TW201331338A - Wavelength conversion composition and wavelength conversion film and solar cell - Google Patents
Wavelength conversion composition and wavelength conversion film and solar cell Download PDFInfo
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- TW201331338A TW201331338A TW101137443A TW101137443A TW201331338A TW 201331338 A TW201331338 A TW 201331338A TW 101137443 A TW101137443 A TW 101137443A TW 101137443 A TW101137443 A TW 101137443A TW 201331338 A TW201331338 A TW 201331338A
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Classifications
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10F—INORGANIC SEMICONDUCTOR DEVICES SENSITIVE TO INFRARED RADIATION, LIGHT, ELECTROMAGNETIC RADIATION OF SHORTER WAVELENGTH OR CORPUSCULAR RADIATION
- H10F77/00—Constructional details of devices covered by this subclass
- H10F77/40—Optical elements or arrangements
- H10F77/42—Optical elements or arrangements directly associated or integrated with photovoltaic cells, e.g. light-reflecting means or light-concentrating means
- H10F77/45—Wavelength conversion means, e.g. by using luminescent material, fluorescent concentrators or up-conversion arrangements
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
- H05B33/00—Electroluminescent light sources
- H05B33/12—Light sources with substantially two-dimensional radiating surfaces
- H05B33/14—Light sources with substantially two-dimensional radiating surfaces characterised by the chemical or physical composition or the arrangement of the electroluminescent material, or by the simultaneous addition of the electroluminescent material in or onto the light source
-
- 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
Landscapes
- Photovoltaic Devices (AREA)
- Compositions Of Macromolecular Compounds (AREA)
Abstract
本發明提供一種光透過性優異，且可使吸收之光高效率地轉換成目標波長區域之光的有機系波長轉換組成物。本發明之波長轉換組成物為於基底聚合物中含有結合螢光性分子與自我叢集性分子而成之螢光體所成。該螢光體由於容易形成配向性集合體，且使螢光性分子效率良好地二聚物化而發出準分子(excimer)螢光，故與過去之有機系波長轉換組成物相較，即使螢光體含量為低濃度，亦可高效率地進行波長轉換同時光透過性優異。The present invention provides an organic wavelength conversion composition which is excellent in light transmittance and which can efficiently convert absorbed light into light in a target wavelength region. The wavelength conversion composition of the present invention comprises a phosphor comprising a fluorescent molecule and a self-assembling molecule in a base polymer. Since the phosphor is easy to form an aligning aggregate and dimerizes the fluorescent polymer efficiently, and emits excimer fluorescence, even if it is fluorescent, compared with the conventional organic wavelength conversion composition. The body content is low, and wavelength conversion can be performed efficiently with excellent light transmittance.
Description
本發明係關於可將特定波長域之光波長轉換成目標波長域之波長轉換組成物。 The present invention relates to wavelength converting compositions that convert wavelengths of light in a particular wavelength domain to a target wavelength domain.
太陽光為300~3000nm左右之波長域的混合光。太陽光例用於如太陽電池之光電轉換裝置時，未必所有波長之光均被利用到。具體被利用之光之波長，於結晶矽系太陽電池中波長域為300~1100nm附近，但在非晶矽太陽電池中為400~600nm附近，化合物系太陽電池為400~1300nm附近，相較於結晶矽系太陽電池，短波長區域之光之利用率較小。 The sunlight is a mixed light of a wavelength range of about 300 to 3000 nm. When sunlight is used for a photoelectric conversion device such as a solar cell, light of all wavelengths is not necessarily used. The wavelength of the specifically used light is in the vicinity of the wavelength range of 300 to 1100 nm in the crystalline lanthanide solar cell, but in the vicinity of 400 to 600 nm in the amorphous yttrium solar cell, the compound solar cell is in the vicinity of 400 to 1300 nm, as compared with The crystalline lanthanide solar cell has a low utilization rate of light in a short wavelength region.
為使太陽電池普及之課題之一列舉為轉換效率之提高。尤其是短波長區域之光之利用率小、轉換效率比結晶矽系太陽電池低之非晶系矽系太陽電池或化合物系太陽電池、有機系太陽電池等成為嚴重之課題。解決策略之一為如何利用迄今未被利用到之波長區域(尤其是短波長區域)之光能量。 One of the topics for popularizing solar cells is listed as an increase in conversion efficiency. In particular, an amorphous lanthanide solar cell, a compound solar cell, or an organic solar cell having a low utilization ratio of light in a short-wavelength region and a conversion efficiency lower than that of a crystalline lanthanide solar cell has become a serious problem. One of the solution strategies is how to utilize the light energy of the wavelength region (especially the short wavelength region) that has not been utilized so far.
因此，就能量效率方面而言，要求將迄今尚未被利用到之波長區域(尤其是短波長區域)之光能量轉換成必要波長之光而使用。 Therefore, in terms of energy efficiency, it is required to convert light energy of a wavelength region (especially a short wavelength region) which has not been utilized so far into light of a necessary wavelength.
其方法之一為開發將螢光體分散於透明聚合物中，將短波長區域之光轉換成適於太陽電池之長波長區域之光之 波長轉換薄膜。 One of the methods is to develop a dispersion of a phosphor in a transparent polymer to convert light in a short wavelength region into light suitable for a long wavelength region of a solar cell. Wavelength conversion film.
例如，專利文獻1、2中揭示將利用如Eu之稀土金屬之無機系粒子作為螢光體分散於透明聚合物中之波長轉換薄膜。然而，該波長轉換薄膜，因於透明聚合物中無機系粒子凝聚，而無助於充分之波長轉換，容易產生太陽光透過率低等之問題。且，由於原料使用稀土金屬故而成本變高。 For example, Patent Literatures 1 and 2 disclose a wavelength conversion film in which inorganic particles of a rare earth metal such as Eu are dispersed as a phosphor in a transparent polymer. However, this wavelength conversion film does not contribute to sufficient wavelength conversion due to aggregation of inorganic particles in the transparent polymer, and is liable to cause problems such as low solar transmittance. Moreover, since the raw material uses rare earth metal, the cost becomes high.
另一方面，如專利文獻3、4中，已報導使用有機材料系螢光體作為分散於透明聚合物中之螢光體之例。然而，為了獲得實用之轉換效率有必要在透明聚合物中以高濃度添加有機材料系螢光體，結果有使太陽光透過率降低，能量轉換效率亦降低之問題。且，由於需要高濃度之有機材料系螢光體，故連帶產生波長轉換薄膜本身之透明性或強度降低等之問題。 On the other hand, as disclosed in Patent Documents 3 and 4, an organic material-based phosphor has been reported as an example of a phosphor dispersed in a transparent polymer. However, in order to obtain practical conversion efficiency, it is necessary to add an organic material-based phosphor to a transparent polymer at a high concentration, and as a result, there is a problem that the solar transmittance is lowered and the energy conversion efficiency is also lowered. Further, since a high concentration of the organic material-based phosphor is required, there is a problem that the transparency or strength of the wavelength conversion film itself is lowered.
[專利文獻1]特開2004-134805號公報 [Patent Document 1] JP-A-2004-134805
[專利文獻2]特開平11-345993號公報 [Patent Document 2] Japanese Patent Publication No. 11-345993
[專利文獻3]特開2001-352091號公報 [Patent Document 3] JP-A-2001-352091
[專利文獻4]特開平10-261811號公報 [Patent Document 4] Japanese Patent Publication No. Hei 10-261811
因此，現狀為對於以往之波長轉換薄膜，在光透過性 或波長轉換效率方面仍有改善餘地，上未達到真正普及。因此，使用不含稀土金屬、即使低濃度波長轉換效率亦高之有機系發光體之波長轉換薄膜之開發被寄予期待。 Therefore, the current status is the light transmittance of the conventional wavelength conversion film. There is still room for improvement in terms of wavelength conversion efficiency, which has not reached real popularity. Therefore, development of a wavelength conversion film using an organic light-emitting body which does not contain a rare earth metal and has a high wavelength conversion efficiency is expected.
該狀況下，本發明之目的係提供一種光透過性優異，可將短波長區域之光高效率地轉換成長波長區域之光之波長轉換組成物及使該波長轉化組成物成形而成之波長轉換薄膜。又，本發明之另一目的係提供具備該波長轉換薄膜之太陽電池。 In this case, an object of the present invention is to provide a wavelength conversion composition which is excellent in light transmittance and can efficiently convert light in a short-wavelength region into light in a wavelength region, and wavelength conversion in which the wavelength conversion composition is formed. film. Further, another object of the present invention is to provide a solar cell including the wavelength conversion film.
亦即，本發明係關於以下之發明者。 That is, the present invention relates to the following inventors.
〈1〉一種波長轉換組成物，其為於基底聚合物中含有結合發光性分子與自我叢集性(clustering)分子而成之發光體。 <1> A wavelength conversion composition comprising an illuminant comprising a luminescent molecule and a self-clustering molecule in a base polymer.
〈2〉如前述〈1〉所記載之波長轉換組成物，其中前述發光體為結合螢光性分子與自我叢集性分子而成之螢光體。 The wavelength conversion composition according to the above <1>, wherein the illuminant is a phosphor in which a fluorescent molecule and a self-cluster molecule are combined.
〈3〉如前述〈2〉所記載之波長轉換組成物，其中前述螢光體為在基底聚合物中集合(association)而配向，並生成準分子(excimer)。 <3> The wavelength conversion composition according to the above <2>, wherein the phosphor is aligned in an underlying polymer to form an excimer.
〈4〉如前述〈2〉或〈3〉之波長轉換組成物，其中前述螢光體係在基底聚合物中集合而形成配向性集合體。 <4> The wavelength conversion composition according to the above <2> or <3>, wherein the fluorescent system is aggregated in the base polymer to form an aligning aggregate.
〈5〉如前述〈4〉所記載之波長轉換組成物，其中前述配向性集合體為纖維狀集合體。 The wavelength conversion composition according to the above <4>, wherein the anisotropic aggregate is a fibrous aggregate.
〈6〉如前述〈2〉至〈5〉中任一項所記載之波長轉換組成物，其中相對於前述基底聚合物100質量份，前述螢光體之比例為0.0001質量份以上10質量份以下。 The wavelength conversion composition according to any one of the above aspects, wherein the ratio of the phosphor is 0.0001 part by mass or more and 10 parts by mass or less based on 100 parts by mass of the base polymer. .
〈7〉如前述〈2〉至〈6〉中任一項之波長轉換組成物，其中前述螢光性分子為芘衍生物。 The wavelength conversion composition according to any one of <2> to <6> wherein the fluorescent molecule is an anthracene derivative.
〈8〉如前述〈7〉項所記載之波長轉換組成物，其中前述芘衍生物係由1-芘丁酸及芘-1-胺所組成群組選出之至少一種。 The wavelength conversion composition according to the item <7>, wherein the anthracene derivative is at least one selected from the group consisting of 1-indolebutyric acid and indole-1-amine.
〈9〉如前述〈2〉至〈6〉中任一項所記載之波長轉換組成物，其中前述螢光性分子為蒽衍生物。 The wavelength conversion composition according to any one of <2> to <6> wherein the fluorescent molecule is an anthracene derivative.
〈10〉如前述〈9〉所記載之波長轉換組成物，其中前述蒽衍生物係由9-(4-羥基苯基)蒽、9-(4-胺基苯基)蒽及9,10-二苯基蒽-1-胺所組成群組選出之至少一種。 <10> The wavelength conversion composition according to the above <9>, wherein the anthracene derivative is 9-(4-hydroxyphenyl)anthracene, 9-(4-aminophenyl)anthracene, and 9,10- At least one selected from the group consisting of diphenylindol-1-amine.
〈11〉如前述〈1〉至〈10〉中任一項所記載之波長轉換組成物，其中前述自我叢集性分子係由胺基酸衍生物、多環芳香族衍生物、膽固醇衍生物及糖衍生物選出之一種以上。 The wavelength conversion composition according to any one of the above aspects, wherein the self-clustered molecule is an amino acid derivative, a polycyclic aromatic derivative, a cholesterol derivative, and a sugar. More than one type of derivative is selected.
〈12〉如前述〈1〉至〈10〉中任一項所記載之波長轉換組成物，其中前述自我叢集性分子係由二-十二烷基化麩醯胺酸、二丁基化麩醯胺酸及二-十二烷基化離胺酸選出之一種以上。 The wavelength conversion composition according to any one of <1> to <10> wherein the self-clustered molecular system consists of di-dodecylated branamic acid and dibutylated bran One or more of the amine acid and the di-dodecylated lysine are selected.
〈13〉如前述〈1〉至〈12〉中任一項所記載之波長轉換組成物，其中前述自我叢集性分子具有分散基。 The wavelength conversion composition according to any one of the above aspects, wherein the self-clusters have a dispersion.
〈14〉如前述〈2〉至〈13〉中任一項所記載之波長轉換組成物，其係進而含有結合前述螢光性分子與自我叢集性分子而成之螢光體以外之螢光物質。 The wavelength conversion composition according to any one of the above aspects, further comprising a fluorescent substance other than the fluorescent body in which the fluorescent molecule and the self-clusting molecule are combined. .
〈15〉如前述〈14〉所記載之波長轉換組成物，其中前述螢光物質係吸收結合前述螢光性分子與自我叢集性分子之螢光體發出之光，且於更長波長處發光之螢光物質。 The wavelength conversion composition according to the above <14>, wherein the fluorescent substance absorbs light emitted from a phosphor of the fluorescent molecule and the self-cluster molecule, and emits light at a longer wavelength. Fluorescent material.
〈16〉如前述〈1〉至〈15〉中任一項所記載之波長轉換組成物，其中前述基底聚合物係於可見光區域不具吸收之聚合物。 The wavelength conversion composition according to any one of <1> to <15> wherein the base polymer is a polymer which does not absorb in a visible light region.
〈17〉如前述〈1〉至〈15〉中任一項所記載之波長轉換組成物，其中前述基底聚合物為聚甲基丙烯酸酯或聚苯乙烯。 The wavelength conversion composition according to any one of <1> to <15> wherein the base polymer is polymethacrylate or polystyrene.
〈18〉一種波長轉換薄膜，其係使如前述〈1〉至〈17〉中任一項之波長轉換組成物成形所成。 <18> A wavelength conversion film formed by molding the wavelength conversion composition according to any one of the above <1> to <17>.
〈19〉一種太陽電池，其特徵為具有如前述〈18〉所記載之波長轉換薄膜與光電轉換元件。 <19> A solar cell characterized by having the wavelength conversion film and the photoelectric conversion element according to <18> above.
〈20〉一種太陽電池，其特徵為具有含有如前述〈1〉至〈17〉中任一項之波長轉換組成物之封裝材、及光電轉換元件。 <20> A solar cell comprising a wavelength conversion composition according to any one of the items <1> to <17> above, and a photoelectric conversion element.
依據本發明，提供一種可將目的波長區域以外之低波長之光高效率地轉換成目標波長之波長轉換組成物及該波長轉換薄膜，以及以具備該波長轉換薄膜之以太陽電池為 代表之應用製品。 According to the present invention, there is provided a wavelength conversion composition capable of efficiently converting light of a low wavelength other than a target wavelength region into a target wavelength, and the wavelength conversion film, and a solar cell having the wavelength conversion film Representative application products.
本發明之波長轉換組成物為於基底聚合物中含有結合發光性分子與自我叢集性分子之具有波長轉換能之發光體之組成物。 The wavelength conversion composition of the present invention is a composition containing a light-emitting energy having a wavelength-converting energy in combination with a luminescent molecule and a self-clusting molecule in the base polymer.
本發明中，所謂「波長轉換」意指吸收特定波長帶之光，且發出更長波長帶之光，藉此將吸收光轉換成長波長側之下轉換(down-conversion)型波長轉換。 In the present invention, "wavelength conversion" means absorption of light of a specific wavelength band and emission of light of a longer wavelength band, thereby converting the absorption light into a wavelength-side down-conversion type wavelength conversion.
至於發光性分子列舉為發出螢光之螢光性分子、發出磷光之磷光性分子，較好為具有可藉縮合反應等與自我叢集性分子結合之官能基(胺基、醛基、羧基、羥基等)者。發光性分子較好為藉由形成螢光性分子，尤其是準分子等而發出斯托科斯位移(Stokes shift)(激發極大波長與發光極大波長之差)較大，且量子收率高之螢光之螢光性分子。 The luminescent molecule is exemplified by a fluorescent molecule that emits fluorescence and a phosphorescent molecule that emits phosphorescence, and preferably has a functional group (amine group, aldehyde group, carboxyl group, hydroxyl group) capable of binding to a self-cluster molecule by a condensation reaction or the like. Etc.) The luminescent molecule is preferably a fluorescene molecule, especially an excimer, which emits a Stokes shift (a difference between an excitation maximum wavelength and an illuminating maximum wavelength) and a high quantum yield. Fluorescent molecules of light.
本發明中，所謂「準分子」為激子二聚物，其特徵為在比單體之螢光更於長波長側具有發光區域。又，嚴格而言係將由同種分子兩個所成之二聚物稱之為準分子，由不同分子所成之二聚物稱為激發複合體(exciplex)，但在本發明中並未區別。亦即，本發明中準分子亦相當於使包含不同螢光性分子之螢光體彼此集合，形成激發複合體之情況。 In the present invention, the "excimer" is an exciton dimer characterized by having a light-emitting region on the longer wavelength side than the fluorescence of the monomer. Further, strictly speaking, a dimer formed of two molecules of the same kind is called an excimer, and a dimer formed of a different molecule is called an exciplex, but it is not different in the present invention. That is, in the present invention, the excimer is also equivalent to the case where the phosphors containing different fluorescent molecules are brought together to each other to form an excited complex.
本發明中之螢光性分子較好為具有形成準分子之部位之分子，或者於組合複數種時為形成激發複合體之分子，就與詳述於後之自我叢集性分子之結合性之觀點而言，較好為包含胺基、醛基、羧基、羥基等之該等分子之衍生物。 The fluorescent molecule in the present invention is preferably a molecule having a site in which an excimer is formed, or a combination of a plurality of molecules to form an excited complex, and a combination with a self-clustered molecule as described in detail later. In general, derivatives of such molecules including an amine group, an aldehyde group, a carboxyl group, a hydroxyl group and the like are preferred.
至於該分子列舉為例如芘衍生物、蒽衍生物、萘衍生物、茀衍生物、苝衍生物、蔻(coronene)衍生物、菲衍生物、螢蒽(fluoranthene)衍生物、咔唑衍生物、衍生物、聯三伸苯衍生物、稠四苯衍生物、稠五苯衍生物、茀酮(fluorenone)衍生物、薁衍生物、寡伸苯基伸乙烯基衍生物、寡伸苯基伸乙基衍生物、卟啉(porphyrin)衍生物、菁色素之衍生物等。該等螢光性分子可單獨使用，亦可組合兩種以上使用。 The molecule is exemplified by, for example, an anthracene derivative, an anthracene derivative, a naphthalene derivative, an anthracene derivative, an anthracene derivative, a coronene derivative, a phenanthrene derivative, a fluoranthene derivative, a carbazole derivative, Derivatives, triazine derivatives, condensed tetraphenyl derivatives, condensed pentabenzene derivatives, fluorenone derivatives, anthracene derivatives, oligophenylene vinyl derivatives, oligophenylene derived ethyl derivatives a substance, a porphyrin derivative, a derivative of a cyanine pigment, and the like. These fluorescent molecules may be used singly or in combination of two or more.
該等中以芘衍生物或蒽衍生物較佳。各種太陽電池中，大多於表層使用紫外線吸收劑以防止內部使用之封裝材之劣化，紫外線並未有效利用。芘衍生物、或蒽衍生物之吸收波長處於紫外線區域，且準分子螢光波長於芘衍生物約為400~550nm，於蒽衍生物約為450~600nm，由於難以引起封裝材材料之劣化，且處於後述之太陽電池所使用之光電轉換元件之吸收波長區域，故適用於使用作為各種太陽電池用之波長轉換組成物(波長轉換薄膜)之情況。再者，藉由使用芘衍生物或蒽衍生物作為螢光性分子，亦可期待減少紫外線光吸收劑之利用。 Among these, an anthracene derivative or an anthracene derivative is preferred. In various solar cells, ultraviolet absorbers are often used on the surface layer to prevent deterioration of the package material used internally, and ultraviolet rays are not effectively utilized. The absorption wavelength of the anthracene derivative or the anthracene derivative is in the ultraviolet region, and the excimer fluorescence wavelength is about 400 to 550 nm in the anthracene derivative and about 450 to 600 nm in the anthracene derivative, which is difficult to cause deterioration of the packaging material, and Since it is in the absorption wavelength region of the photoelectric conversion element used in the solar cell described later, it is suitable for use as a wavelength conversion composition (wavelength conversion film) for various solar cells. Further, by using an anthracene derivative or an anthracene derivative as a fluorescent molecule, it is also expected to reduce the use of an ultraviolet light absorber.
芘衍生物可列舉為例如芘羧酸、芘二羧酸、芘丁酸、 甲基芘羧酸、甲氧基芘丁酸、芘甲醛、芘胺、芘二胺、硝基芘胺、芘硫醇、芘二硫醇、苯基芘。更具體而言列舉為1-芘羧酸、1,6-芘二羧酸、1-芘丁酸、6-甲基芘-1-羧酸、6-甲氧基芘-1-丁酸、芘-1-甲醛、芘-1-胺、芘-2-胺、芘-1,6-二胺、6-硝基芘-1-胺、芘-1-硫醇、芘-1,6-二硫醇、2-苯基芘、6-丙基芘-1-丙酸，但並不限於該等。又，該等螢光性分子可單獨亦可組合兩種以上。 The anthracene derivative may, for example, be an anthracene carboxylic acid, a hydrazine dicarboxylic acid Methyl hydrazine carboxylic acid, methoxy amic acid, hydrazine formaldehyde, decylamine, hydrazine diamine, nitroguanamine, hydrazine thiol, decanedithiol, phenyl hydrazine. More specifically, it is 1-indolecarboxylic acid, 1,6-nonanedicarboxylic acid, 1-indolebutyric acid, 6-methylindole-1-carboxylic acid, 6-methoxyindole-1-butyric acid,芘-1-carbaldehyde, indole-1-amine, indole-2-amine, indole-1,6-diamine, 6-nitroindol-1-amine, indole-1-thiol, indole-1,6- Dithiol, 2-phenylindole, 6-propylindole-1-propionic acid, but not limited to these. Further, these fluorescent molecules may be used alone or in combination of two or more.
其中，以芘-1-丁酸、芘-1-胺較佳。 Among them, 芘-1-butyric acid and 芘-1-amine are preferred.
蒽衍生物可列舉為苯基蒽胺、二苯基蒽胺、(羥基苯基)蒽、(羧基苯基)蒽、吡啶基蒽、萘基蒽、(羥基萘基)蒽、(胺基萘基)蒽、蒽氧基乙酸、雙(二羥基苯基)蒽。更具體而言，作為蒽衍生物列舉為9-(4-羥基苯基)蒽、9-(4-胺基苯基)蒽、9,10-二苯基蒽-1-胺、9-(4-羧基苯基)蒽、9-(4-吡啶基)蒽、9-(1-萘基)蒽、9-(1-羥基-4-萘基)蒽、9-(1-胺基-4-萘基)蒽、4-(9-蒽基)苯氧基乙酸、9,10-雙(3,5-二羥基苯基)蒽，但並不限於該等。又，該等螢光性分子可單獨亦可組合兩種以上。 The anthracene derivative may, for example, be phenylguanamine, diphenylguanamine, (hydroxyphenyl)anthracene, (carboxyphenyl)anthracene, pyridylpurine, naphthyl anthracene, (hydroxynaphthyl)anthracene, (amino naphthalene) Base) hydrazine, decyloxyacetic acid, bis(dihydroxyphenyl)fluorene. More specifically, as an anthracene derivative, it is exemplified as 9-(4-hydroxyphenyl)anthracene, 9-(4-aminophenyl)anthracene, 9,10-diphenylindol-1-amine, 9-( 4-carboxyphenyl)anthracene, 9-(4-pyridyl)anthracene, 9-(1-naphthyl)anthracene, 9-(1-hydroxy-4-naphthyl)anthracene, 9-(1-amino- 4-naphthyl)anthracene, 4-(9-fluorenyl)phenoxyacetic acid, 9,10-bis(3,5-dihydroxyphenyl)anthracene, but is not limited thereto. Further, these fluorescent molecules may be used alone or in combination of two or more.
其中，以9-(4-羥基苯基)蒽、9-(4-胺基苯基)蒽、9,10-二苯基蒽-1-胺較佳。 Among them, 9-(4-hydroxyphenyl)anthracene, 9-(4-aminophenyl)anthracene, and 9,10-diphenylindol-1-amine are preferred.
又，本發明中使用之磷光性分子列舉為含有屬於元素週期表之8族、9族或10族之任一種金屬，且顯示磷光發光之錯合物系化合物，列舉為例如銦錯合物、鋨錯合物、稀土類錯合物等之顯示磷光發光之有機金屬錯合物。 Further, the phosphorescent molecule used in the present invention is exemplified by a compound containing a metal belonging to Group 8, Group 9, or Group 10 of the periodic table of the elements and exhibiting phosphorescence, and is exemplified by, for example, an indium complex. An organometallic complex which exhibits phosphorescence, such as a ruthenium complex or a rare earth complex.
成為該等有機金屬錯合物之配位子之有機化合物列舉為例如咔唑衍生物、吡啶衍生物、卟啉衍生物、聯三伸苯衍生物、聯吡啶衍生物、羅莎琳衍生物、蒽衍生物、酞菁衍生物等。 The organic compound which becomes a ligand of the organic metal complex is exemplified by, for example, a carbazole derivative, a pyridine derivative, a porphyrin derivative, a hydrazine derivative, a bipyridine derivative, a Rosalin derivative, and a hydrazine derivative. , phthalocyanine derivatives, and the like.
又，作為磷光性分子，除錯合物化合物以外，亦可使用曙紅(eosin)衍生物、葉綠素(chlorophyll)衍生物、β胡蘿蔔素(carotene)衍生物、環狀嗪衍生物、二苯乙烯(stilbene)衍生物、聯三伸苯衍生物等。 Further, as the phosphorescent molecule, an eosin derivative, a chlorophyll derivative, a carotene derivative, a cyclic azine derivative, or a stilbene may be used in addition to the complex compound. (stilbene) derivatives, triazine derivatives, and the like.
又，所謂「自我叢集性分子」為有自我組織化地集合作用之分子，本發明中意指於成為對象之基底聚合物中可自我組織化之分子。又，一般之自我叢集性分子在適當溶劑中會形成集合體，但在基底聚合物等之含有大量異種成分之溶液中大多為難以形成集合體之情況。本發明中之自我叢集性分子為不僅在溶劑中且在含有基底聚合物之溶液中亦可形成集合體者，於藉由餾除溶劑等予以固化之情況，亦可於固體中維持該集合體。再者，即使為在含基底聚合物之溶液中或融液中未形成集合體之分子，仍可藉由餾除溶劑等而薄膜化(固化)，在構成薄膜之基底聚合物中會自我組織化地集合．配向之分子亦屬於本發明中之自我叢集性分子。 Further, the "self-clustered molecule" is a molecule that self-organizes and aggregates, and the present invention means a molecule that can be self-organized in the target base polymer. Further, a general self-clustered molecule forms an aggregate in a suitable solvent, but in a solution containing a large amount of heterogeneous components such as a base polymer, it is often difficult to form an aggregate. The self-clustering molecule in the present invention is a method in which agglomerates are formed not only in a solvent but also in a solution containing a base polymer, and the mixture is solidified by a solvent or the like, and the aggregate can be maintained in a solid. . Further, even if the molecule of the aggregate is not formed in the solution containing the base polymer or in the melt, it can be thinned (cured) by distilling off a solvent or the like, and self-organized in the base polymer constituting the film. Set. The aligning molecules are also self-clusters in the present invention.
此種自我叢集性分子較好為具有在基底聚合物中促進集合之部位(例如，醯胺鍵、酯鍵、胺基甲酸酯鍵、脲鍵)，且具有用以賦予適度分散性之烴部位之分子。前述烴部位列舉為例如碳數3~40之直鏈烷基、分枝烷基、環 狀烷基。又，前述烴部位亦可在確保與基底聚合物之親和性之範圍內含有雜原子(氧、氮、硫)。 Such a self-cluster molecule preferably has a site that promotes aggregation in the base polymer (for example, a guanamine bond, an ester bond, a urethane bond, a urea bond), and has a hydrocarbon to impart moderate dispersibility. The molecule of the part. The hydrocarbon moiety is exemplified by, for example, a linear alkyl group having 3 to 40 carbon atoms, a branched alkyl group, and a ring. Alkyl group. Further, the hydrocarbon site may contain a hetero atom (oxygen, nitrogen, sulfur) within a range that ensures affinity with the base polymer.
至於此種自我叢集性分子，列舉為例如各種胺基酸衍生物、多環芳香族衍生物、膽固醇衍生物、糖衍生物，較佳之例為麩胺酸二烷基醯胺、或天門冬胺酸二烷酯、離胺酸二烷基醯胺、醯基葡糖胺、烷氧基偶氮苯、二烷氧基蒽等。 As such self-clustering molecules, for example, various amino acid derivatives, polycyclic aromatic derivatives, cholesterol derivatives, sugar derivatives, preferably dimethylamine glutamine or aspartame, are exemplified. Dialkyl acid ester, dialkyl decylamine amide, decyl glucosamine, alkoxy azobenzene, dialkoxy hydrazine, and the like.
較佳之具體例列舉為二-十二烷基化麩醯胺酸、二丁基化麩醯胺酸及二-十二烷基化離胺酸。 Preferred specific examples are di-dodecyl glutamic acid, dibutylated glutamic acid and di-dodecyl lysine.
又，該等自我叢集性分子可單獨使用亦可組合兩種以上。 Further, these self-clusters may be used alone or in combination of two or more.
結合上述發光性分子與自我叢集性分子而成之發光體之製造方法可為任何方法，列舉為例如，使發光性分子與自我叢集性分子溶解於適當溶劑中，於其中添加縮合劑，使發光性分子與自我叢集性分子之各所具有之官能基反應而結合之方法。 The method for producing an illuminant in which the luminescent molecule and the self-cluster molecule are combined may be any method, and for example, a luminescent molecule and a self-clusting molecule are dissolved in a suitable solvent, and a condensing agent is added thereto to cause luminescence. A method in which a sex molecule reacts with a functional group possessed by each self-clustered molecule.
本發明之波長轉換組成物中，較好使用結合上述螢光性分子與自我叢集性分子之螢光體作為基底聚合物中所含之發光體。 In the wavelength conversion composition of the present invention, a phosphor incorporating the above-mentioned fluorescent molecule and self-clusters is preferably used as the illuminant contained in the base polymer.
藉由使用該螢光體，由構成前述螢光體之自我叢集性分子之作用，使前述螢光體於基底聚合物中叢集，故亦使與自我叢集性分子一起構成螢光體之螢光性分子高效率地集合．配向，促進適於波長轉換之準分子之生成，因而提高波長轉換效率。 By using the phosphor, the phosphors are clustered in the base polymer by the action of the self-collecting molecules constituting the phosphor, so that the phosphor of the phosphor is also formed together with the self-clusters. Sexual molecules gather efficiently. The alignment promotes the generation of excimer suitable for wavelength conversion, thereby improving the wavelength conversion efficiency.
另一方面，未與自我叢集性分子結合而僅將螢光性分子分散於基底聚合物中時，二聚物構造之形成變得困難，螢光性分子之濃度無法成為高濃度(10質量%左右)時無法發出實用等級之準分子螢光。因此，不僅成本高，且連帶有薄膜之透明度或薄膜強度等降低之問題。 On the other hand, when the fluorescent molecules are not dispersed in the base polymer, the formation of the dimer structure becomes difficult, and the concentration of the fluorescent molecules cannot be made high (10% by mass). Excimer fluorescence of a practical level cannot be issued when it is left and right. Therefore, not only the cost is high, but also the problem of the transparency of the film or the strength of the film is lowered.
又，在基底聚合物中使螢光性分子集合之方法，有於聚合物側鏈上結合螢光性分子而成之聚合物螢光體，將其含於基底聚合物中之方法。以該方法，在基底聚合物中雖亦可集合某種程度量之螢光性分子，但螢光性分子在前述聚合物螢光體中因立體障礙而無法自由配置，故該螢光性分子難以處於對於激子生成有利之配向狀態。因此，上述聚合物螢光體與本發明之螢光體比較，螢光性分子之準分子之生成概率低。結果，將前述聚合物螢光體添加於基底聚合物時，為了促進準分子之生成，不得不以高濃度使用前述聚合物螢光體，不僅導致成本高、薄膜強度下降，且因凝聚而連帶使透明度降低。 Further, a method of collecting fluorescent molecules in a base polymer is a method in which a polymer phosphor in which a fluorescent molecule is bonded to a polymer side chain is contained in a base polymer. In this method, a certain amount of fluorescent molecules may be collected in the base polymer, but the fluorescent molecules are not freely displaceable in the polymer phosphor due to steric hindrance, so the fluorescent molecules are It is difficult to be in an alignment state favorable for exciton generation. Therefore, the polymer phosphor has a low probability of generating an excimer of a fluorescent molecule as compared with the phosphor of the present invention. As a result, when the polymer phosphor is added to the base polymer, the polymer phosphor has to be used at a high concentration in order to promote the formation of the excimer, which not only causes high cost, decreases film strength, but also causes aggregation due to aggregation. Reduce transparency.
如上述，本發明之波長轉換組成物中之螢光體，相較於不具有自我叢集性部位之螢光體或結合於聚合物側鏈上之螢光體，即使基底聚合物中所含螢光體濃度(亦即，螢光性分子濃度)為低濃度，仍可容易地形成發出準分子螢光之二聚物構造，故可提高波長轉換組成物之波長轉換效率。而且該螢光體，以及該螢光體經配向而集合之配向性集合體本身幾乎不吸收可見光(亦即為透明)，也不會妨礙薄膜整體之光透過性，故可吸收短波長區域之光，發出 於更長波長側之準分子螢光。 As described above, the phosphor in the wavelength conversion composition of the present invention has a firefly contained in the base polymer as compared with a phosphor having no self-collecting portion or a phosphor bonded to the side chain of the polymer. Since the concentration of the light body (that is, the concentration of the fluorescent molecule) is low, the structure of the dimer emitting excimer fluorescence can be easily formed, so that the wavelength conversion efficiency of the wavelength conversion composition can be improved. Further, the phosphor and the alignment assembly in which the phosphors are aligned are hardly absorbing visible light (that is, transparent), and do not interfere with the light transmittance of the entire film, so that the short-wavelength region can be absorbed. Light, issued Excimer fluorescence on the longer wavelength side.
配向性集合體為使結合上述螢光性分子與自我叢集性分子而成之螢光體進行配向且集合者。配向性集合體之形狀較好以使螢光性分子鄰接之方式集合。至於以使螢光性分子鄰接之方式集合之形態列舉為微胞型之球狀集合體、纖維狀集合體等，尤其以纖維狀集合體較佳。若為纖維狀集合體，則其厚度方向之大小變小，不會引起光散射。再者，若為纖維狀集合體，則由於可使螢光性分子幾乎均等地鄰接，故發光之光之波長幾乎為一定故較佳。 The alignment aggregate is a mixture of a phosphor obtained by binding the above-mentioned fluorescent molecule and a self-clustered molecule. The shape of the alignment aggregate is preferably such that the fluorescent molecules are adjacent to each other. The form in which the fluorescent molecules are adjacent to each other is exemplified by a microcell type spherical aggregate, a fibrous aggregate, or the like, and particularly a fibrous aggregate is preferable. When it is a fibrous aggregate, the magnitude of the thickness direction becomes small, and light scattering does not occur. Further, in the case of a fibrous aggregate, since the fluorescent molecules can be almost uniformly adjacent, the wavelength of the light to be emitted is almost constant, which is preferable.
基底聚合物為使結合發光性分子與自我叢集性分子之發光體、尤其是結合螢光性分子與自我叢集性分子而成之螢光體、進而使該螢光體經配向並集合而成之配向性集合體分散用之基材(基質)。 The base polymer is a phosphor obtained by binding an illuminating molecule and an illuminant of a self-clustered molecule, in particular, a fluorescent molecule and a self-clustered molecule, and then aligning and concentrating the phosphor. A substrate (matrix) for dispersing an aggregate assembly.
基底聚合物只要是對於上述發光體中所含之發光性分子之吸收波長、發光波長之光、尤其是螢光性分子之吸收波長、發光波長之光為透明之聚合物即可，基底聚合物較好為在可見光區域中不具有極大吸收波長之聚合物，最好基底聚合物為在可見光區域不具有吸收之聚合物， 至於該種基底聚合物可使用例如聚甲基丙烯酸酯(PMMA)、聚苯乙烯(PS)、聚碳酸酯(PC)、聚對苯二甲酸乙二酯(PET)、聚氯化乙烯(PVC)、聚偏氯化乙烯(PVDC)、乙烯．乙酸乙烯酯共聚物(EVA)、乙烯-乙烯醇(EVOH)、丁醛、維尼綸(vinylon)、聚乙烯吡咯烷酮、聚乙烯醇、環氧樹脂、聚矽氧樹脂、聚醯亞胺 樹脂等。由於基底聚合物中可使用該種廣泛使用之聚合物故為低成本，對於薄膜化不需要特別之基礎技術。 The base polymer may be a polymer which is transparent to the absorption wavelength of the luminescent molecule contained in the illuminant, the light of the illuminating wavelength, especially the absorption wavelength of the luminescent molecule, and the light of the illuminating wavelength. Preferably, the polymer does not have a maximum absorption wavelength in the visible light region, and preferably the base polymer is a polymer which does not have absorption in the visible light region. As such a base polymer, for example, polymethacrylate (PMMA), polystyrene (PS), polycarbonate (PC), polyethylene terephthalate (PET), polyvinyl chloride (PVC) can be used. ), polyvinylidene chloride (PVDC), ethylene. Vinyl acetate copolymer (EVA), ethylene vinyl alcohol (EVOH), butyraldehyde, vinylon, polyvinylpyrrolidone, polyvinyl alcohol, epoxy resin, polyoxyn resin, polyimine Resin, etc. Since such a widely used polymer can be used in the base polymer, it is low in cost, and no special basic technique is required for film formation.
上述聚合物中，聚甲基丙烯酸酯或聚苯乙烯由於上述發光體、螢光體及配向性集合體之分散性高，可以低成本取得在可見光區域中不具有吸收性之透明性高之聚合物故較佳。 Among the above polymers, polymethacrylate or polystyrene has high dispersibility of the above-mentioned illuminant, phosphor and alignment assembly, and it is possible to obtain a polymerization having high transparency without absorption in a visible light region at low cost. The object is better.
本發明之波長轉換組成物相較於以往之含有有機系螢光體之波長轉換組成物，即使基底聚合物中所含發光體(螢光體)為低濃度亦可獲得充分之轉換效率。基底聚合物中所含之發光體(螢光體)之濃度係考慮薄膜等成形品之形狀、厚度，在不喪失作為波長轉換組成物整體之透明性之範圍內予以決定。具體而言，發光性分子為螢光性分子時，通常以螢光體分子換算相對於基底聚合物100質量份，為0.0001質量份以上10質量份以下，為更提高透明度時，為2質量份以下。濃度太高時，作為波長轉換組成物整體之透明性下降，而有使基底聚合物之性質改變等不良影響故較不佳。 The wavelength conversion composition of the present invention can obtain sufficient conversion efficiency even when the illuminant (phosphor) contained in the base polymer has a low concentration as compared with the conventional wavelength conversion composition containing the organic phosphor. The concentration of the illuminant (fluorescent body) contained in the base polymer is determined in consideration of the shape and thickness of the molded article such as a film, without losing the transparency as a whole of the wavelength conversion composition. Specifically, when the luminescent molecule is a fluorescent molecule, it is usually 0.0001 part by mass or more and 10 parts by mass or less based on 100 parts by mass of the base polymer in terms of phosphor molecules, and 2 parts by mass for further improving transparency. the following. When the concentration is too high, the transparency as a whole of the wavelength conversion composition is lowered, and the adverse effect such as the change in the properties of the base polymer is disadvantageous.
本發明之波長轉換組成物之製造方法並無特別限制，列舉為將結合發光性分子(尤其是螢光性分子)與自我叢集性分子之發光體與基底聚合物分散於適當溶劑中之後，餾除溶劑之方法。藉由該方法，本發明之波長轉換組成物可成為薄膜狀或封裝材等之形態。 The method for producing the wavelength conversion composition of the present invention is not particularly limited, and it is exemplified by dispersing a light-emitting molecule (particularly a fluorescent molecule) and a self-clusters molecule and a base polymer in a suitable solvent. The method of removing the solvent. According to this method, the wavelength conversion composition of the present invention can be in the form of a film or a package.
上物發光體(螢光體)就可獲得更均一分散之波長轉換組成物方面而言，上述發光體(螢光體)中之自我叢集 性分子較好具有分散基。該分散基意指用於某種程度提高與基底聚合物之親和性之官能基，意指用以抑制透明性下降或抑制成為光散射原因之凝聚之官能基。 The self-cluster in the above-mentioned illuminant (fluorescent body) in terms of a more uniform dispersion of the wavelength conversion composition of the upper illuminant (fluorescent body) The sex molecule preferably has a dispersing group. The dispersing group means a functional group for improving the affinity with the base polymer to some extent, and means a functional group for suppressing a decrease in transparency or suppressing aggregation which is a cause of light scattering.
因此，依據基底聚合物之種類，分散基之種類亦有不同，但基底聚合物為如上述聚苯乙烯等之廣泛使用之聚合物，疏水性高之聚合物時，較好為烷基、烯基、快基等之脂肪族烴基。又，依據基底聚合物之種類，膽固醇基或全氟鏈亦為「分散基」之候補。 Therefore, depending on the type of the base polymer, the type of the dispersion is different, but the base polymer is a widely used polymer such as the above polystyrene, and when the polymer having high hydrophobicity is preferably an alkyl group or an alkene. An aliphatic hydrocarbon group such as a base or a fast group. Further, depending on the type of the base polymer, the cholesteryl group or the perfluoro chain is also a candidate for the "dispersion group".
脂肪族烴基可為直鏈狀、分枝狀、環狀之任一種，依據基底聚合物之種類，通常選自碳數2~30之中。烷基之具體例列舉為丁基、第二丁基、己基、2-乙基己基、辛基、壬基、癸基、十一烷基、十二烷基、十八烷基等。 The aliphatic hydrocarbon group may be linear, branched or cyclic, and is usually selected from the group consisting of carbon atoms 2 to 30 depending on the type of the base polymer. Specific examples of the alkyl group are butyl, t-butyl, hexyl, 2-ethylhexyl, octyl, nonyl, decyl, undecyl, dodecyl, octadecyl and the like.
該等脂肪族烴基相對於自我叢集性分子可結合1或複數個，於結合複數個時，各可相同亦可不同。 The aliphatic hydrocarbon groups may be bonded to one or a plurality of self-clusters, and may be the same or different when a plurality of combinations are combined.
又，本發明之波長轉換組成物為更提高波長轉換效率，亦可進而含有結合上述螢光性分子與自我叢集性分子之螢光體以外之螢光物質。該螢光物質最好為吸收使上述螢光性分子與自我叢集性分子結合而成之螢光體發出之光，且發出更長波長之光之螢光物質。 Further, the wavelength conversion composition of the present invention may further increase the wavelength conversion efficiency, and may further contain a fluorescent substance other than the phosphor that binds the fluorescent molecule and the self-clusters. Preferably, the fluorescent substance is a fluorescent substance that absorbs light emitted from a phosphor that combines the fluorescent molecules with self-clusters and emits light of a longer wavelength.
至於螢光物質可使用以往習知之螢光物質(包含稀土類元素之複合氧化物等之無機系螢光物質、若丹明(Rhodamine)類、香豆素類等有機系螢光物質)，其種類或含量係考慮結合上述螢光性分子與自我叢集性分子而成之螢光體之種類或量而適當選擇。又，亦可使用(未結 合自我叢集性分子)上述螢光性分子作為有機系之螢光物質。 As the fluorescent material, a conventional fluorescent material (an inorganic fluorescent material such as a composite oxide of a rare earth element, an organic fluorescent substance such as a Rhodamine or a coumarin) can be used. The type or content is appropriately selected in consideration of the kind or amount of the phosphor in which the above-mentioned fluorescent molecule and self-clustered molecule are combined. Also, can also be used (not yet The self-collecting molecule is a fluorescent substance of the above-mentioned fluorescent substance.
結合上述螢光性分子與自我叢集性分子而成之螢光體中之螢光性分子為芘衍生物時，作為吸收該螢光體發出之光，並發出更長波長之光之螢光物質，例示具體例時列舉為蒽、9-苯基蒽、苝、紅螢烯、香豆素6、香豆素153、9,10-二苯基蒽、尼羅紅(Nile Red)等。 When a fluorescent molecule in a phosphor formed by combining the above-mentioned fluorescent molecule and a self-collecting molecule is an anthracene derivative, it is a fluorescent substance that absorbs light emitted from the phosphor and emits light of a longer wavelength. Specific examples are hydrazine, 9-phenylindole, anthracene, erythroprene, coumarin 6, coumarin 153, 9,10-diphenylanthracene, Nile Red, and the like.
本發明之波長轉換薄膜為使本發明之波長轉換組成物成形，成為薄膜狀者。波長轉換薄膜之成形並無特別限制，可藉以往習知之樹脂薄膜成形之方法(例如，吹塑法、簾流法、澆鑄法等)進行。 The wavelength conversion film of the present invention is formed by molding the wavelength conversion composition of the present invention into a film shape. The formation of the wavelength conversion film is not particularly limited, and it can be carried out by a conventional method of forming a resin film (for example, a blow molding method, a curtain flow method, a casting method, or the like).
本發明之波長轉換薄膜之厚度，考慮成為目標之波長轉換效率、透明性、強度等，可根據目標成為任意之厚度。例如，成為太陽電池用之波長轉換薄膜時通常大多為0.1 mm~10mm左右。 The thickness of the wavelength conversion film of the present invention is considered to be a target wavelength conversion efficiency, transparency, strength, and the like, and may be any thickness depending on the target. For example, when it is used as a wavelength conversion film for a solar cell, it is usually about 0.1 mm to 10 mm.
又，本發明之波長轉換薄膜可藉由薄膜之最佳化(材料之選擇或均質化、多層化、變形改善等)而可期待轉換效率之大幅改善。 Further, the wavelength conversion film of the present invention can be expected to greatly improve the conversion efficiency by optimizing the film (material selection, homogenization, multilayering, deformation improvement, etc.).
又，上述本發明之發光體(螢光體)中之自我叢集性分子具有上述分散基時，由於在溶劑中之前述發光體(螢光體)之分散性亦提高，故有可藉塗佈法容易地製造波長轉換薄膜之優點。 Further, when the self-clustered molecule in the illuminant (fluorescent body) of the present invention has the above-described dispersion group, the dispersibility of the illuminant (fluorescent body) in the solvent is also improved, so that it is possible to apply the coating. The method easily manufactures the advantages of the wavelength conversion film.
本發明之波長轉換組成物、波長轉換薄膜由於波長轉換效率高，且不會阻礙基底聚合物之性質，故可適用於利用波長轉換之各種用途中。 Since the wavelength conversion composition and the wavelength conversion film of the present invention have high wavelength conversion efficiency and do not hinder the properties of the base polymer, they can be suitably used in various applications using wavelength conversion.
列舉為例如，應用於太陽光發電產業、農業、照明產業。 For example, it is applied to the solar power generation industry, agriculture, and lighting industry.
至於對太陽光產業之應用列舉為例如具有使本發明之波長轉換組成物形成之波長轉換薄膜與光電轉換元件之太陽電池。該太陽電池為將波長轉換薄膜配置於光電轉換元件之前段，將入射至該波長轉換薄膜之光轉換成適於光電轉換元件之波長並供給至光電轉換元件，藉此提高光電轉換效率。 The application to the solar industry is, for example, a solar cell having a wavelength conversion film and a photoelectric conversion element which form the wavelength conversion composition of the present invention. In the solar cell, the wavelength conversion film is disposed in front of the photoelectric conversion element, and light incident on the wavelength conversion film is converted into a wavelength suitable for the photoelectric conversion element and supplied to the photoelectric conversion element, thereby improving photoelectric conversion efficiency.
使用之波長轉換薄膜係選擇所含有之發光體(螢光體)及基底聚合物之種類、發光體(螢光體)之含量，以能提供適於使用之光電轉換元件之波長之光。又，亦可組合(層合)複數片波長轉換薄膜而使用。 The wavelength conversion film to be used is selected from the types of the illuminant (fluorescent body) and the base polymer contained in the luminescent body (fluorescent body) so as to provide light of a wavelength suitable for the photoelectric conversion element to be used. Further, a plurality of wavelength conversion films may be combined (laminated) and used.
另外，太陽電池中之光電轉換元件有時以封裝材封裝，但若為含本發明之波長轉換組成物之封裝材，則與上述本發明之波長轉換薄膜同樣，可提供轉換成適合光電轉換元件之波長，故可提高光電轉換效率。又，含有本發明之波長轉換組成物之封裝材意指僅以本發明之波長轉換組成物形成之封裝材，以及將本發明之波長轉換組成物添加於其他習知之封裝材材料中而形成之封裝材。 Further, the photoelectric conversion element in the solar cell may be packaged in a package material, but if it is a package material containing the wavelength conversion composition of the present invention, it can be converted into a suitable photoelectric conversion element as in the above-described wavelength conversion film of the present invention. The wavelength is increased, so that the photoelectric conversion efficiency can be improved. Further, the package containing the wavelength conversion composition of the present invention means a package formed only by the wavelength conversion composition of the present invention, and the wavelength conversion composition of the present invention is added to other conventional package materials. Packaging material.
又，亦可組合(層合)含有波長轉換組成物之波長轉換薄膜與含波長轉換組成物之封裝材而使用。 Further, it is also possible to use (lamination) a wavelength conversion film containing a wavelength conversion composition and a package containing a wavelength conversion composition.
本發明之太陽電池中之光電轉換元件可使用太陽電池中使用之習知光電轉換元件，具體而言列舉為單結晶矽、多結晶矽、非晶矽等之矽系光電轉換元件；CIS、CIGS、InGaAs、GaAs、CdTe等化合物系光電轉換元件；色素增感型、有機薄膜型等之有機系光電轉換元件及層合或接合該等而成之複合型光電轉換元件。本發明之太陽電池可藉由含有如上述之本發明波長轉換組成物之波長轉換薄膜或封裝材，將適於光電轉換元件之波長之光供給至光電轉換元件，故對於轉換效率低之非晶矽、化合物系光電轉換元件、有機系光電轉換元件之開展有望。 The photoelectric conversion element in the solar cell of the present invention can use a conventional photoelectric conversion element used in a solar cell, and specifically, a lanthanide photoelectric conversion element such as a single crystal ruthenium, a polycrystalline ruthenium or an amorphous ruthenium; CIS, CIGS; A compound photoelectric conversion element such as InGaAs, GaAs, or CdTe; an organic photoelectric conversion element such as a dye-sensitized type or an organic thin film type; and a composite photoelectric conversion element obtained by laminating or joining the same. The solar cell of the present invention can supply light of a wavelength suitable for a photoelectric conversion element to a photoelectric conversion element by a wavelength conversion film or a package containing the wavelength conversion composition of the present invention as described above, so that the conversion efficiency is low. It is expected that the development of a compound-based photoelectric conversion element and an organic photoelectric conversion element is expected.
至於農業，可使用本發明之波長轉換組成物、波長轉換薄膜作為溫室用之波長轉換材料。本發明之波長轉換組成物由於吸收短波長區域之光能量，故不僅可減輕對植物之傷害，且可轉換成光合成中易於利用之波長。亦即，不僅可作為波長轉換材料，且扮演濾光之角色。 As for agriculture, the wavelength conversion composition of the present invention and a wavelength conversion film can be used as a wavelength conversion material for a greenhouse. Since the wavelength conversion composition of the present invention absorbs light energy in a short-wavelength region, it can not only reduce damage to plants, but can also be converted into a wavelength that is easy to use in photosynthetic synthesis. That is, it can function not only as a wavelength conversion material but also as a filter.
又，作為照明產業，可使用作為LED或有機EL用之波長轉換材料。本發明之波長轉換組成物、波長轉換薄膜由於可吸收發光能量，且發出不同波長之光，故可適當組合發光元件與發光性分子而發出各種波長之光。 Further, as the lighting industry, a wavelength conversion material for LED or organic EL can be used. Since the wavelength conversion composition and the wavelength conversion film of the present invention can absorb luminescence energy and emit light of different wavelengths, the light-emitting element and the luminescent molecule can be appropriately combined to emit light of various wavelengths.
以下，以實施例更詳細說明本發明，但本發明只要不改變其要旨則不限於以下之實施例。 Hereinafter, the present invention will be described in more detail by way of examples, but the invention should not be construed as limited to the examples below.
波長轉換組成物、波長轉換薄膜之製造中使用之化合 物如下。 Combination of wavelength conversion composition and wavelength conversion film used in the manufacture of a wavelength conversion film The objects are as follows.
二-十二烷基化L-麩醯胺酸(合成品)二丁基化L-麩醯胺酸(合成品)二-十二烷基化L-離胺酸(合成品)二-(2-乙基己基)L-麩醯胺酸(合成品)9-(4-胺基苯基)蒽(合成品)9,10-二苯基蒽-1-胺(和成品)9,10-二苯基蒽(東京化成工業股份有限公司)尼羅紅(東京化成工業股份有限公司)1-芘丁酸(東京化成工業股份有限公司)芘-1-胺(東京化成工業股份有限公司)四氫呋喃(Nacalai Tesque股份有限公司)三乙胺(Nacalai Tesque股份有限公司)氰基磷酸二乙酯(和光純藥工業股份公司製造)甲醇(Nacalai Tesque股份有限公司)香豆素153(Aldrich股份有限公司)聚苯乙烯(Aldrich，Mw：~280,000)聚甲基丙烯酸酯(Aldrich，Mw：~120,000)二甲胺基萘(東京化成工業股份有限公司)乙烯-乙酸乙烯酯共聚物(Aldrich股份有限公司)(乙烯60mol%-乙酸乙烯酯40mol%) Di-dodecyl L-glutamic acid (synthetic) dibutylated L-glutamic acid (synthesis) di-dodecyl L-lysine (synthetic) II-( 2-ethylhexyl)L-glutamic acid (synthetic) 9-(4-aminophenyl)anthracene (synthesis) 9,10-diphenylindole-1-amine (and finished product) 9,10 -Diphenyl hydrazine (Tokyo Chemical Industry Co., Ltd.) Nile Red (Tokyo Chemical Industry Co., Ltd.) 1-indole acid (Tokyo Chemical Industry Co., Ltd.) 芘-1-amine (Tokyo Chemical Industry Co., Ltd.) Tetrahydrofuran (Nacalai Tesque Co., Ltd.) Triethylamine (Nacalai Tesque Co., Ltd.) Diethyl cyanophosphate (manufactured by Wako Pure Chemical Industries, Ltd.) Methanol (Nacalai Tesque Co., Ltd.) Coumarin 153 (Aldrich Co., Ltd.) Polystyrene (Aldrich, Mw: ~280,000) polymethacrylate (Aldrich, Mw: ~120,000) dimethylaminonaphthalene (Tokyo Chemical Industry Co., Ltd.) ethylene-vinyl acetate copolymer (Aldrich Co., Ltd.) (Ethylene 60 mol% - vinyl acetate 40 mol%)
1.螢光體之製造方法 1. Method for manufacturing phosphor
藉以下方法合成結合螢光性分子與自我叢集性分子而 成之自我叢集性螢光體(以下稱為「螢光體」)。 Combining the following methods to synthesize fluorescent molecules and self-clusters A self-assembled phosphor (hereinafter referred to as "fluorescent body").
「螢光體-1」 "Fluorescent-1"
使用1-芘丁酸(0.37g)作為螢光性分子，使用二-十二烷基化L-麩醯胺酸(0.60g)作為自我叢集性分子，溶解於四氫呋喃(70mL)中，於冰浴中邊混合邊添加三乙胺(0.32mL)及氰基磷酸二乙酯(0.38mL)。在室溫混合12小時進行反應後，去除溶劑，自甲醇進行再結晶，獲得螢光體-1(0.89g)。 1-芘-butyric acid (0.37 g) was used as a fluorescent molecule, and di-dodecyl L-glutamic acid (0.60 g) was used as a self-collecting molecule, dissolved in tetrahydrofuran (70 mL), and iced. Triethylamine (0.32 mL) and diethyl cyanophosphate (0.38 mL) were added while mixing in a bath. After mixing at room temperature for 12 hours, the solvent was removed and recrystallized from methanol to obtain a phosphor-1 (0.89 g).
針對螢光體-1，以透過型電子顯微鏡進行評價。透過型顯微鏡觀察係將螢光體-1(7.2mg)溶解於苯(20mL)中，澆鑄於銅網上，使用透過型電子顯微鏡(日本電子，JEM-2000X)進行。 For the phosphor-1, evaluation was performed by a transmission electron microscope. In the transmission microscope, phosphor-1 (7.2 mg) was dissolved in benzene (20 mL), cast on a copper mesh, and subjected to transmission electron microscopy (Japan Electronics, JEM-2000X).
螢光體-1之透過型顯微鏡照片示於圖1。螢光體-1形成由奈米纖維所成之纖維狀集合體。又，用以比較所觀察之參考樣品(1-芘丁酸)並未確認到該種由奈米纖維所成之纖維狀集合體之形成。 A transmission micrograph of the phosphor-1 is shown in Fig. 1. Phosphor-1 forms a fibrous aggregate made of nanofibers. Further, the comparison of the observed reference sample (1-indolebutyric acid) did not confirm the formation of the fibrous aggregate formed of the nanofibers.
「螢光體-2」 "Fluorescent-2"
代替二-十二烷基化L-麩醯胺酸，使用二丁基化L-麩醯胺酸(0.5g)作為自我叢集性分子，以與螢光體-1相同之方法獲得螢光體-2。 Instead of di-dodecyl L-glutamic acid, dibutylated L-glutamic acid (0.5 g) was used as a self-clustered molecule, and a phosphor was obtained in the same manner as in the case of phosphor-1. -2.
「螢光體-3」 "Fluorescent-3"
代替1-芘丁酸，使用芘-1-胺(0.2g)作為螢光性分子，且代替二-十二烷基化L-麩醯胺酸，使用二-十二烷基化L-離胺酸(0.6g)作為自我叢集性分子，以與螢光體-1相同之方法獲得螢光體-3。 Instead of 1-indoleic acid, an indole-1-amine (0.2 g) was used as a fluorescent molecule, and instead of di-dodecyl L-glutamic acid, a di-dodecylation L-ion was used. Amino acid (0.6 g) was used as a self-clusting molecule to obtain a phosphor-3 in the same manner as in the phosphor-1.
「螢光體-4」 "Fluorescent-4"
代替二-十二烷基化L-麩醯胺酸，使用二(2-乙基己基)L-麩醯胺酸(0.6g)作為自我叢集性分子，以與螢光體-1相同之方法獲得螢光體-4。 Instead of di-dodecyl L-glutamic acid, bis(2-ethylhexyl)L-glutamic acid (0.6 g) was used as a self-cluster molecule in the same manner as Phosphor-1 Phosphor-4 was obtained.
「螢光體-5」 "Fluorescent-5"
代替1-芘丁酸，使用9-(4-胺基苯基)蒽(0.3g)作為螢光性分子，且代替二-十二烷基化L-麩醯胺酸，使用二-十二烷基化L-離胺酸(0.6g)作為自我叢集性分子，以與螢光體-1相同之方法獲得螢光體-5。 Instead of 1-indoleic acid, 9-(4-aminophenyl)anthracene (0.3 g) was used as a fluorescent molecule, and instead of di-dodecyl L-glutamic acid, two-twelfth was used. Alkyl L-ionic acid (0.6 g) was used as a self-clustered molecule, and a phosphor-5 was obtained in the same manner as in the phosphor-1.
「螢光體-6」 "Fluorescent-6"
代替1-芘丁酸，使用9,10-二苯基蒽-1-胺(0.4g)作為螢光性分子，且代替二-十二烷基化L-麩醯胺酸，使用二-十二烷基化L-離胺酸(0.6g)作為自我叢集性分子，以與螢光體-1相同之方法獲得螢光體-6。 Instead of 1-indoleic acid, 9,10-diphenylindol-1-amine (0.4 g) was used as a fluorescent molecule, and instead of di-dodecyl L-glutamic acid, two-tenth was used. Dialkylated L-lysine (0.6 g) was used as a self-clusting molecule to obtain a phosphor-6 in the same manner as in the phosphor-1.
表1彙整列出合成之螢光體-1~6之螢光性分子與自我叢集性分子。 Table 1 summarizes the fluorescent molecules and self-clusters of synthetic phosphor-1~6.
2.波長轉換薄膜之製造方法 2. Method for manufacturing wavelength conversion film
藉以下製造方法製造波長轉換薄膜。 The wavelength conversion film was produced by the following manufacturing method.
「波長轉換薄膜-1」 "Wavelength Conversion Thin Film-1"
將螢光體-1(1mg)與作為基底聚合物之聚苯乙烯(1g)溶解於苯(20mL)中，在室溫下澆鑄於玻璃基板上，使溶劑蒸發，藉此獲得相對於基底聚合物100質量份，以芘衍生物換算含01質量份螢光體之波長轉換薄膜-1。 Phosphor-1 (1 mg) and polystyrene (1 g) as a base polymer were dissolved in benzene (20 mL), cast on a glass substrate at room temperature, and the solvent was evaporated, thereby obtaining polymerization with respect to the substrate. 100 parts by mass of the wavelength-converting film-1 containing 01 parts by mass of a phosphor in terms of an anthracene derivative.
「波長轉換薄膜-2」 "Wavelength Conversion Film-2"
將螢光體-1(7.2mg)與作為基底聚合物之聚苯乙烯(1g)溶解於苯(20mL)中，在室溫下澆鑄於玻璃基板上，使溶劑蒸發，藉此獲得相對於基底聚合物100質量份，以芘衍生物換算含0.72質量份螢光體之波長轉換薄膜-2。 Phosphor-1 (7.2 mg) and polystyrene (1 g) as a base polymer were dissolved in benzene (20 mL), cast on a glass substrate at room temperature, and the solvent was evaporated, thereby obtaining relative to the substrate. 100 parts by mass of the polymer, the wavelength conversion film-2 containing 0.72 parts by mass of the phosphor in terms of an anthracene derivative.
「波長轉換薄膜-3」 "Wavelength Conversion Film-3"
將螢光體-1(30mg)與作為基底聚合物之聚苯乙烯(1g)溶解於氯仿(20mL)中，在室溫下澆鑄於玻璃基板上，使溶劑蒸發，藉此獲得相對於基底聚合物100質量份，以芘衍生物換算含3.0質量份螢光體之波長轉換薄膜-3。 Phosphor-1 (30 mg) and polystyrene (1 g) as a base polymer were dissolved in chloroform (20 mL), cast on a glass substrate at room temperature, and the solvent was evaporated, thereby obtaining polymerization with respect to the substrate. 100 parts by mass of the wavelength conversion film-3 containing 3.0 parts by mass of a phosphor in terms of an anthracene derivative.
「波長轉換薄膜-4」 "Wavelength Conversion Film-4"
將螢光體-2(3.6mg)與作為基底聚合物之聚甲基丙烯酸酯(1g)溶解於乙酸乙酯(20mL)中，在室溫下澆鑄於玻璃基板上，使溶劑蒸發，藉此獲得相對於基底聚合物100質量份，以芘衍生物換算含0.36質量份螢光體之波長轉換薄膜-4。 Phosphor-2 (3.6 mg) and polymethacrylate (1 g) as a base polymer were dissolved in ethyl acetate (20 mL), and cast on a glass substrate at room temperature to evaporate the solvent. A wavelength conversion film-4 containing 0.36 parts by mass of a phosphor in terms of an anthracene derivative was obtained with respect to 100 parts by mass of the base polymer.
「波長轉換薄膜-5」 "Wavelength Conversion Film-5"
將螢光體-5(5mg)與作為基底聚合物之苯乙烯(1g)溶解於甲苯(20mL)中，在室溫下澆鑄於玻璃基板上，使溶劑蒸發，藉此獲得相對於基底聚合物100質量份，以蒽衍生物換算含0.5質量份螢光體之波長轉換薄膜-5。 Phosphor-5 (5 mg) and styrene (1 g) as a base polymer were dissolved in toluene (20 mL), cast on a glass substrate at room temperature, and the solvent was evaporated, whereby a base polymer was obtained. 100 parts by mass of a wavelength conversion film-5 containing 0.5 part by mass of a phosphor in terms of an anthracene derivative.
「波長轉換薄膜-6」 "Wavelength Conversion Film-6"
將螢光體-1(3.6mg)及二甲胺基萘(1.0mg)與作為基底聚合物之苯乙烯(1g)溶解於苯(20mL)中，在室溫 下澆鑄於玻璃基板上，使溶劑蒸發，藉此獲得波長轉換薄膜-6。 Phosphor-1 (3.6 mg) and dimethylaminonaphthalene (1.0 mg) were dissolved in benzene (20 mL) with styrene (1 g) as a base polymer at room temperature. The lower wavelength is cast on the glass substrate to evaporate the solvent, whereby the wavelength conversion film-6 is obtained.
「波長轉換薄膜-7」 "Wavelength Conversion Film-7"
將螢光體-4(5mg)與作為基底聚合物之苯乙烯(1mg)溶解於甲苯(20mL)中，在室溫下澆鑄於玻璃基板上，使溶劑蒸發，藉此獲得波長轉換薄膜-7。 Phosphor-4 (5 mg) and styrene (1 mg) as a base polymer were dissolved in toluene (20 mL), cast on a glass substrate at room temperature, and the solvent was evaporated, whereby a wavelength conversion film-7 was obtained. .
「波長轉換薄膜-8(比較例)」 "Wavelength Conversion Film-8 (Comparative Example)"
製造含不含自我叢集性分子之螢光體之波長轉換薄膜-8作為比較例。 A wavelength conversion film-8 containing a phosphor containing no self-clusters was produced as a comparative example.
將作為螢光性分子之1-芘丁酸(2.9mg)與作為基底聚合物之聚苯乙烯(1g)溶解於苯(20mL)中，在室溫下澆鑄於玻璃基板上，使溶劑蒸發，藉此獲得波長轉換薄膜-8。 1-fluorenated butyric acid (2.9 mg) as a fluorescent molecule and polystyrene (1 g) as a base polymer were dissolved in benzene (20 mL), and cast on a glass substrate at room temperature to evaporate the solvent. Thereby, the wavelength conversion film-8 was obtained.
「波長轉換薄膜-9」 "Wavelength Conversion Film-9"
將螢光體-1(7.2mg)及9,10-二苯基蒽(1.0mg)，與作為基底聚合物之乙烯-乙酸乙烯酯共聚物(1g)溶解於乙酸乙酯(10mL)中，在室溫下澆鑄於玻璃基板上，使溶劑蒸發，藉此獲得相對於基底聚合物100質量份，以芘衍生物換算含0.72質量份螢光體-1、以9,10-二苯基蒽換算含0.1質量份之波長轉換薄膜-9。 Phosphor-1 (7.2 mg) and 9,10-diphenylanthracene (1.0 mg) were dissolved in ethyl acetate (10 mL) with ethylene-vinyl acetate copolymer (1 g) as a base polymer. It was cast on a glass substrate at room temperature, and the solvent was evaporated, whereby 100 parts by mass of the base polymer was obtained, and 0.72 parts by mass of the phosphor-1 was used in terms of an anthracene derivative, and 9,10-diphenylanthracene was used. 0.1 parts by mass of the wavelength conversion film-9 was converted.
「波長轉換薄膜-10」 "Wavelength Conversion Film-10"
將螢光體-1(7.2mg)及9,10-二苯基蒽(1.0mg)、香豆素153(0.3mg)、尼羅紅(0.12m)，與作為基底聚合物之乙烯-乙酸乙烯酯共聚物(1g)溶解於乙酸乙酯(10mL)中，在室溫下澆鑄於玻璃基板上，使溶劑蒸發，藉此獲得相對於基底聚合物100質量份，以芘衍生物換算含0.72質量份螢光體-1，以9,10-二苯基蒽換算含0.1質量份，以香豆素153換算含003質量份，以尼羅紅換算含0.012質量份之波長轉換薄膜-10。 Phosphor-1 (7.2 mg) and 9,10-diphenylanthracene (1.0 mg), coumarin 153 (0.3 mg), Nile Red (0.12 m), and ethylene-acetic acid as a base polymer The vinyl ester copolymer (1 g) was dissolved in ethyl acetate (10 mL), and cast on a glass substrate at room temperature to evaporate the solvent, thereby obtaining 100 parts by mass relative to the base polymer, and 0.72 in terms of an anthracene derivative. The mass fraction of the phosphor-1 was 0.1 parts by mass in terms of 9,10-diphenylfluorene, and contained 003 parts by mass in terms of coumarin 153, and contained 0.012 parts by mass of the wavelength conversion film-10 in terms of Nile Red.
表2彙整列出波長轉換薄膜-1~10之構成。 Table 2 summarizes the composition of the wavelength conversion film-1~10.
3.評價 3. Evaluation
(1)目視觀察 (1) Visual observation
觀察波長轉換薄膜-1~10後，目視為透明，未見到白濁等。代表例之波長轉換薄膜-2-之照片示於圖2(a)。 After observing the wavelength conversion film -1 to 10, the film was regarded as transparent, and no white turbidity was observed. A photograph of a representative wavelength conversion film-2- is shown in Fig. 2(a).
波長轉換薄膜-1~10經UV照射(波長365nm)後，清楚地確認到薄膜發光。作為代表例，波長轉換薄膜-2之照片示於圖2(b)。 After the wavelength conversion film-1 to 10 was irradiated with UV (wavelength: 365 nm), the film was clearly confirmed to emit light. As a representative example, a photograph of the wavelength conversion film-2 is shown in Fig. 2(b).
(2)螢光光譜之評價 (2) Evaluation of fluorescence spectrum
針對波長轉換薄膜-2、與波長轉換薄膜-8，使用螢光光譜測定裝置(日本分光，FP-6500)進行螢光光譜之評價，結果示於圖3(波長轉換薄膜-2)、圖4(波長轉換薄膜-8)。 For the wavelength conversion film-2 and the wavelength conversion film-8, the fluorescence spectrum was evaluated using a fluorescence spectrometer (Japan Spectroscopic, FP-6500), and the results are shown in Fig. 3 (wavelength conversion film-2), Fig. 4 (wavelength conversion film-8).
如圖3所示，分散有使結合自我叢集性分子的二-十二烷基化L-麩醯胺酸與螢光性分子的1-芘丁酸而成之螢光體1之波長轉換薄膜-2中，獲得以長波長之450nm附近作為最大波峰之螢光光譜。1-芘丁酸本身之螢光光譜(未圖示)之波峰為390nm，故於波長轉換薄膜-2確認到螢光波長轉換到長波長側。 As shown in FIG. 3, a wavelength conversion film of a phosphor 1 in which a di-dodecyl L-glutamic acid and a fluorescent molecule of 1-fluorene-butyric acid are bonded to a self-clustered molecule is dispersed. In -2, a fluorescence spectrum having a maximum peak near 450 nm of a long wavelength was obtained. Since the peak of the fluorescence spectrum (not shown) of 1-butyric acid itself is 390 nm, it was confirmed by the wavelength conversion film-2 that the fluorescence wavelength was converted to the long wavelength side.
另一方面，分散有使未結合自我叢集性分子之1-芘丁酸之波長轉換薄膜-8於接近1-芘丁酸本身之波峰之390nm附近有波峰，未見到螢光波長轉換。 On the other hand, a wavelength conversion film-8 in which 1-butyric acid which is not bonded to a self-clustered molecule is dispersed has a peak near 390 nm which is close to the peak of 1-indoleic acid itself, and no fluorescence wavelength conversion is observed.
用以參考，圖5中顯示波長轉換薄膜-2之發光特性、 太陽光之光譜及非晶矽之吸收帶。可知波長轉換薄膜-2之發光與非晶矽之吸收帶重疊。 For reference, FIG. 5 shows the luminescence characteristics of the wavelength conversion film-2, The spectrum of sunlight and the absorption band of amorphous enamel. It is understood that the light emission of the wavelength conversion film-2 overlaps with the absorption band of the amorphous germanium.
與上述同樣對波長轉換薄膜-9及波長轉換薄膜-10，進行吸收光譜、螢光光譜之評價結果示於圖6(波長轉換薄膜-9)、圖7(波長轉換薄膜-10)。 The results of evaluation of the absorption spectrum and the fluorescence spectrum of the wavelength conversion film-9 and the wavelength conversion film-10 in the same manner as described above are shown in Fig. 6 (wavelength conversion film-9) and Fig. 7 (wavelength conversion film-10).
如圖6所示，波長轉換薄膜-9之螢光光譜中，源自螢光體-1之螢光光譜消失，且在430nm附近觀察到源自二苯基蒽之螢光光譜。此認為是因為引起由螢光體-1朝二苯基蒽之能量移動所致。 As shown in Fig. 6, in the fluorescence spectrum of the wavelength conversion film-9, the fluorescence spectrum derived from the phosphor-1 disappeared, and a fluorescence spectrum derived from diphenylanthracene was observed in the vicinity of 430 nm. This is believed to be caused by the movement of energy from phosphor-1 to diphenylphosphonium.
如圖7所示，波長轉換薄膜-10之螢光光譜中，源自螢光體-1、9,10-二苯基蒽之螢光光譜消失，且在470nm附近觀察到源自香豆素153之螢光光譜、在570nm附近觀察到源自尼羅紅之螢光光譜。此認為是引起能量自螢光體-1經由9,10-二苯基蒽，朝香豆素153、尼羅紅移動所致。 As shown in Fig. 7, in the fluorescence spectrum of the wavelength conversion film-10, the fluorescence spectrum derived from the phosphor-1, 9,10-diphenylfluorene disappeared, and coumarin derived from around 470 nm was observed. A fluorescence spectrum of 153 was observed, and a fluorescence spectrum derived from Nile Red was observed around 570 nm. This is believed to be caused by the movement of energy from phosphor-1 via 9,10-diphenylanthracene to coumarin 153 and Nile Red.
(3)圓二色性(CD)光譜 (3) Circular dichroism (CD) spectrum
圖8中顯示波長轉換薄膜-2之圓二色性(CD)光譜。測定係使用圓二色性(CD)光譜測定裝置(日本分光，J725)進行。 The circular dichroism (CD) spectrum of the wavelength conversion film-2 is shown in FIG. The measurement was carried out using a circular dichroism (CD) spectrometry apparatus (Japan Spectroscopic, J725).
如由圖8所了解，獲得極大之CD強度，且確認波長轉換薄膜-2中所含之結合螢光性分子與自我叢集性分子而成之螢光體在基底聚合物中配向並集合，形成配向性集合體。 As understood from FIG. 8, a very large CD intensity is obtained, and it is confirmed that the phosphors combined with the fluorescent molecules contained in the wavelength conversion film-2 and the self-clustered molecules are aligned and aggregated in the base polymer to form An omnidirectional collection.
(4)作為太陽電池之評價 (4) Evaluation as a solar cell
(試驗1) (Test 1)
進行具備本發明之波長轉換薄膜之非晶矽太陽電池之性能評價。 Performance evaluation of an amorphous germanium solar cell having the wavelength conversion film of the present invention was carried out.
首先，於非晶矽太陽電池YG-B5050(Shenzhen Global Solar Energy Technology Co.,Ltd製造，5×5cm)之表面貼附波長轉換薄膜-2(厚度：0.04mm)，接著，為了抑制光在薄膜表面之散射，而滴加適量之二乙二醇擴及薄膜表面上後，以石英基板覆蓋。 First, a wavelength conversion film-2 (thickness: 0.04 mm) was attached to the surface of an amorphous germanium solar cell YG-B5050 (manufactured by Shenzhen Global Solar Energy Technology Co., Ltd., 5 × 5 cm), and then, in order to suppress light in the film The surface is scattered, and after adding an appropriate amount of diethylene glycol to the surface of the film, it is covered with a quartz substrate.
將所得具備波長轉換薄膜之太陽電池固定在太陽光模擬器(SAN-EI ELECTRIC製造(XES-70S1)，AM 1.5G，100mW/cm2，照射光尺寸7×7cm)，評價轉換效率。 The obtained solar cell having the wavelength conversion film was fixed to a solar simulator (manufactured by SAN-EI ELECTRIC (XES-70S1), AM 1.5G, 100 mW/cm 2 , and an irradiation light size of 7 × 7 cm), and the conversion efficiency was evaluated.
又，作為比較，以與上述相同之方法，製造無薄膜之非晶矽太陽電池、具備不含螢光體之聚苯乙烯薄膜(厚度：0.035mm)之非晶矽太陽電池及具備波長轉換薄膜-8(厚度：0.036mm)之非晶矽太陽電池，且進行轉換效率之評價。 Further, for comparison, a film-free amorphous germanium solar cell, an amorphous germanium solar cell including a phosphor-free polystyrene film (thickness: 0.035 mm), and a wavelength conversion film were produced in the same manner as described above. An amorphous germanium solar cell of -8 (thickness: 0.036 mm) was evaluated for conversion efficiency.
圖9顯示結果。又，圖9中之轉換效率係以無薄膜之非晶矽太陽電池之轉換效率作為基準之相對值。 Figure 9 shows the results. Further, the conversion efficiency in Fig. 9 is a relative value based on the conversion efficiency of a film-free amorphous germanium solar cell.
如圖9所示，具備波長轉換薄膜-2之太陽電池與無薄膜之太陽電池比較，可知轉換效率提高5%以上。且，具備波長轉換薄膜-2之太陽電池與具備含有未與自我叢集性分子結合之螢光體之波長轉換薄膜-8之太陽電池比較，可 知轉換效率提高3.5%以上。 As shown in FIG. 9, the solar cell including the wavelength conversion film-2 was found to have a conversion efficiency of 5% or more as compared with a solar cell without a film. Moreover, the solar cell including the wavelength conversion film-2 can be compared with a solar cell having a wavelength conversion film-8 containing a phosphor that is not combined with a self-cluster molecule. It is known that the conversion efficiency is increased by 3.5% or more.
由該等結果，確認本發明之波長轉換薄膜有助於太陽電池之轉換效率提高。 From these results, it was confirmed that the wavelength conversion film of the present invention contributes to an improvement in conversion efficiency of the solar cell.
(試驗2) (Test 2)
針對波長轉換薄膜-2、波長轉換薄膜-9及波長轉換薄膜-10，以電流測定法進行評價。 The wavelength conversion film-2, the wavelength conversion film-9, and the wavelength conversion film-10 were evaluated by an amperometric method.
首先，將製膜於聚對苯二甲酸乙二酯薄膜上之波長轉換薄膜-2(厚度0.040nm)設置在連接於電流計之市售多結晶矽太陽電池(太陽工房股份有限公司製造，7.0cm2)上，經UV燈(365nm)照射，測定電流值。結果示於圖10中。 First, a wavelength conversion film-2 (thickness: 0.040 nm) formed on a polyethylene terephthalate film was placed on a commercially available polycrystalline germanium solar cell connected to an ammeter (manufactured by Sun Studio Co., Ltd., 7.0). On a cm 2 ), the current value was measured by irradiation with a UV lamp (365 nm). The results are shown in Fig. 10.
與未設置波長轉換薄膜-2之情況相比較，設置波長轉換薄膜-2時太陽電池產生之電流值提高33%(12.3μA→16.4μA)。該結果，認為是多結晶矽太陽電池之分光感度低之365nm的光藉波長轉換薄膜-2而朝長波長側轉換所致。 The current value generated by the solar cell was increased by 33% (12.3 μA → 16.4 μA) when the wavelength conversion film-2 was provided as compared with the case where the wavelength conversion film-2 was not provided. As a result, it is considered that the 365 nm light having a low spectral sensitivity of the polycrystalline germanium solar cell is converted to the long wavelength side by the wavelength conversion film-2.
同樣地針對製膜於聚對苯二甲酸乙二酯上之波長轉換薄膜-9(厚度0.040nm)，以上述電流測定法進行評價。結果示於圖10。 Similarly, the wavelength conversion film-9 (thickness: 0.040 nm) formed on polyethylene terephthalate was evaluated by the above current measurement method. The results are shown in Figure 10.
與未設置波長轉換薄膜-9之情況相比較，設置波長轉換薄膜-9時太陽電池產生之電流值提高96%(12.3μA→23.5μA)。該結果，認為是多結晶矽太陽電池之分光感度低之365nm的光藉波長轉換薄膜-9而朝長波長側轉換所 致。 Compared with the case where the wavelength conversion film-9 is not provided, the current value generated by the solar cell is increased by 96% (12.3 μA → 23.5 μA) when the wavelength conversion film-9 is provided. As a result, it is considered that the 365 nm light having a low spectral sensitivity of the polycrystalline germanium solar cell is converted to the long wavelength side by the wavelength conversion film-9. To.
同樣地針對製膜於聚對苯二甲酸乙二酯上之波長轉換薄膜-10(厚度0.040nm)，以上述電流測定法進行評價。結果示於圖10。 Similarly, the wavelength conversion film-10 (thickness: 0.040 nm) formed on polyethylene terephthalate was evaluated by the above current measurement method. The results are shown in Figure 10.
與未設置波長轉換薄膜-10之情況相比較，設置波長轉換薄膜-10時太陽電池產生之電流值提高78%(12.3μA→21.5μA)。該結果，認為是多結晶矽太陽電池之分光感度低之365nm的光藉波長轉換薄膜-10而轉換到長波長側所致。 The current value generated by the solar cell was increased by 78% (12.3 μA → 21.5 μA) when the wavelength conversion film-10 was provided, as compared with the case where the wavelength conversion film-10 was not provided. As a result, it is considered that the light of 365 nm having a low spectral sensitivity of the polycrystalline germanium solar cell is converted to the long wavelength side by the wavelength conversion film-10.
依據本發明，提供可較好地適用於以太陽電池為代表之應用製品之波長轉換組成物、波長轉換薄膜。本發明之波長轉換組成物及該波長轉換薄膜為未利用如Eu之稀土金屬之有機材料，且對於以往之有機螢光體，為螢光體含量少之有機材料，故具有維持聚合物材料所具有之輕量性及柔軟性，且應用性亦高之優點。 According to the present invention, there is provided a wavelength conversion composition and a wavelength conversion film which can be suitably applied to an application product represented by a solar cell. The wavelength conversion composition of the present invention and the wavelength conversion film are organic materials which do not utilize a rare earth metal such as Eu, and the organic phosphor of the prior art is an organic material having a small amount of phosphor, so that the polymer material is maintained. It has the advantages of light weight and softness, and high applicability.
另外，具備本發明之波長轉換薄膜之太陽電池由於轉換效率大幅提高，故本發明在產業上受到期待。 Further, since the solar cell including the wavelength conversion film of the present invention has a large conversion efficiency, the present invention is expected in the industry.
圖1為螢光體-1之透過型顯微鏡照片。 Fig. 1 is a transmission type microscope photograph of the phosphor-1.
圖2(a)為波長轉換薄膜-2(未照射UV)、(b)波長轉換薄膜-2(照射UV)之照片。 Fig. 2(a) is a photograph of the wavelength conversion film-2 (not irradiated with UV) and (b) the wavelength conversion film-2 (irradiated with UV).
圖3為顯示波長轉換薄膜-2之螢光光譜之圖。 Fig. 3 is a view showing the fluorescence spectrum of the wavelength conversion film-2.
圖4為顯示波長轉換薄膜-8之螢光光譜之圖。 Fig. 4 is a view showing the fluorescence spectrum of the wavelength conversion film-8.
圖5為顯示波長轉換薄膜-2之螢光光譜、太陽光之光譜及非晶矽之分光感度特性之圖。 Fig. 5 is a graph showing the fluorescence spectrum of the wavelength conversion film-2, the spectrum of sunlight, and the spectral sensitivity characteristics of amorphous germanium.
圖6為顯示波長轉換薄膜-9之吸收光譜、螢光光譜之圖。 Fig. 6 is a view showing an absorption spectrum and a fluorescence spectrum of the wavelength conversion film-9.
圖7為顯示波長轉換薄膜-10之吸收光譜、螢光光譜之圖。 Fig. 7 is a view showing an absorption spectrum and a fluorescence spectrum of the wavelength conversion film-10.
圖8為顯示波長轉換薄膜-2之圓二色性(CD)光譜之圖。 Fig. 8 is a graph showing the circular dichroism (CD) spectrum of the wavelength conversion film-2.
圖9為顯示具備波長轉換薄膜之非晶矽太陽電池之轉換效率之圖(波長轉換薄膜-2及波長轉換薄膜-8)。 Fig. 9 is a graph showing the conversion efficiency of an amorphous germanium solar cell having a wavelength conversion film (wavelength conversion film-2 and wavelength conversion film-8).
圖10為顯示具備波長轉換薄膜之非晶矽太陽電池之以電流測定法獲得之評價結果之圖(波長轉換薄膜-2、波長轉換薄膜-9及波長轉換薄膜-10)。 Fig. 10 is a view showing the results of evaluation by current measurement of an amorphous germanium solar cell having a wavelength conversion film (wavelength conversion film-2, wavelength conversion film-9, and wavelength conversion film-10).
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