚合物薄膜。
但是，现有技术中用于包封的材料具有缺点。特别是玻璃导致高的组件重量，这例如对顶部结构提出高的要求，并且PVA和PVB在光作用下与痕量水一起释放损害太阳能电池功能的酸。前侧扩散阻挡或者包封层的效用在人工气候室中借助于根据DIN EN 61646的加速老化试验来测试。包封的太阳能组件在85℃以及85％相对空气湿度下贮存超过1000h，并定期按照其电特征进行分析，并由此测定降解。
已知的是，为了前侧面包封太阳能电池，使用SiOx层。这类SiOx层由气相通过CVD法如微波等离子体增强气相沉积(MWPECVD)和PVD法如磁控溅射来沉积。这些真空技术方法与高昂的成本相关，并且另外还有以下缺点：由此制备的层具有较低的粘附性和机械强度。此外，CVD法需要使用高度易燃气体(SiH4，CH4，H2)和毒性气体(NH3)。
作为用于黄铜矿太阳能电池的基材材料，使用玻璃或由金属或聚酰亚胺构成的薄膜。玻璃在许多方面被证明是有利的，因为其是电绝缘的，具有光滑的表面并且在制备黄铜矿吸收体层期间提供钠，所述钠从玻璃扩散入吸收体层，并且作为掺杂物改善吸收体层的性质。玻璃的缺点在于其重量大以及缺乏柔韧性。特别地，由于其刚性，不能以低成本的辊对辊方法(Rolle zu Rolle Verfahren)涂覆。由金属或塑料构成的薄膜型基材比玻璃轻并且是柔性的，使得其适于通过低成本的辊对辊方法进行制备。但是，由于金属薄膜或塑料薄膜的特性，其对黄铜矿层复合体的性质产生不良影响，并且也不具有用于吸收体掺杂的钠沉积物。由于升高的温度(有时超过500℃)(在太阳能电池制备期间基材暴露于该温度)，优选使用由钢或钛构成的金属膜。
为了将太阳能电池整体连接到钛膜或钢膜上，必须使光伏层状结构或后触点与基材薄膜电绝缘。为此，将由电绝缘材料构成的层施加到该金属基材薄膜上。此外，该电绝缘层应起到扩散阻挡作用，以便阻止损害吸收体层的金属离子扩散。例如，铁原子提高黄铜矿吸收体层中载流子(电子和空穴)的复合率，由此减少光电流。硅氧化物(SiOx)适于作为绝缘的和阻止扩散的阻挡层的材料。
现有技术已知的是，主要由SiOx或SiNx组成的保护层以及包封层用于电子器件以及基于硅或其他半导体材料的太阳能电池。
US 7,067,069公开了用于硅基太阳能电池的由SiO2构成的绝缘包封层，其中，SiO2层通过施加聚硅烷以及随后在100-800℃，优选300-500℃的温度下的硬化来制备。
US 6,501,014B1涉及一种物品，特别是具有由硅酸盐类材料构成的具有透明、耐热和耐候性保护层的基于非晶硅的太阳能电池。该保护层以简单的方式在使用聚硅氮烷的条件下来制备。在基于聚硅氮烷的保护层和光伏层状体系之间布置柔性橡胶状粘合层或者缓冲体层。
US 7,396,563教导了借助PA-CVD沉积介电的并且钝化的聚硅氮烷层，其中，使用聚硅烷作为CVD前体。
US 4,751,191公开了借助PA-CVD沉积用于太阳能电池的聚硅氮烷层。所获得的聚硅氮烷层以光刻技术结构化，并用于掩蔽金属触点以及用作防反光层。
现有技术所述的具有由SiOx或SiNx构成的包封层的太阳能电池在其制备中成本过高，并且需要使用两层或更多层的层复合体，其除了包封层外，还包括载体薄膜、缓冲体层、增粘剂层和/或反射体层。特别地，对于不是基于硅的光电吸收体的太阳能电池，需要弥补包封层热失衡的缓冲体层。热失衡，即相邻层的热膨胀系数的差异引起机械应力，其通常导致裂隙形成以及剥离。尤其还遇见这一问题：包封层在低温下沉积在太阳能电池上。然而，如此在低温下产生的包封层对于水蒸气和氧气大多不具有足够的阻挡作用。
考虑到现有技术，本发明目的在于，提供具有高效率和高耐老化性的黄铜矿太阳能电池以及其低成本的制备方法。
本发明目的通过包括基材、光伏层状结构和基于聚硅氮烷的包封层的黄铜矿太阳能电池得以实现。
以下依据附图更清楚地阐释本发明，其中：
图1描述太阳能电池的透视剖面图，以及
图2描述不具有和具有包封层的太阳能电池的反射曲线。
图1以透视视角示出了通过具有基材1、任选的阻挡层2、光伏层状结构4和包封层5的本发明的太阳能电池10的剖面图。该太阳能电池10优选设置为薄膜太阳能电池并具有铜-铟-硫化物(CIS)或铜-铟-镓-硒化物(CIGSe)型光伏层状结构4。
本发明的包封层5具有彼此相对的第一和第二表面。在优选的具体实施方式中，所述包封层的所述第一表面直接邻接于光伏层状结构4，并且所述包封层的所述第二表面形成太阳能电池的外侧。
本发明太阳能电池10的改进方案的特征在于，
-其设置为薄膜太阳能电池并具有铜-铟-硫化物(CIS)或铜-铟-镓-硒化物(CIGSe)型光伏层状结构4；
-所述光伏层状结构4包括由钼构成的后触点41，组成为CuInSe2、CuInS2、CuGaSe2、CuIn1-xGaxSe2其中0＜x≤0.5或Cu(InGa)(Se1-ySy)2其中0＜y≤1；的吸收体42，由CdS构成的缓冲体43，由ZnO或ZnO:Al构成的窗层44以及由Al或银构成的前触点45，
-基材1由包含金属、金属合金、玻璃、陶瓷或塑料的材料构成；
-基材1以膜的形式，特别是以钢膜或钛膜的形式形成；
-包封层5具有100-3000nm，优选200-2500nm，以及特别是300-2000nm的厚度；
-基材1由导电材料构成，并且电镀沉积了组成光伏层状结构(4)的一个或多个层；
-太阳能电池10包括在基材1和光伏层状结构4之间布置的基于聚硅氮烷的阻挡层2；
-阻挡层2含有钠或包括含钠的前驱层21；
-包封层5和任选地由硬化的聚硅氮烷和添加剂在溶剂中的溶液构成的阻挡层2，该溶剂优选是二丁基醚；
-所述聚硅氮烷具有通式(I)
-(SiR′R″-NR″′)n-(I)
其中R′、R″、R″′相同或不同，并且彼此独立地为氢或任选取代的烷基、芳基、乙烯基或(三烷氧基甲硅烷基)烷基残基，其中n为整数并如此确定n，使得所述聚硅氮烷具有150-150000g/mol，优选50000-150000g/mol，和特别为100000-150000g/mol的数均分子量；
-至少一种聚硅氮烷选自其中R′、R″和R″′＝H的全氢聚硅氮烷；
-太阳能电池10对于波长范围为300-900nm的光具有低于97％，优选低于96％，和特别地低于95％的平均相对反射率，以施加包封层5之前的太阳能电池10的反射率计；
和
-太阳能电池10对于波长范围为1100-1500nm的光具有大于120％，优选大于150％，和特别地大于200％的平均相对反射率，以施加包封层5之前的太阳能电池10的反射率计。
图2示出了具有和不具有本发明的基于聚硅氮烷的包封层的黄铜矿太阳能电池的光谱反射率的测量结果(图2中以实线表示“具有SiOx”，以虚线表示“不具有SiOx”)。依照DIN EN ISO 8980-4，对具有包封层的本发明太阳能电池和不具有包封层的参比太阳能电池进行光谱反射率测量。除了所述包封层外，本发明的太阳能电池和参比太阳能电池具有同样的结构，并经历了同样的制备过程。为了确定平均相对反射率，将所获得的光谱反射曲线叠加，并在300-900nm和1100-1500nm两个波长区间内进行数值评估。在此，在每个上述波长区间内在彼此间距可以在1-20nm范围内选择的等距取样点上，计算本发明的太阳能电池和参比太阳能电池的反射值的商，并且得出所有的、在区间内含有的取样点的商的平均值。
在300-900nm的波长区间内，本发明的太阳能电池具有低于97％直至低于95％的平均相对反射率。反射率是外部量子效率(EQE)和太阳能电池效率的系数。与此相应地，相对于参比太阳能电池，本发明的包封层提高太阳能电池的外部量子效率平均多于3％至超过5％。采用现有技术已知的包封层，相对于参比，平均反射率提高最高为2％。因此，通过本发明包封层，常规的黄铜矿太阳能电池的效率提高了1.01-1.03的系数。在例如15％的效率下，这相应于改进了多于0.15％-0.45％。
黄铜矿太阳能电池的效率随温度升高而降低。由于对红外线升高的反射率，本发明的包封层降低了通过日射引起的太阳能电池的升温，并由此也以这种方式有助于改善效率。在波长范围为1100-1500nm时，本发明的太阳能电池具有大于120％直至大于200％的平均相对反射率。
在根据DIN EN 61646的加速老化试验(在85℃的温度和85％的相对湿度下的湿热试验)中，在800h后，本发明太阳能电池表现出高于70％，优选高于75％和特别是高于80％的效率，以初始值计，即在老化试验开始前。
制备本发明太阳能电池的方法包括以下步骤a)-f)：
a)将基于黄铜矿的光伏层状结构施加到任选地配备有阻挡层的基材上，
b)用含有至少一种通式(I)的聚硅氮烷的溶液涂覆光伏层状结构
-(SiR′R″-NR″′)n-(I)
其中R′、R″、R″′相同或不同，并且彼此独立地为氢或任选取代的烷基、芳基、乙烯基或(三烷氧基甲硅烷基)烷基残基，其中n为整数并如此确定n，使得所述聚硅氮烷具有150-150000g/mol，优选50000-150000g/mol，和特别为100000-150000g/mol的数均分子量，
c)通过蒸发去除溶剂，其中获得厚度为100-3000nm，优选200-2500nm，特别为300-2000nm的聚硅氮烷层，
d)任选地一次或多次重复步骤b)和c)
e)通过i)加热到20-1000℃，特别是80-200℃范围内的温度和/或ii)用180-230nm范围内的波长段的紫外线辐照，使所述聚硅氮烷层硬化，其中所述加热和/或辐照在1min-14h，优选1min-60min和特别是1min-30min期间内进行，优选在由含水蒸气的空气或氮气构成的气氛下，
和
f)任选地，在20-1000℃，优选60-130℃温度下，在相对湿度为60-90％的空气中，在1min-2h，优选30min-1h期间内，对所述聚硅氮烷层进行后硬化。
本发明的方法的有利实施方式的特征在于，用于涂覆的聚硅氮烷溶液含有一种或多种下述成分：
-至少一种其中R′、R″和R″′＝H的全氢聚硅氮烷；和
-催化剂，以及任选的其他添加剂。
优选地所述黄铜矿太阳能电池在柔性带状基材上以辊对辊方法制成。
在用于制备本发明的包封层的聚硅氮烷溶液中，聚硅氮烷的份额为1-80重量％，优选2-50重量％，和特别是5-20重量％，以溶液的总重量计。
适合作为溶剂的特别是有机溶剂，优选非质子溶剂，其不含水以及反应性基团如羟基-或氨基基团，并且对聚硅氮烷是惰性的。实例是芳族或脂族烃及其混合物。它们例如是脂族或芳族烃、卤代烃、酯如乙酸乙酯或乙酸丁酯、酮如丙酮或甲乙酮、醚如四氢呋喃或二丁基醚、以及单-和聚亚烷基二醇二烷基醚(Glymes)或由这些溶剂组成的混合物。
聚硅氮烷溶液的其他组分可以是催化剂，例如有机胺、酸以及金属或金属盐或这些化合物的混合物，其促进层形成过程。特别合适作为胺催化剂的是N，N-二乙基乙醇胺、N，N-二甲基乙醇胺、N，N-二甲基丙醇胺、三乙胺、三乙醇胺和3-吗啉代丙胺。催化剂优选以0.001-10重量％，特别地0.01-6重量％，特别优选地0.1-5重量％的量使用，以聚硅氮烷重量计。
其他组分可以是用于衬底润湿和成膜的添加剂以及由氧化物如SiO2、TiO2、ZnO、ZrO2或Al2O3构成的无机纳米颗粒。
为了制备本发明的太阳能电池，按照已知的方法在基材如钢膜上产生基于黄铜矿的光伏层状结构。优选地，在施加光伏层状结构之前，为钢膜配备电绝缘层，特别是基于聚硅氮烷的SiOx阻挡层。由此通过DC磁控溅射沉积约1μm的钼层作为后触点，并优选结构化成整体连接(P1节段)。为此所需的将带状钼层分成条带用激光切割装置实施。
黄铜矿吸收体层的制备优选在3阶段PVD工艺中在约3·10-6mbar的压力下进行。PVD工艺总时间为约1.5h。在此，有利的是，如此进行所述工艺，使得基材最高温度低于400℃。
随后，以湿式化学方式在约60℃的温度下沉积CdS缓冲体层。由i-ZnO和用铝掺杂的ZnO构成的窗层通过DC磁控溅射沉积。
为了制备本发明包封层，将上述组成的聚硅氮烷溶液以常规的涂覆方法，例如通过喷嘴或浸浴施加到基材上，优选施加到钢膜上，并且任选地用弹性刮刀刮平，以确保在光伏层状结构上均匀的厚度分布或材料覆盖。在柔性基材如由金属或塑料构成的适于辊对辊涂覆的膜上，也可以采用缝隙式喷嘴作为施加系统用于获得非常薄的均匀的层。此后蒸发溶剂。这可在室温下或在使用合适的干燥器时在较高的温度，优选40-60℃下在辊对辊方法中以＞1m/min的速度进行。
涂覆聚硅氮烷溶液，随后蒸发溶剂的步骤顺序任选地重复一次、两次或更多次，以便获得干燥的、未硬化的(“生的”)的总厚度为100-3000nm的聚硅氮烷层。通过多次进行由涂覆和干燥组成的步骤顺序，在生的聚硅氮烷层中的溶剂含量明显降低或消除。通过这种方式可以改善硬化的聚硅氮烷膜在黄铜矿层状结构上的粘附性。多次涂覆和干燥的另一优点在于，很大程度上覆盖并封闭单层中可能存在的孔洞或裂隙，以便进一步降低水蒸气透过性。
在100-180℃范围内的温度下在0.5-1h期间内通过硬化将该干燥的或生的聚硅氮烷层转化成透明的陶瓷相。所述硬化在对流烘箱中进行，该烘箱可选地用过滤的且用水蒸气润湿的空气或用氮气运行。视温度、持续时间和烘箱气氛(含水蒸汽的空气或氮气)而定，所述陶瓷相具有不同的组成。如果硬化例如在含水蒸汽的空气中进行，则获得组成为SiNvHwOxCy的相，其中x＞v；v＜1；0＜x＜1.3；0≤w≤2.5且y＜0.5。而在氮气气氛下的硬化则形成组成为SiNvHwOxCy的相，其中v＜1.3；x＜0.1；0≤w≤2.5且y＜0.2。
此外，水蒸气透过性可以采用以下方式降低：将聚硅氮烷再次硬化。这种“后硬化”特别地在温度约为85℃，相对湿度为85％空气中在1h期间内进行。光谱分析显示，后硬化明显降低聚硅氮烷层的氮含量。
本说明书、权利要求书以及附图中公开的本发明的特征既可以单独地，也可以以任意组合的方式用于在其多种实施方式中实现本发明。
Claims (20)
1.黄铜矿太阳能电池(10)，包括基材(1)、光伏层状结构(4)和基于聚硅氮烷的包封层(5)。
2.根据权利要求1的太阳能电池(10)，其特征在于，其设置成薄膜太阳能电池，并具有铜-铟-硫化物(CIS)或铜-铟-镓-硒化物(CIGSe)型光伏层状结构(4)。
3.根据权利要求1或2的太阳能电池(10)，其特征在于，光伏层状结构(4)包括由钼构成的后触点(41)，组成为CuInSe2、CuInS2、CuGaSe2、CuIn1-xGaxSe2其中0＜x≤0.5或Cu(InGa)(Se1-ySy)2其中0＜y≤1的吸收体(42)，由CdS构成的缓冲体(43)，由ZnO或ZnO:Al构成的窗层(44)以及由Al或银构成的前触点(45)。
4.根据权利要求1、2或3的太阳能电池(10)，其特征在于，基材(1)由包含金属、金属合金、玻璃、陶瓷或塑料的材料构成。
5.根据权利要求1-4一项或多项的太阳能电池(10)，其特征在于，基材(1)以膜的形式，特别是以钢膜或钛膜的形式形成。
6.根据权利要求1-5一项或多项的太阳能电池(10)，其特征在于，所述包封层(5)具有100-3000nm，优选200-2500nm，以及特别是300-2000nm的厚度。
7.根据权利要求1-6一项或多项的太阳能电池(10)，其特征在于，基材(1)由导电材料构成，并且电镀沉积了组成光伏层状结构(4)的一个或多个层。
8.根据权利要求1-7一项或多项的太阳能电池(10)，其特征在于，其包括在基材(1)和光伏层状结构(4)之间布置的基于聚硅氮烷的阻挡层(2)。
9.根据权利要求8的太阳能电池(10)，其特征在于，阻挡层(2)含有钠或包括含钠的前驱层(21)。
10.根据权利要求1-9一项或多项的太阳能电池(10)，其特征在于，包封层(5)和任选地阻挡层(2)由硬化的聚硅氮烷和添加剂在溶剂中的溶液构成，该溶剂优选是二丁基醚。
11.根据权利要求10的太阳能电池(10)，其特征在于，所述聚硅氮烷具有通式(I)
-(SiR′R″-NR″′)n-(I)
其中R′、R″、R″′相同或不同，并且彼此独立地为氢或任选取代的烷基、芳基、乙烯基或(三烷氧基甲硅烷基)烷基残基，其中n为整数并如此确定n，使得所述聚硅氮烷具有150-150000g/mol，优选50000-150000g/mol，和特别为100000-150000g/mol的数均分子量。
12.根据权利要求11的太阳能电池(10)，其特征在于，至少一种聚硅氮烷选自其中R′、R″和R″′＝H的全氢聚硅氮烷。
13.根据权利要求1-12一项或多项的太阳能电池(10)，其特征在于，其对于波长范围为300-900nm的光具有低于97％，优选低于96％，和特别地低于95％的平均相对反射率，以施加包封层(5)之前的太阳能电池(10)的反射率计。
14.根据权利要求1-13一项或多项的太阳能电池(10)，其特征在于，其对于波长范围为1100-1500nm的光具有大于120％，优选大于150％，和特别地大于200％的平均相对反射率，以施加包封层(5)之前的太阳能电池(10)的反射率计。
15.根据权利要求1-14一项或多项的太阳能电池(10)，其特征在于，在根据DIN EN 61646的加速老化试验中在800h后，其具有大于70％，优选大于75％和特别是大于80％的效率，以初始值计。
16.黄铜矿太阳能电池的制备方法，包括步骤：
a)将基于黄铜矿的光伏层状结构施加到任选地配备有阻挡层的基材上，
b)用含有至少一种通式(I)的聚硅氮烷的溶液涂覆光伏层状结构
-(SiR′R″-NR″′)n-(I)
其中R′、R″、R″′相同或不同，并且彼此独立地为氢或任选取代的烷基、芳基、乙烯基或(三烷氧基甲硅烷基)烷基残基，其中n为整数并如此确定n，使得所述聚硅氮烷具有150-150000g/mol，优选50000-150000g/mol，和特别为100000-150000g/mol的数均分子量，
c)通过蒸发去除溶剂，其中，获得厚度为100-3000nm，优选200-2500nm，和特别为300-2000nm的聚硅氮烷层，
d)任选地一次或多次重复步骤b)和c)，
e)通过i)加热到20-1000℃，特别是80-200℃范围内的温度和/或ii)用180-230nm范围内的波长段的紫外线辐照，使所述聚硅氮烷层硬化，其中，所述加热和/或辐照在1min-14h，优选1min-60min和特别是1min-30min期间内进行，优选在由含水蒸气的空气或氮气构成的气氛下，
和
f)任选地，在20-1000℃，优选60-130℃温度下，在相对湿度为60-90％的空气中，在1min-2h，优选30min-1h期间内，对所述聚硅氮烷层进行后硬化。
17.根据权利要求16的方法，其特征在于，所述聚硅氮烷溶液含有至少一种其中R′、R″和R″′＝H的全氢聚硅氮烷。
18.根据权利要求16或17的方法，其特征在于，所述聚硅氮烷溶液含有催化剂，以及任选地其他添加剂。
19.根据权利要求16、17或18的方法，其特征在于，所述黄铜矿太阳能电池在柔性带状基材上以辊对辊方法制成。
20.含有至少一种通式(I)的聚硅氮烷的聚硅氮烷溶液的用途，
-(SiR′R″-NR″′)n-(I)
其中R′、R″、R″′相同或不同，并且彼此独立地为氢或任选取代的烷基、芳基、乙烯基或(三烷氧基甲硅烷基)烷基残基，其中n为整数并如此确定n，使得所述聚硅氮烷具有150-150000g/mol的数均分子量，用于制备铜-铟-硫化物(CIS)或铜-铟-镓-硒化物(CIGSe)型黄铜矿薄膜太阳能电池的包封层。
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| DE102009013904A DE102009013904A1 (de) | 2009-03-19 | 2009-03-19 | Solarzellen mit einer Verkapselungsschicht auf Basis von Polysilazan |
| DE102009013904.4 | 2009-03-19 | ||
| PCT/EP2010/001636 WO2010105796A1 (de) | 2009-03-19 | 2010-03-16 | Solarzellen mit einer verkapselungsschicht auf basis von polysilazan |
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| US9893220B2 (en) * | 2013-10-15 | 2018-02-13 | Nanoco Technologies Ltd. | CIGS nanoparticle ink formulation having a high crack-free limit |
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| CN106661272B (zh) | 2014-07-29 | 2020-01-10 | Az电子材料(卢森堡)责任有限公司 | 用作光电组件中的涂覆试剂的杂化材料 |
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| JP2012521080A (ja) | 2012-09-10 |
| JP5731471B2 (ja) | 2015-06-10 |
| DE102009013904A1 (de) | 2010-09-23 |
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