CN107210329A - 无色发光太阳能集光器,具有扩展到近红外区的吸收的无重金属、基于至少三元硫属化合物的半导体纳米晶体 - Google Patents
无色发光太阳能集光器,具有扩展到近红外区的吸收的无重金属、基于至少三元硫属化合物的半导体纳米晶体 Download PDFInfo
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Classifications
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- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/04—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices
- H01L31/054—Optical elements directly associated or integrated with the PV cell, e.g. light-reflecting means or light-concentrating means
- H01L31/0547—Optical elements directly associated or integrated with the PV cell, e.g. light-reflecting means or light-concentrating means comprising light concentrating means of the reflecting type, e.g. parabolic mirrors, concentrators using total internal reflection
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- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
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- H01L31/04—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices
- H01L31/054—Optical elements directly associated or integrated with the PV cell, e.g. light-reflecting means or light-concentrating means
- H01L31/055—Optical elements directly associated or integrated with the PV cell, e.g. light-reflecting means or light-concentrating means where light is absorbed and re-emitted at a different wavelength by the optical element directly associated or integrated with the PV cell, e.g. by using luminescent material, fluorescent concentrators or up-conversion arrangements
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/0248—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies
- H01L31/0256—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by the material
- H01L31/0264—Inorganic materials
- H01L31/032—Inorganic materials including, apart from doping materials or other impurities, only compounds not provided for in groups H01L31/0272 - H01L31/0312
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/0248—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies
- H01L31/0256—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by the material
- H01L31/0264—Inorganic materials
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- H01L31/0322—Inorganic materials including, apart from doping materials or other impurities, only compounds not provided for in groups H01L31/0272 - H01L31/0312 comprising only AIBIIICVI chalcopyrite compounds, e.g. Cu In Se2, Cu Ga Se2, Cu In Ga Se2
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- H—ELECTRICITY
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- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/0248—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies
- H01L31/0352—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by their shape or by the shapes, relative sizes or disposition of the semiconductor regions
- H01L31/035209—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by their shape or by the shapes, relative sizes or disposition of the semiconductor regions comprising a quantum structures
- H01L31/035218—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by their shape or by the shapes, relative sizes or disposition of the semiconductor regions comprising a quantum structures the quantum structure being quantum dots
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
- Y02E10/52—PV systems with concentrators
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
- Y02E10/541—CuInSe2 material PV cells
Abstract
本发明涉及一种发光太阳能集光器,其包括玻璃或塑性基体,其含有基于IB和IIIA族金属(UIPAC命名中分别为11和16族)和至少一种硫族元素(VIA族,或IUPAC命名中的16族)的至少三元半导体。
Description
本发明涉及根据主权利要求的前序部分的太阳能集光器。
众所周知,发光太阳能集光器(LSC)包含形成集光器本体的玻璃或塑料波导,其涂覆或掺杂有高度发射性的元素或成分(通常称为荧光体)。直射和/或漫反射的太阳光被这些荧光体吸收并在较高波长下再发射。以这种方式产生的发光通过全内反射向波导的边缘传播,并且通过耦合到集光器本体周边的高效光伏电池转换成电能。
更具体地,发光太阳能集光器通常由具有大致片材状或平行六面体形状的本体(即上述波导)构成,其掺杂有有机荧光体或有机金属荧光体。荧光体吸收入射光,并通过荧光或磷光再次发射。发射的光被全内反射引导到波导的边缘,在那里它被沿着波导的侧面定位的光伏电池转换成电。通过适当选择波导中的荧光体的浓度及其光学性质,可提供具有期望的透明度的着色设备,并且可以以容易地结合到建筑体(例如以光伏窗户的形式)中的任何形状。
另外,这些设备或集光器可以通过将来自大面积的光集中在较小的面积上而使所用的光伏电池的数量最小化,从而使得使用非标准的光伏模块在财务上是可行的,否则这将是过度昂贵的。为了生产高效的太阳能集光器,荧光体必须是高度光稳定的,并且在可见光和近红外光谱区具有广泛的吸收光谱,高发光效率以及本征吸收光谱和光发射光谱之间最大的可能能量分离(由“斯托克斯偏移(Stokes shift)”表示)。最后提到的要求是制造大型集光器的基础,其中由给定荧光体发射的光在到达集光器本体的边缘之前必须覆盖较长的距离(其通常但不排它地具有层状或片材状的形状)。
有一种已知的使用有机荧光体的方法,它们是高度发光的,但是相对可光降解。它们的斯托克斯偏移通常是有限的,导致因荧光体所发射的光的再吸收而引起的显著的光损失。
已经尝试通过使用具有大的斯托克斯偏移的有机稀土配合物克服使用有机荧光体的这个缺点,然而,这些元件仅可以使用太阳光谱的一小部分和/或显示出非常低的发光效率。
当使用胶态纳米晶体(QD)作为并入到太阳能集光器的本体或波导中的发射体时,遇到类似的问题。在这种情况下,虽然这些纳米晶体具有高发射效率和大的光吸收系数,但它们通常在吸收光谱和发射光谱之间显示出很大的重叠,导致发射光的高度再吸收。这是构建大型太阳能集光器的障碍,将设备的尺寸限制在几平方厘米。
为了克服这个问题,已经尝试制造核-壳QD,其中核提供发射功能而壳负责吸收太阳辐射。该解决方案证明,对于用涂覆有形成纳米颗粒体积的超过90%的CdS厚壳的CdSe制成的QD,使得可以制造大型太阳能集光器,但是受限于固有限制,该固有限制阻碍了其在实际环境中的使用。这是因为使用的QD具有受限于壳材料(CdS)的能隙的吸收光谱,其落入绿色/黄色光谱区(约520nm)中,从而对最大可实现的效率设定了限制,并且需要集光器设备高度着色。这不可避免地影响了它们在现实世界中在真实建筑环境或其它用途中的可能应用。
此外,这些QD通常使用有毒材料如镉、碲、铅等。由于环保和公共卫生的原因,这可能会阻止其使用。
根据另一个实施方案,通过用过渡金属离子掺杂QD来消除自吸收,该过渡金属离子作为在主体半导体中光产生的激子的间隙内复合中心。
例如,已可使用掺杂有Mn的ZnSe制造具有上述类型QD的太阳能集光器。
然而,像基于核-壳QD的之前策略一样,使用Mn和其它过渡金属的这种掺杂在太阳光谱的覆盖率上也受到相当大的限制,这大大降低了可获得的最大效率。在这种具体情况下,当使用基于掺杂有Mn的ZnSe的QD的设备时,它固有地不可能在高于500nm波长下吸收部分太阳辐射,导致最终设备的高着色,对其效率以及其建筑并入的可能性具有负面影响。
本发明的目的是提供一种发光太阳能集光器(LSC),其是对已知以及已经公开但仍处于设计阶段的解决方案(例如包含核-壳型QD的那些)的改进。
特别地,本发明的一个目的是提供可以具有高效率的太阳能集光器,也就是说具有非常低或至少可忽略的(或甚至零)的由再吸收引起的光学损耗的太阳能集光器。
另一个目的是提供无色的太阳能集光器或设备,换句话说,具有中性色(灰色等级,如同具有中性光密度的普通滤光片)的太阳能集光器或设备,因此不会引入明显的色度失真,因此其可以用作适用于建筑并入的元件,例如光伏窗户,或通常作为窗户或窗玻璃板或者固定结构或移动结构诸如车辆的透明元件。
另一个目的是提供一种具有扩展遍及可见光和近红外区的吸收光谱的太阳能集光器或设备,以便最大化可用于产生电能的太阳光的份数。
另一个目的是生产一种不含重金属(例如但不限于Pb、Cd和Hg)和已知有毒性的其它元素(例如但不限于Te和As)的发光太阳能集光器,因此它可以以环保的方式轻松使用。
通过根据所附权利要求的发光太阳能集光器实现对于本领域技术人员来说显而易见的这些和其它目的。
为了便于理解本发明,仅通过非限制性的例子附上下面的附图,附图中:
图1示出了包含并入胶态纳米颗粒或纳米晶体或QD的聚合物基体的发光太阳能集光器(LSC)的示意图;
图2示出了用于制造图1的设备或集光器的用ZnS层钝化的CISeS QD在405nm的光激发下的吸收光谱(线A)和光致发光光谱(线B)。
图3示出了根据本发明的用于制造构建LSC的电池所用的工序的示意图;
图4示出了与对应的吸收光谱(线C)和分散在甲苯(在设计阶段QD分散于其中的典型溶剂之一)中的相同QD的发射光谱(线D)相比,用ZnS层钝化并用于示例性设备的CISeSQD(其定义如下)在405nm激发下的吸收光谱(线E)和光致发光光谱(线F);
图5示出了当激发点位于与边缘增大的距离“d”时,在LSC的边缘处收集的用ZnS层钝化的CISeS QD的发光光谱。
参考上述附图,发光太阳能集光器或LSC包含由玻璃或塑性材料(plasticmaterial)制成的本体1(其中存在纳米晶体),仅为了描述目的而将这些示出在集光器的本体1中的可清晰识别的元件;这些纳米晶体或纳米颗粒由2表示。在本体1的边缘3,4,5,6处具有用于收集由本体1中存在的QD发射的光辐射(以hν2表示)并将其转换为电的光伏电池7。设备本体上的入射辐射由hν1表示。
LSC的本体1可以由各种材料制成。这些材料的实例可以包括但不限于以下:聚丙烯酸酯和聚甲基丙烯酸甲酯、聚烯烃、聚乙烯基、环氧树脂、聚碳酸酯、聚乙酸酯、聚酰胺、聚氨酯、聚酮、聚酯、聚氰基丙烯酸酯、有机硅、聚二醇、聚酰亚胺、氟化聚合物、聚纤维素和衍生物例如甲基纤维素、羟甲基纤维素、聚嗪和二氧化硅基玻璃。
纳米晶体或纳米颗粒是其尺寸通常小于10-20nm的元件,并且在任何情况下都小于具有相同组成的相应的一体化(monolithic)材料的激子玻尔半径特征,以便表现出量子限制。这些QD可以表现出实际上100%的光致发光效率和可以通过颗粒的尺寸控制来选择的发射光谱,从而允许与包含单结或多结设备的各种类型的太阳能电池的最佳结合。
根据本发明的基本特征,在这里描述的LSC中用作发射体的胶态纳米晶体是由至少三元硫属化物制成的半导体QD,包含:IB族(或IUPAC命名中的第11族)的过渡金属,IIIA族(或IUPAC命名中的第13族)的金属和VIA族(或IUPAC命名中的第16族)的硫族元素。作为非限制性实例,这些半导体可以是CuInS2、AgInS2、CuInSe2或AgInSe2;或者,这些纳米晶体是还包含IIB族(IUPAC命名中的第12族)过渡金属的四元半导体硫属化物,例如作为非限制性实例,CuInZnS2、CuInZnSe2或AgInZnSe2,可能涂覆有合适的有机和/或无机钝化层,如下所述。纳米晶体也可以由上述三元或四元半导体的合金制成(非限制性实例是CuInSeS、AgInSeS、CuInZnSeS和AgInZnSeS)。
作为一般规则,这些QD是包含IB族的过渡金属(IUPAC命名中的第11族),IIIA族的金属(IUPAC命名中的第13族),连同VIA族(IUPAC命名中的第16组)的至少一种硫族元素的三元或四元半导体,具有通式MIMIIIAVI 2类型或MIMIIIAVI 2-xBVI x类型,或MIMIIIMIIAVI 2-xBVI x类型或MIMIIIMIIAVI类型,其中:
MI是IB族(或IUPAC命名中的第11族)的过渡金属,
MIII是IIIA(或IUPAC命名中的第13族)的过渡金属,
MII是IIB(或IUPAC命名中的第12族)的过渡金属,
AVI是VIA族(或IUPAC命名中的第16族)的硫族元素,
BVI是VIA族(或IUPAC命名中的第16族)的硫族元素,
X是元素BVI的原子,
2-x是元素AVI的原子。
与上述的核-壳类型的QD即异质QD相比,它们形成均匀结构,其中光吸收是由于半导体材料的能带-能带跃迁而导致的,而通过半导体能带中的载流子与位于晶格中的能隙内缺陷状态中的相应异号载流子的辐射复合而在比吸收的光波长更高的波长下发生光的发射。因此,发射的光不被QD再吸收,并且在波导中传播到后者的侧面3-6,其中定位一个或多个无机或有机太阳能电池7,这些电池将集中的光转换成电能。
用作均匀结构而不是核-壳异质结构的这种特殊QD的选择使得可以生产具有大尺寸(几十到几百线性厘米)的发光太阳能集光器,其具有有限的由于发射光的再吸收引起的光学损耗。分散在固体基体或本体1中的纳米晶体的浓度决定了集光器或设备的透明程度,使得可以生产适合用作建筑结构如建筑物或移动结构如机动车辆中的光伏窗户的半透明太阳能集光器。作为非限制性实例,在具有ZnS钝化并在970nm发射的CdSeS QD的情况下,可使用相对于由交联聚(甲基丙烯酸月桂酯)和QD组成的组合材料为0.5重量%浓度的QD,以便产生能够吸收入射在LSC上的20%(大约)的阳光的设备。
通过选择总体参数例如试剂的类型和浓度、温度和反应时间,QD的组成和尺寸的选择还可以使得获得在整个可见近红外区扩展的吸收光谱,其使设备的效率最大化并且赋予最终材料(其可以是固体塑性玻璃或适用施加于透明玻璃或塑性结构的膜)灰色渐变的中性着色。
此外,通过以合适的方式选择QD的组成,可以有利地避免重金属(例如镉、铅或汞)或已知有毒性的其它元素(例如碲或砷),从而提供符合环保要求且无害于健康的产品。
因此,由于本发明,不是通过材料的特定纳米结构去耦吸收和光学发射的功能,而是通过使用半导体纳米晶体的本征缺陷状态去耦,如上所述,所述半导体纳米晶体可以是金属如铜和银的三元硫属化物(例如铜或银铟的硫化物或硒化物)或它们的合金(CuInSexS2-x、AgInSexS2-x)或含锌的四元化合物例如CuInZnS2、CuInZnSe2、AgInZnS2,AgInZnSe2和这些合金。吸收和发射功能的这种去耦确保QD不吸收它们的发射(无论选择的尺寸如何),从而可以生产大型设备或集光器。
此外,在这些设备中,可以采用半导体量子化状态中的载流子波函数的量子限制效应,通过纳米晶体的尺寸调制来选择光吸收和发射光谱,并且两者都可以扩展到近红外。这使得可以生产吸收整个可见光谱的材料,从而使最终设备的着色为中性或者灰色或棕色的色调(技术上无色),因此适合在城市环境中使用。
合成参数的适当选择还使得可以调制纳米晶体的尺寸,使得光学吸收在整个可见光谱上扩展并且在近红外上扩展至约1000nm,并且使得发射落在硅太阳能电池的高波长(1100nm)下的工作限度内。这使这些纳米晶体更容易用于所提出的目的,并且与已良好确立的技术诸如硅光伏电池完全兼容。还可以进一步调制这些尺寸以使光吸收进一步扩展到近红外内,使得发射落入非标准太阳能电池,例如基于锗(1800nm)、铟和镓的砷化物(高达3200nm)等的太阳能电池的操作区内。
在根据本发明制造的发光太阳能集光器中,每个QD用作光学天线,其由通过纳米晶体的尺寸可控制的能带-能带光学跃迁而吸收入射在本体1上的光,以便在整个可见光谱上获得连续的吸收光谱。作为这种光吸收的结果,光生载流子以比吸收的光更长的波长在间隙内的缺陷状态被辐射复合。由于这些状态的浓度相对于形成QD的半导体材料的量最小-事实上,它们主要是由于形成QD的元素的亚化学计量或由于晶体基体中的结构缺陷(空穴和/或间隙缺陷)-杂质的光学吸收相对于QD的能带-能带吸收可以忽略不计。由于这个特征,可以产生其中吸收和光发射的功能被去耦的结构,并且因此可以以有限的再吸收传递本征发光。
实施方案的实例如下所示:本发明的第一实施方案通过如下方式提供了可靠(solid)集光器的制造:将纳米晶体分散在聚甲基丙烯酸甲酯/聚(甲基丙烯酸月桂酯)和通过工业过程制备的环氧树脂的塑料基体中,使用称为“模铸”的工艺和/或原位聚合,其保持纳米颗粒的光学性质和发射效率完整。第二个实施方案是基于富含纳米晶体的活性膜的制造,要用作玻璃和/或塑性窗的涂层。
上述两个实施方案提供具有大大降低的自吸收的设备,其能够在整个可见光太阳光谱和近红外中吸收。太阳能集光器在通过再吸收抑制光学损耗方面的性能比现有技术对于在近红外光谱区中操作的设备的性能显著更好。
现在将描述包含上述类型的QD的LSC的特定实施方案。举例来说,让我们考虑具有基于IB-IIIA-VIA 2类型的三元半导体硫属化合物成分的纳米晶体,例如CuInS2(简称为CIS)、CuInSe2(称为CISe)和这些的合金(CuInSexS2-x或CISeS);这些纳米晶体不含重金属,并且可以通过不使用试剂注入和使用便宜前体的高化学效率的方法以大量制造。此外,它们对光吸收的大冲击横截面及其可以光谱扩展到近红外区的吸收,使得它们非常适合于太阳辐射的收集和转换。
上述QD也是具有可以通过尺寸控制而选择的发光光谱的高效发射体,并且通过适当的表面处理或钝化,其光致发光量子效率可以提高到大于80%。这可以由有机分子或具有大能隙的无机材料(例如锌的硫化物或硒化物)或这两种材料的组合的薄外层组成。
在实施例中,使用CISeS纳米晶体,这些纳米晶体受到ZnS薄层的钝化,其进一步涂覆有油酸以形成具有大表面积和降低的再吸收损失的LSC,并扩展了整个可见光谱的覆盖率。CISeS QD的这种钝化使得在其暴露于塑性基体的聚合过程所需的自由基引发剂之后可以保持QD的发射效率以及光谱发射特性。将QD并入交联的聚(甲基丙烯酸月桂酯)基体中产生聚合物片材,其为无色和自主或自支撑的,并且具有优异的光学品质。这种并入不会引起由LSC透射,反射和漫反射的光的任何可检测的色度失真。因此,该片材适合于并入现有结构或新结构中,例如用于形成或生产光伏窗户。
通过使用以这种方式制造的LSC,获得高达入射太阳辐射的3.2%的光功率转换效率,这与目前用大型设备获得的数值相比是高的数值。目前对于具有与本发明相当的尺寸(等于10cm×10cm)的LSC报道的最大值为1.8%,尽管这是通过用反射层涂覆片材的反面(其大大提高了效率)而获得的,但是这使该设备完全不透明,且因此不适合建筑性并入。
分散在常见溶剂如甲苯中的QD的光吸收和光致发光光谱如图2所示,这表明这些QD对高效无色LSC的适用性。吸收光谱(线A)在整个可见光区中扩展并到达近红外,从而确保太阳辐射的最佳利用,其在海平面(sea level)下的形状由线Z(光谱A.M.1.5G)表示。光致发光光谱(线B)以960nm为中心,其吸收实际上可忽略,并且单晶硅太阳能电池的效率最大。事实上,在单晶硅光伏电池(P线)的典型的外部量子效率曲线和发光光谱之间可以看到很好的重叠,其在发光峰达到最大值。
选用聚(甲基丙烯酸月桂酯)(PLMA)基体,因为该聚合物具有防止纳米晶体聚集的长侧链,并且已经成功地用于制造高光学品质的聚合物-QD纳米复合材料。生产过程包括将纳米颗粒初始分散在小体积的甲基丙烯酸月桂酯(LMA)中约3小时以确保单个QD的细分散。然后,将所得混合物与交联剂,例如乙二醇二甲基丙烯酸酯(EGDM)一起加入到一定体积的单体中。特别地,这里使用的QD-LMA和EGDM混合物之间的重量比率为20%:80%(w/w)。还以等于1重量%(w/w)的量添加了例如以商品名Irgacure 651已知的自由基光引发剂。
混合约20分钟后,并在超声波浴中处理整个混合物约10分钟后,通过模铸(典型的光学聚合物片材的制备方法)制备太阳能集光器。如图3所示。特别地,将如上所述制造的均匀混合物倒入由低粗糙度的钢化玻璃制成的模具31中,并用365nm的光辐照(该工序由该图中的箭头32)5分钟,以激活自由基聚合。然后,在黑暗中完成聚合30分钟,然后将波导从模具中取出,沿着周边边缘切割并抛光(该工序由箭头34表示)。
由于最终设备特别大的面积,因此在整个聚合过程(5分钟辐照和休息30分钟)中将样品保持在模具中以防止裂纹的发展。在该工序之后,获得了高光学品质的最终片材状材料35。
对所得材料的光谱测量显示,QD的光学性能完全抵抗暴露于自由基聚合工序。图4显示了如前所述(分别为线E和F)在甲苯溶液中且并入交联的聚(甲基丙烯酸月桂酯)的光聚合基体中的纳米颗粒在405nm激发下的吸收光谱(线C)和光致发光光谱(线D)。基体的吸收光谱示为线G。
图5示出了跨所得片材的厚度测量的吸收光谱(线H)和当集光器从片材的周边边缘(检测器位于此处)之一以增大的距离“d”被激发时测量的光致发光和发光光谱(线L)。以这种方式收集的光致发光光谱显示随着“d”的增大,强度逐渐下降,仅部分地由发光的再吸收而引起,且主要是由于波导的上表面和下表面的光子损失。后一种效应由聚合物化合物的浅和深缺陷的光学扩散引起的,这可以通过改进模铸工艺容易地消除。为了澄清实际上由于自吸收而导致的测量损耗有多少,图5中插图为比较的目的而示出了归一化的光致发光光谱,其形状变化仅取决于QD和聚合物基体本身的吸收(应该注意,基体在相关的光学窗口中只表现出弱的光吸收:参见图5中的线H)。将会注意到,对于长的光学距离“d”(12cm),光谱轮廓的失真是最小的。对结果的这种额外分析表明,如果考虑到先前已知的在近红外区中操作的发光太阳能集光器(使用基于重金属如PbS的纳米颗粒)显示出由小于8cm的光程(“d”)的再吸收引起的约70%的光损耗,则用本文所检验的示例性实施方案中使用的以ZnS钝化的CISeS纳米颗粒所实现的再吸收抑制是特别明显的。
发光太阳能集光器开发的一个重要方面是,它们可以用于获得未着色的基于LSC的光伏窗户;也就是说,它们不具有特定光波长的选择性吸收,从而防止颜色感知的失真和透射阳光的彩色滤光。
通过使用IB-IIIA-VIA 2型的四元半导体QD实现所有这些结果,该四元半导体包含:IB族(或IUPAC命名中的第11族)的过渡金属,IIIA族的金属(或IUPAC命名中的第13族)和VIA族(或IUPAC命名中的第16族)的硫族元素,或它们的合金,或通过使用上述类型的包含锌的四元半导体,例如CuInZnS2、CuInZnSe2或AgInZnS2、AgInZnSe2实现所有这些结果。
由于本发明,因此可以生产具有减少的再吸收损失的发光太阳能集光器,其基于包括在塑性或二氧化硅基玻璃基体中的具有大的斯托克斯偏移(>0.2eV)的胶态纳米晶体。通过使用这些纳米晶体,可克服以前使用有机或QD基的发色团遇到的所有限制,这些限制通常与阳光光谱的部分覆盖相关,并且因此固有地限制了光功率转换效率,以及所产生的太阳能集光器的强烈着色,以及具有大的斯托克斯偏移的QD的组成元素的毒性。
特别地,利用上述实施方案,获得高达3.2%的功率转换效率,这对于具有大表面积(12cm×12cm)的LSC而言是高数值。
此外,根据本发明生产的集光器基本上没有颜色,因此不会引起颜色感知的失真,或引起透射的阳光的任何彩色滤光。
已经描述了本发明的特定实施方案;然而,可以根据前面描述的内容产生其它实施方案,使得认为它们落入所附权利要求的范围内。
Claims (15)
1.太阳能集光器,包含由含有胶态纳米晶体(2)的二氧化硅基玻璃或聚合物材料制成的本体(1),其特征在于,这些纳米晶体是至少三元半导体硫属化物的纳米晶体,其含有:IB族或IUPAC命名第11族的过渡金属,IIIA族或IUPAC命名中的13族的金属,以及至少一种VIA族或IUPAC命名中的第16族的硫族元素。
2.根据权利要求1的太阳能集光器,其特征在于纳米晶体(2)具有根据下式的组成:
MIMIIIAVI 2,其中
MI是IB族或IUPAC命名中的第11族的过渡金属,
MIII是I IIA族或IUPAC命名中的第13族的过渡金属,
AVI是VIA族或IUPAC命名中的第16族的硫族元素。
3.根据权利要求1的太阳能集光器,其特征在于纳米晶体(2)包括所述至少三元半导体的合金。
4.根据权利要求1的太阳能集光器,其特征在于纳米晶体(2)包括四元半导体。
5.根据权利要求4的太阳能集光器,其特征在于纳米晶体具有根据下式的组成:
MIMIIIAVI 2-xBVI x,其中
MI是IB族或IUPAC命名中的第11族的过渡金属,
MIII是I IIA或IUPAC命名中的第13族的过渡金属,
AVI是VIA族或IUPAC命名中的第16族的硫族元素,
BVI是VIA族或IUPAC命名中的第16族的硫族元素,
x是元素BVI的原子,以及
2-x是元素AVI的原子。
6.根据权利要求1所述的太阳能集光器,其特征在于,所述纳米晶体含有金属例如铜、银、锌、铝、铟和镓。
7.根据权利要求4的太阳能集光器,其特征在于纳米晶体具有根据下式的组成:
MIMIIIMIIAVI,其中
MI是IB族或IUPAC命名中的第11族的过渡金属,
MIII是IIIA或IUPAC命名中的第13族的过渡金属,
MII是过渡金属,以及
AVI是VIA族或IUPAC命名中的第16族的硫族元素。
8.根据权利要求4的太阳能集光器,其特征在于纳米晶体具有根据下式的组成:
MIMIIIAVI 2-xBVI x,其中
MI是IB族或IUPAC命名中的第11族的过渡金属,
MIII是IIIA或IUPAC命名中的第13族的过渡金属,
MII是过渡金属,
AVI是VIA族或IUPAC命名中的第16族的硫族元素,
BVI是VIA族或IUPAC命名中的第16族的硫族元素,
x是元素BVI的原子,以及
2-x是元素AVI的原子。
9.根据权利要求1的太阳能集光器,其特征在于纳米晶体不含重金属。
10.根据权利要求1的太阳能集光器,其特征在于纳米晶体具有大于0.2eV的大的斯托克斯偏移。
11.根据权利要求1的太阳能集光器,其特征在于塑性本体是聚合物或二氧化硅基玻璃基体。
12.根据权利要求9的太阳能集光器,其特征在于该基体包含以下聚合物中的至少一种:聚丙烯酸酯和聚甲基丙烯酸甲酯、聚烯烃、聚乙烯基、环氧树脂、聚碳酸酯、聚乙酸酯、聚酰胺、聚氨酯、聚酮、聚酯、聚氰基丙烯酸酯、有机硅、聚二醇、聚酰亚胺、氟化聚合物、聚纤维素和衍生物例如甲基纤维素、羟甲基纤维素、聚嗪和二氧化硅基玻璃。
13.根据权利要求1的太阳能集光器,其特征在于它具有片材状构造,其中纳米基体分散在塑性或二氧化硅基玻璃的基体中。
14.根据权利要求1的太阳能集光器,其特征在于它具有膜状构造。
15.用于建筑物或用于移动结构的窗户,包含通过使用根据权利要求1的发光太阳能集光器制成的至少一个部件。
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