KR101195761B1 - Manufacturing method of dye-sensitizes solar cell with cnt and pt counter electrodes - Google Patents
Manufacturing method of dye-sensitizes solar cell with cnt and pt counter electrodes Download PDFInfo
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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
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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
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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- Y02E10/542—Dye sensitized solar cells
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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
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Abstract
Description
본 발명은 염료감응형 태양전지 제조방법에 관한 것으로, 보다 상세하게는 불용성의 탄소나노튜브(CNT: Carbon Nano Tube, 이하 'CNT' 라 함)를 질산용액을 이용하여 산처리한 후 염료감응형 태양전지(DSSC: Dye-Sensitized Solar Cell) 상대전극으로서 투명 CNT를 코팅ㆍ증착하고 그 위에 백금(Pt: Platinum, 이하 'Pt' 라 함)을 코팅하여 사용하는 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법에 관한 것이다.
The present invention relates to a dye-sensitized solar cell manufacturing method, and more specifically, dye-sensitized after insoluble carbon nanotubes (CNT: Carbon Nano Tube, hereinafter referred to as 'CNT') by acid treatment using a nitric acid solution Dye-Sensitized Solar Cell (DSSC) counter electrode is equipped with CNT / Pt composite counter electrode which is coated and deposited with transparent CNT and coated with platinum (Pt: Platinum). It relates to a dye-sensitized solar cell manufacturing method.
현대 사회는 지난 반세기 이상동안 화석연료의 과도한 소비로 인하여 온실효과, 환경오염 등 심각한 지구 환경 문제와 급격한 자원 고갈 문제에 직면해 있다. 이러한 문제를 극복하고자 전세계의 유수(有數)의 연구자들은 태양광, 태양열, 풍력, 수소 에너지와 같은 재생가능하고 청정한 에너지를 개발하기 위해 노력하고 있다. 그 중에서 태양광 에너지는 지구로 연간 약 1×1018 kWh 에너지를 방사하는 무한한 잠재력을 가진 에너지원으로서, 차세대 에너지원으로 각광을 받고 있어 전세계 각국에서 다양한 태양전지를 이용하여 빛을 전기에너지로 변환시키려는 노력이 시도되어 왔다.Modern society has faced severe global environmental problems such as greenhouse effect and environmental pollution and rapid resource depletion due to excessive consumption of fossil fuels for more than half a century. To overcome this problem, leading researchers around the world are working to develop renewable and clean energy such as solar, solar, wind and hydrogen. Among them, solar energy is an energy source with infinite potential to emit about 1 × 10 18 kWh of energy per year to the earth, and it is attracting attention as the next generation energy source, and converts light into electric energy using various solar cells in various countries around the world. Efforts have been made.
현재 전반적으로 상용화되어 있는 태양전지는 태양전지의 약 74%를 차지하고 있는 결정질 실리콘 태양전지로, 광전효율이 15~20% 정도로 우수하나, 고가의 제조단가 및 사용후 재료의 독성배출 등으로 많은 문제점을 내포하고 있으며, 동시에 제조공정에 있어 대형의 반도체공정의 고가의 장비를 사용해야하고 원료가격의 부담 등으로 인하여 태양전지의 상업화에 그 한계성을 보이고 있다. 이러한 태양전지의 한계성을 극복하기 위해 차세대 태양전지로서 염료감응형 태양전지(DSSC: Dye-Sensitized Solar Cell)가 주목되고 있다.Currently, the commercially available solar cell is a crystalline silicon solar cell which occupies about 74% of the solar cell. The photovoltaic efficiency is excellent at about 15-20%, but there are many problems due to expensive manufacturing cost and toxic emission of used materials. At the same time, the expensive equipment of large-scale semiconductor process must be used in the manufacturing process, and due to the burden of raw material price, the commercialization of solar cell has been limited. Dye-Sensitized Solar Cells (DSSCs) are attracting attention as next-generation solar cells to overcome the limitations of such solar cells.
이하, 도 1은 종래의 염료감응형 태양전지의 일반적 구조를 개략적으로 보여주는 도면이다.1 is a view schematically showing a general structure of a conventional dye-sensitized solar cell.
도 1에 도시한 바와 같이, 염료감응형 태양전지는 전면 전극기판(10), 차단층(20), 염료/티타니아층(30), 전해질(40),상대 전극기판(50)을 포함한다.As shown in FIG. 1, the dye-sensitized solar cell includes a
여기서,전면 전극기판(10)은 유리 또는 플라스틱 기판(11) 상에 투명전도성막(13)이 형성된 구조를 갖는다.Here, the
또한, 차단층(20)은 전면 전극기판(10)과 염료/티타니아층(30) 간의 접착력 향상의 역할과, 전해질(40)이 전면 전극기판(10)에 직접 닿는 것을 차단하는 역할을 수행하여 단로방지에 의한 효율 향상의 효과를 가져온다. 또한, 에너지 준위의 균형화로 전자와 정공의 재결합을 방지하여 전자의 수집율이 좋아져 효율 개선 효과가 있다. 차단층(20)으로서, TiO2를 형성할 수도 있고, TiO2-WO3 또는 WO3를 형성할 수도 있다. 또한, 상대 전극기판(50)은 유리 또는 플라스틱 기판(51) 상에 투명전도성막(53)과 Pt 또는 탄소 필름(55)이 순차적으로 형성된 구조를 갖는다.In addition, the
이러한 종래의 염료감응형 태양전지에서는 전면 전극과 상대 전극에 모두 불소가 도핑된 산화주석막(FTO: Flourine Tin Oxide 막)을 사용하는 것이 대부분이었다.In such a conventional dye-sensitized solar cell, a fluorine-doped tin oxide film (FTO: Flourine Tin Oxide film) was mostly used for both the front electrode and the counter electrode.
태양전지용으로 사용되는 투명전도성막은 빛을 잘 투과하는 성질(투과율)과 전자를 잘 흐르게 할 수 있는 특성(전기전도도)이 우수할 것이 요구된다. 그러나, 기존엔 CNT 기판을 가지고 적용한 사례가 없으므로 새로운 태양전지 개념으로 도입하려고 한다.
Transparent conductive films used for solar cells are required to be excellent in the property of transmitting light well (transmittance) and the characteristics of good electron flow (electrical conductivity). However, there is no case of applying the CNT substrate in the past, so it will be introduced as a new solar cell concept.
따라서 본 발명의 목적은 상기와 같은 문제를 해결하기 위해, 불용성의 CNT를 질산용액을 이용하여 산처리한 후 염료감응형 태양전지 상대전극으로서 투명 CNT를 코팅ㆍ증착하고 그 위에 Pt을 코팅하여 사용함으로써, 제조공정이 단순한 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법을 제공하는 것이다.Accordingly, an object of the present invention is to solve the above problems, insoluble CNT acid treatment using a nitric acid solution, and then coated and deposited transparent CNT as a dye-sensitized solar cell counter electrode, and then coated with Pt thereon. Accordingly, the present invention provides a method for manufacturing a dye-sensitized solar cell having a simple CNT / Pt composite counter electrode.
또한 본 발명의 다른 목적은 균일 CNT 투명 페이스트, 탄소 계열 박막 및 그래핀 요소를 포함하여 이용함으로써 전극의 열화 가능성이 있는 염료감응형 태양전지의 신뢰도를 향상시킴과 동시에 다양한 기판에 전극을 형성시킬 수 있는 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법을 제공하는 것이다.In addition, another object of the present invention is to include a uniform CNT transparent paste, a carbon-based thin film and a graphene element to improve the reliability of the dye-sensitized solar cell that may deteriorate the electrode and at the same time to form the electrode on a variety of substrates It is to provide a dye-sensitized solar cell manufacturing method having a CNT / Pt composite counter electrode.
또한 본 발명의 다른 목적은 아세트산을 에탄올에 용해시후, TiO2 분말을 넣고 혼합하여 제조된 TiO2 페이스트를 이용하여, 전면 전극기판 상에 적절한 두께의 차단층을 형성하여, 광투과율과 효율을 증가시키는 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법을 제공하는 것이다.
Another object of the present invention is to dissolve acetic acid in ethanol, TiO 2 TiO 2 prepared by mixing the powder The present invention provides a method for manufacturing a dye-sensitized solar cell having a CNT / Pt composite counter electrode which increases light transmittance and efficiency by forming a blocking layer having an appropriate thickness on a front electrode substrate using a paste.
본 발명에 따른 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법은 아세트산을 에탄올에 용해시킨후, TiO2 분말을 넣고 혼합하여, TiO2 페이스트를 제조하는 단계; 1~20wt% : 1~40wt% : 98~40wt%의 비율로 바인더, 단일벽CNT, 용매를 준비하는 단계; 상기 바인더를 상기 용매에 녹여 분산용액을 만든 후, 상기 분산용액에 상기 단일벽CNT를 혼합하여 단일벽CNT 페이스트를 만드는 단계; 상기 TiO2 페이스트로 형성된 투명전도성막을 상대전극용 기판 위에 코팅하고, 그 위에 상기 단일벽CNT 페이스트를 코팅하고, 그 위에 Pt를 코팅하여 상대전극을 제조하는 단계; 및 상기 상대전극을 상온에서 600℃까지의 범위에서 소성시켜 단일벽CNT 전극막을 제조하는 상대전극 열처리 단계를 포함하는 것을 특징으로 한다.
Dye-sensitized solar cell manufacturing method having a CNT / Pt composite counter electrode according to the present invention after dissolving acetic acid in ethanol, TiO 2 Add powder and mix, TiO 2 Preparing a paste; Preparing a binder, a single wall CNT, and a solvent at a ratio of 1 to 20 wt%: 1 to 40 wt%: 98 to 40 wt%; Dissolving the binder in the solvent to form a dispersion solution, and then mixing the single wall CNT with the dispersion solution to form a single wall CNT paste; The TiO 2 Coating a transparent conductive film formed of a paste on a counter electrode substrate, coating the single-wall CNT paste thereon, and coating Pt thereon to prepare a counter electrode; And a counter electrode heat treatment step of manufacturing the single-wall CNT electrode film by firing the counter electrode at room temperature up to 600 ° C.
상술한 바와 같이, 본 발명에 따른 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법은 제조공정이 단순하고, 균일 CNT 투명 페이스트, 탄소 계열 박막 및 그래핀 요소를 포함하여 이용함으로써 전극의 열화 가능성이 있는 염료감응형 태양전지의 신뢰도를 향상시킴과 동시에 다양한 기판에 전극을 형성시킬 수 있다는 이점이 있다.
As described above, the dye-sensitized solar cell manufacturing method having a CNT / Pt composite counter electrode according to the present invention has a simple manufacturing process, and includes an electrode by using a uniform CNT transparent paste, a carbon-based thin film, and graphene elements. In addition, it is possible to improve the reliability of the dye-sensitized solar cell which may deteriorate and to form electrodes on various substrates.
도 1은 종래의 염료감응형 태양전지의 일반적 구조의 개략도.
도 2는 본 발명에 따른 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법의 일 실시 예를 설명하는 흐름도.
도 3은 본 발명에 따른 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지의 상대전극을 포함하는 태양전지의 개념도.
도 4a 내지 4d는 TiO2 나노 분말층의 두께에 따른 염료감응형 태양전지의 박막의 표면 및 단면을 나타낸 SEM 사진.
도 5은 TiO2 나노 분말층의 두께에 따른 염료감응형 태양전지의 박막의 특성의 변화 및 UV 투과율 측정 그래프.1 is a schematic diagram of a general structure of a conventional dye-sensitized solar cell.
Figure 2 is a flow chart illustrating an embodiment of a dye-sensitized solar cell manufacturing method having a CNT / Pt composite counter electrode according to the present invention.
3 is a conceptual diagram of a solar cell including a counter electrode of a dye-sensitized solar cell having a CNT / Pt composite counter electrode according to the present invention.
4A-4D shows TiO 2 Dye-Sensitized Solar Cell According to the Thickness of Nano Powder Layer SEM photograph showing the surface and cross section of the thin film.
5 is TiO 2 Dye-Sensitized Solar Cell According to the Thickness of Nano Powder Layer Graph of changes in properties and UV transmittance of thin films.
이하, 도면을 참조하면서 본 발명에 따른 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법을 보다 상세히 기술하기로 한다. 본 발명을 설명함에 있어서 관련된 공지기술 또는 구성에 대한 구체적인 설명이 본 발명의 요지를 불필요하게 흐릴 수 있다고 판단되는 경우에는 그 상세한 설명은 생략될 것이다. 그리고, 후술되는 용어들은 본 발명에서의 기능을 고려하여 정의된 용어들로서 이는 클라이언트나 운용자, 사용자의 의도 또는 관례 등에 따라 달라질 수 있다. 그러므로 정의는 본 명세서 전반에 걸친 내용을 토대로 내려져야 할 것이다.Hereinafter, a dye-sensitized solar cell manufacturing method having a CNT / Pt composite counter electrode according to the present invention will be described in detail with reference to the drawings. In the following description of the present invention, a detailed description of known functions and configurations incorporated herein will be omitted when it may make the subject matter of the present invention rather unclear. In addition, terms to be described below are terms defined in consideration of functions in the present invention, which may vary according to a client's or operator's intention or custom. Therefore, the definition should be based on the contents throughout this specification.
도면 전체에 걸쳐 같은 참조번호는 같은 구성 요소를 가리킨다.Like numbers refer to like elements throughout the drawings.
도 2는 본 발명에 따른 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법의 일 실시 예를 설명하는 흐름도이며, 도 3은 본 발명에 따른 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지의 상대전극을 포함하는 태양전지의 개념도이며, 도 4a 내지 4d는 TiO2 나노 분말층의 두께에 따른 염료감응형 태양전지의 박막의 표면 및 단면을 나타낸 SEM 사진이며, 도 5은 TiO2 나노 분말층의 두께에 따른 특성의 변화 및 UV 측정 그래프이다.2 is a flowchart illustrating an embodiment of a method for manufacturing a dye-sensitized solar cell having a CNT / Pt composite counter electrode according to the present invention, and FIG. 3 is a dye having a CNT / Pt composite counter electrode according to the present invention. A conceptual diagram of a solar cell including a counter electrode of a sensitive solar cell, and FIGS. 4A to 4D are TiO 2. Dye-Sensitized Solar Cell According to the Thickness of Nano Powder Layer SEM image showing the surface and cross section of the thin film, Figure 5 is TiO 2 It is a graph of change of properties and UV measurement according to the thickness of the nanopowder layer.
본 발명에 따른 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법의 일 실시 예를 설명하는 흐름도인 도 2에 도시된 바와 같이, 본 발명에 따른 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법은 TiO2 페이스트 제조단계(S201), 용매, 바인더, 탄소나노튜브를 준비하는 단계(S202), 탄소나노튜브 페이스트 제조단계(S203), 상대전극 제조단계(S204), 상대전극 열처리 단계(S205)로 구성된다.As shown in FIG. 2, which is a flowchart illustrating an embodiment of a dye-sensitized solar cell manufacturing method including a CNT / Pt composite counter electrode according to the present invention, the CNT / Pt composite counter electrode according to the present invention is provided. Dye-sensitized solar cell manufacturing method is TiO 2 Paste manufacturing step (S201), solvent, binder, preparing carbon nanotubes (S202), carbon nanotube paste manufacturing step (S203), counter electrode manufacturing step (S204), counter electrode heat treatment step (S205). .
여기서, 용매로는 에틸알콜, 메틸알콜, 이소프로필 알코올 등과 같은 알코올류, 아세톤, 메틸에틸케톤, 에틸 이소케톤 등과 같은 케톤류, 에틸렌글리콜류, 아닐린류, 톨루엔, 클로로포름 등 중에서 선택되는 하나 또는 2개 이상의 용액을 사용하며, 탄소나노튜브의 분산이 용이한 에틸알콜을 사용하는 것이 바람직하다.Here, the solvent is one or two selected from alcohols such as ethyl alcohol, methyl alcohol, isopropyl alcohol, ketones such as acetone, methyl ethyl ketone, ethyl isoketone, ethylene glycol, aniline, toluene, chloroform and the like. Using the above solution, it is preferable to use ethyl alcohol which is easy to disperse carbon nanotubes.
또한 탄소나노투브 페이스트는 닥터블레이드법(doctorblade), 스크린프린팅법(screenprinting), 롤프린팅법(roll printing), 스프레이법(spray), 스핀코팅법(spincoating), 딥핑법(dipping) 중의 어느 하나의 방법에 의해 상기 기판 위에 코팅되나 스핀코팅법을 사용하는 것이 바람직하다.In addition, the carbon nanotube paste is any one of doctorblade, screenprinting, roll printing, spray, spincoating, and dipping. It is coated on the substrate by the method, but it is preferable to use the spin coating method.
또한, 바인더로는 탄소나노튜브의 분산성 및 결합력을 향상시킬 수 있는 폴리비닐부티랄이 사용하는 것이 바람직하다.In addition, as the binder, polyvinyl butyral, which can improve dispersibility and bonding strength of carbon nanotubes, is preferably used.
또한, CNT는 단일벽CNT, 이중벽CNT, 다중벽CNT 등이 사용되며, 단일벽CNT가 사용되는 것이 바람직하다.In addition, as the CNT, a single wall CNT, a double wall CNT, a multi wall CNT, or the like is used, and a single wall CNT is preferably used.
또한, 상대전극용 기판은 도전성이 없는 유리기판, 투명전도막이 코팅되어 있는 FTO 또는 ITO 와 같은 전도성 기판, 전도성 플라스틱, 알루미나기판, 마그네시아 등과 같은 세라믹기판을 포함하는 절연성 기판 등의 모든 기판을 사용할 수 있다.In addition, the counter electrode substrate may be any substrate, such as a non-conductive glass substrate, a conductive substrate such as FTO or ITO coated with a transparent conductive film, and an insulating substrate including a ceramic substrate such as a conductive plastic, an alumina substrate, and magnesia. have.
또한 본 발명에 따른 염료감응형 태양전지용 CNT/Pt 복합체를 이용한 태양전지의 상대전극은 아세트산을 에탄올에 용해시킨후, TiO2 분말을 넣고 혼합하여, TiO2 페이스트를 제조하는 단계(S201); 1~20wt% : 1~40wt% : 98~40wt%의 비율로 바인더, 단일벽CNT, 용매를 준비하는 단계(S202)와; 상기 바인더를 상기 용매에 녹여 분산용액을 제조한 후, 상기 분산용액에 상기 단일벽CNT를 혼합하여 단일벽CNT 페이스트를 만드는 단계(S203); 상기 단일벽CNT 페이스트를 상대전극용 기판 위에 코팅하고, 그 위에 Pt를 코팅하여 상대전극을 제조하는 단계(S204); 상기 상대전극을 상온에서 600℃까지의 범위에서 소성시켜 단일벽CNT 전극막을 제조하는 상대전극 열처리 단계(S205)를 포함하는 제조방법에 의해 제조된다. 여기서, 상대전극을 상온에서 600℃까지의 범위에서 소성시킴으로써, 상대전극의 열처리온도에 따라 표면 거칠기를 제어할 수는 요건을 만들 수 있다.In addition, the counter electrode of the solar cell using the CNT / Pt composite for dye-sensitized solar cell according to the present invention after dissolving acetic acid in ethanol, TiO 2 Add powder and mix, TiO 2 Preparing a paste (S201); Preparing a binder, a single wall CNT, and a solvent at a ratio of 1 to 20 wt%: 1 to 40 wt%: 98 to 40 wt% (S202); Dissolving the binder in the solvent to prepare a dispersion solution, and then mixing the single wall CNT with the dispersion solution to form a single wall CNT paste (S203); Coating the single-wall CNT paste on a counter electrode substrate and coating Pt thereon to prepare a counter electrode (S204); The counter electrode is fired in a range from room temperature to 600 ° C. to produce a single-wall CNT electrode film. Here, by firing the counter electrode in a range from room temperature to 600 ° C., it is possible to make a requirement to control the surface roughness according to the heat treatment temperature of the counter electrode.
도 3은 본 발명에 따른 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지의 상대전극을 포함하는 태양전지의 개념도로서, 본 발명의 염료감응형 태양전지는 후술할 본 발명의 CNT/Pt 복합체를 이용한 태양전지의 상대전극의 제조방법에 의해 제조된 상대전극(301), 전해질층(302) 및 일전극(303)을 구비하는데, 상기 일전극(303)은 전면 전극기판(304) 위에 형성된 전극(305)과 광흡수층(306)으로 구성되고, 상기 광흡수층(306)은 금속산화물층, 예를 들어 TiO2 표면에 염료가 흡착된 층이다.3 is a conceptual diagram of a solar cell including a counter electrode of a dye-sensitized solar cell having a CNT / Pt composite counter electrode according to the present invention, and the dye-sensitized solar cell of the present invention will be described below. A
즉, 유리로 된 투명기판, 투명기판의 내측표면에 형성된 SnO2 재질의 도전성 투명전극 코팅층과, 그 표면에는 염료가 흡착된 TiO2 다공질 음극전극과 후술할 본 발명에 따른 조성물의 CNT 전극막으로 형성된 양극부의 상대전극과, 상기 음극전극과 상대전극 사이에는 p형 반도체의 역할을 담당하는 전해질로 충진된다.That is, a transparent substrate made of glass, a conductive transparent electrode coating layer of SnO 2 material formed on the inner surface of the transparent substrate, a TiO 2 porous cathode electrode having dye adsorbed on the surface thereof, and a CNT electrode film of the composition according to the present invention to be described later. The counter electrode of the formed anode portion and the cathode electrode and the counter electrode are filled with an electrolyte serving as a p-type semiconductor.
도 3에서, 도면부호 307은 상대 전극기판이며, 308은 투명전도성막이며, 309는 CNT/Pt 복합체이며, 310은 전해질이다.In FIG. 3,
이하, 본 발명에 따른 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법의 바람직한 실시 예를 상세히 설명한다,
Hereinafter, a preferred embodiment of the dye-sensitized solar cell manufacturing method having a CNT / Pt composite counter electrode according to the present invention will be described in detail.
[실시 예][Example]
TiOTiO 22 페이스트 제조Paste manufacturer
먼저, 아세트산(acetic acid)을 에탄올에 완전히 용해시킨 다음, TiO2 분말을 넣고 혼합한 후, 이 혼합물이 균일한 페이스트를 형성할 때까지 고에너지 볼밀링법(high ball milling)을 수행함과 동시에 알파-테르피놀(α-Terpinol)과 에틸셀룰로우즈(ethylcellulose)를 첨가하여 원하는 점도를 맞추고, 롤볼밀링법(roll ball milling)으로 광전극 코팅용 페이스트를 제조한다. 이렇게 제조된 TiO2 페이스트를 이용하여 TiO2 나노분말층을 형성 및 소결시킨다.
First, acetic acid is completely dissolved in ethanol, and then TiO 2 After mixing and mixing the powder, high energy ball milling is performed until the mixture forms a uniform paste, while alpha-terpinol and ethylcellulose are added. The desired viscosity was added to the mixture to prepare a photoelectrode coating paste by roll ball milling. Thus prepared TiO 2 TiO 2 using paste The nanopowder layer is formed and sintered.
염료의 흡착Dye adsorption
TiO2 나노분말층을 형성 및 소결 후, 대표적인 루테늄계 염료인 N719의 dye를 각각 24 시간 동안 흡착시켰다. 즉, TiO2 나노입자가 소결된 투명전도성 전극을 적당량이 에타놀에 희석한 N719를 흡착시킨다.
TiO 2 After forming and sintering the nanopowder layer, dyes of N719, a representative ruthenium-based dye, were adsorbed for 24 hours, respectively. That is, TiO 2 A transparent conductive electrode sintered with nanoparticles is adsorbed with N719 diluted in an appropriate amount of ethanol.
CNTCNT 페이스트 제조 Paste manufacturer
100㎎의 단일CNT를 정제 및 분산하기 위해 50㎖의 5~50vol%의 질산용액에 담궈 3시간 동안 초음파 처리한다.To purify and disperse 100 mg of single CNT, soak in 50 ml of 5-50 vol% nitric acid solution and sonicate for 3 hours.
그 후, 상기 CNT를 덮고 있는 질산을 제거하기 위해 증류수로 반복하여 세척한 후, 종이필터로 걸러낸다. 이후 바인더로 에폭시 수지를 첨가한 후 알코올 용매에 혼합하여 6시간 동안 재차 초음파 처리를 하여 CNT 페이스트를 완성한다.
Thereafter, after repeated washing with distilled water to remove the nitric acid covering the CNT, it is filtered with a paper filter. After the addition of epoxy resin as a binder and mixed in an alcohol solvent and sonicated for 6 hours again to complete the CNT paste.
상대전극 제조Relative electrode manufacturing
완성된 CNT 페이스트를 스프레이 코팅 방식으로 기판 상에 코팅한 후 130~600℃에서 1시간 동안 경화시킴으로써, CNT 박막을 형성시킨다. 이후 형성된 CNT 박막 상에 2.5~10mol 농도의 Pt을 코팅한다. 여기서, CNT 페이스트를 경화시키는 온도에 따라 CNT 박막의 접착력이 달라지며, Pt의 농도에 따라 Pt의 입자들이 이러한 CNT 코팅에 영향을 미칠 수 있다(실험결과, 10mol 농도까지의 Pt가 좋은 영향을 미친다는 것이 발견되었음).
The finished CNT paste is coated on a substrate by spray coating, and then cured at 130 to 600 ° C. for 1 hour to form a CNT thin film. Then, Pt is coated with a concentration of 2.5-10 mol on the formed CNT thin film. Here, the adhesion of the CNT thin film varies depending on the temperature at which the CNT paste is cured, and the Pt particles may affect the CNT coating depending on the concentration of Pt (the results show that Pt up to 10 mol concentration has a good effect). Was found).
상대전극 열처리Counter Electrode Heat Treatment
이렇게 완성된 상대전극을 도막의 안전성과 전기전도도를 감안하여 상온에서600℃까지의 범위에서 1시간 열처리 후 상대전극으로 사용한다.
The completed counter electrode is used as a counter electrode after annealing for 1 hour in a range from room temperature to 600 ° C. in consideration of the safety and electrical conductivity of the coating film.
도 4a 내지 4d는 TiO2 박막을 7㎛, 14㎛, 21㎛, 28㎛ 별로 코팅한 연료감응형 태양전지 박막의 표면 및 단면을 나타낸 SEM 사진으로서, 박막의 입자는 18-20㎚ 입자의 크기로 코팅되었다. 도 4a 내지 4d에 알 수 있는 바와 같이, 박막의 두께가 두꺼울수록 박막의 소결이 증대되고 집성되는 현상을 관찰할 수가 있다. 여기서, 상기 TiO2 박막은 400~600℃에서 2~7시간 동안 소성시킴으로써, 그 두께가 7~30㎛가 된다. 여기서, TiO2 박막은 400℃ 이상의 소성온도에서 염료흡착이 가능하나, 600℃ 이상에서는 기판에 악영향을 미칠 수 있다.4A-4D shows TiO 2 SEM image showing the surface and cross-section of a fuel-sensitized solar cell thin film coated with thin films of 7 μm, 14 μm, 21 μm, and 28 μm. The particles of the thin film were coated with a size of 18-20 nm. As can be seen from FIGS. 4A to 4D, the thicker the thin film, the more the sintering and aggregation of the thin film can be observed. Here, the TiO 2 thin film is baked at 400 to 600 ° C. for 2 to 7 hours, and the thickness thereof becomes 7 to 30 μm. Where TiO 2 The thin film is capable of adsorbing dye at a firing temperature of 400 ° C. or higher, but may adversely affect the substrate at 600 ° C. or higher.
또한, 도 5는 TiO2 나노 분말층의 두께에 따른 염료감응형 태양전지의 박막의 특성의 변화 및 UV 측정 그래프로서, 도 5에 도시된 바와 같이, TiO2 박막이 21㎛일 때 광투과율과 염료감응형 태양전지의 효율이 증대함을 알 수 있다.5 is TiO 2. Dye-Sensitized Solar Cell According to the Thickness of Nano Powder Layer As a graph of the change in the properties of the thin film and UV measurement, as shown in Figure 5, TiO 2 It can be seen that the light transmittance and the efficiency of the dye-sensitized solar cell increase when the thin film is 21 μm.
이하, 표 1은 TiO2 박막의 두께에 따른 염료감응형 태양전지의 효율변화를 나타낸 것이다.
Hereinafter, Table 1 shows TiO 2. Dye-Sensitized Solar Cell According to Thin Film Thickness The change in efficiency is shown.
[표 1]에서 알 수 있듯이, TiO2 박막이 3층으로 제조된 양극에서 가장 높은 효율을 보이는 것으로 관찰되었다. 이는 앞서 도 5에서 TiO2 박막이 21㎛일 때 광투과율과 염료감응형 태양전지의 효율이 증대한다는 것과 일치됨을 알 수 있다.As Table 1 shows, TiO 2 It was observed that the thin film showed the highest efficiency at the anode made of three layers. This is because TiO 2 in FIG. It can be seen that when the thin film is 21 μm, the light transmittance and the efficiency of the dye-sensitized solar cell are increased.
이렇게 제조된 본 발명에 따른 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법은 제조공정이 단순하고, 균일 CNT 투명전극을 이용함으로써 전극의 열화 가능성이 있는 염료감응형 태양전지의 신뢰도를 향상시킴과 동시에 다양한 기판에 전극을 형성시킬 수 있다.The dye-sensitized solar cell manufacturing method having the CNT / Pt composite counter electrode according to the present invention thus manufactured has a simple manufacturing process and reliability of the dye-sensitized solar cell having the possibility of deterioration of the electrode by using a uniform CNT transparent electrode. The electrode can be formed on various substrates at the same time.
비록 본 발명의 실시 예에선, CNT 페이스트를 스프레이 코팅 방식으로 기판 상에 코팅하였으나, 이에 한정되지 않고 카본계열 소재나 또는 그래핀(graphene)이 사용될 수도 있음은 물론이다.Although in the embodiment of the present invention, the CNT paste is coated on the substrate by a spray coating method, without being limited to this, carbon-based material or graphene may be used.
이상과 같이 본 발명은 양호한 실시 예에 근거하여 설명하였지만, 이러한 실시 예는 본 발명을 제한하려는 것이 아니라 예시하려는 것이므로, 본 발명이 속하는 기술분야의 숙련자라면 본 발명의 기술사상을 벗어남이 없이 위 실시 예에 대한 다양한 변화나 변경 또는 조절이 가능할 것이다. 그러므로, 본 발명의 보호 범위는 본 발명의 기술적 사상의 요지에 속하는 변화 예나 변경 예 또는 조절 예를 모두 포함하는 것으로 해석되어야 할 것이다.
While the present invention has been particularly shown and described with reference to exemplary embodiments thereof, it is to be understood that the invention is not limited to the disclosed exemplary embodiments, but, on the contrary, Various changes, modifications or adjustments to the example will be possible. Therefore, the scope of protection of the present invention should be construed as including all changes, modifications, and adjustments that fall within the spirit of the technical idea of the present invention.
301: 상대전극 302: 전해질층
303: 일전극 304, 307: 기판
305: 전극 306: 광흡수층
308: 전도성막 309: CNT/Pt 복합체
310: 전해질301: counter electrode 302: electrolyte layer
303: one
305: electrode 306: light absorption layer
308: conductive film 309: CNT / Pt composite
310: electrolyte
Claims (8)
1~20wt% : 1~40wt% : 98~40wt%의 비율로 바인더, 단일벽CNT, 용매를 준비하는 단계;
상기 바인더를 상기 용매에 녹여 분산용액을 만든 후, 상기 분산용액에 상기 단일벽CNT를 혼합하여 단일벽CNT 페이스트를 만드는 단계;
상기 TiO2 페이스트로 형성된 투명전도성막을 상대전극용 기판 위에 코팅하고, 그 위에 상기 단일벽CNT 페이스트를 코팅하고, 그 위에 Pt를 코팅하여 상대전극을 제조하는 단계; 및
상기 상대전극을 상온에서 600℃까지의 범위에서 소성시켜 단일벽CNT 전극막을 제조하는 상대전극 열처리 단계를 포함하는 것을 특징으로 하는 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법.
Acetic acid was dissolved in ethanol and then TiO 2 Add powder and mix, TiO 2 Preparing a paste;
Preparing a binder, a single wall CNT, and a solvent at a ratio of 1 to 20 wt%: 1 to 40 wt%: 98 to 40 wt%;
Dissolving the binder in the solvent to form a dispersion solution, and then mixing the single wall CNT with the dispersion solution to form a single wall CNT paste;
The TiO 2 Coating a transparent conductive film formed of a paste on a counter electrode substrate, coating the single-wall CNT paste thereon, and coating Pt thereon to prepare a counter electrode; And
A method of manufacturing a dye-sensitized solar cell having a CNT / Pt composite counter electrode, comprising a counter electrode heat treatment step of baking the counter electrode at room temperature up to 600 ° C. to produce a single-wall CNT electrode film.
상기 단일벽CNT 페이스트를 스프레이 코팅 방식으로 기판 상에 코팅한 후 130~600℃에서 1시간 동안 경화시킴으로써 CNT 박막을 형성하는 단계와
상기 형성된 CNT 박막 상에 2.5~10mol 농도의 Pt을 코팅하는 단계를 더 포함함하는 것을 특징으로 하는 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법.
The method of claim 1, wherein the counter electrode manufacturing step
Forming a CNT thin film by coating the single-wall CNT paste on a substrate by spray coating and curing at 130 to 600 ° C. for 1 hour.
A method of manufacturing a dye-sensitized solar cell having a CNT / Pt composite counter electrode further comprising coating Pt at a concentration of 2.5 to 10 mol on the formed CNT thin film.
상기 TiO2 페이스트를 이용하여 400~600℃에서 2~7시간 동안 소결시켜 7~30㎛의 두께로 형성시키는 것을 특징으로 하는 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법.
The method of claim 1, wherein the transparent conductive film,
The TiO 2 Dye-sensitized solar cell manufacturing method having a CNT / Pt composite counter electrode, characterized in that the paste is sintered at 400 ~ 600 ℃ for 2-7 hours to form a thickness of 7 ~ 30㎛.
100㎎의 단일CNT를 정제 및 분산하기 위해 50㎖의 5~50vol%의 질산용액에 담궈 3시간 동안 초음파 처리하며;
상기 CNT를 덮고 있는 질산을 제거하기 위해 증류수로 반복하여 세척하고 종이필터로 걸러내며;
상기 걸러진 CNT에 바인더로 에폭시 수지를 첨가한 후, 알코올 용매에 혼합하여 6시간 동안 재차 초음파 처리를 하여 형성되는 것을 특징으로 하는 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법.
The method of claim 1, wherein the single-wall CNT paste,
Soak for 3 hours in 50 ml of 5-50 vol% nitric acid solution to purify and disperse 100 mg of single CNT;
Repeated washing with distilled water to remove nitric acid covering the CNTs and filtered through a paper filter;
The dye-sensitized solar cell manufacturing method having a CNT / Pt composite counter electrode, characterized in that formed by ultrasonic treatment for 6 hours after adding the epoxy resin as a binder to the filtered CNT.
The CNT according to claim 1, wherein the counter electrode substrate is any one of an insulating substrate including a glass substrate, an FTO or ITO conductive substrate coated with a transparent conductive film, a conductive plastic, an alumina substrate, and a magnesia ceramic substrate. Dye-sensitized solar cell manufacturing method having a / Pt composite counter electrode.
상기 탄소나노튜브 페이스트는 닥터블레이드법(doctorblade), 스크린프린팅법(screenprinting), 롤프린팅법(Roll printing), 스프레이법(spray), 스핀코팅법(spincoating), 딥핑법(dipping) 중의 어느 하나의 방법에 의해 상기 상대전극용 기판 위에 코팅되는 것을 특징으로 하는 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법.
The method of claim 1,
The carbon nanotube paste is any one of a doctorblade method, a screen printing method, a roll printing method, a spray method, a spray method, a spin coating method, and a dipping method. Dye-sensitized solar cell manufacturing method having a CNT / Pt composite counter electrode, characterized in that the coating on the counter electrode substrate by a method.
상기 바인더는 폴리비닐부티랄인 것을 특징으로 하는 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법.
The method of claim 1,
The binder is a polyvinyl butyral, characterized in that the dye-sensitized solar cell manufacturing method having a CNT / Pt composite counter electrode.
상기 용매는 에틸알콜, 메틸알콜, 이소프로필 알코올, 아세톤, 메틸에틸케톤, 에틸 이소케톤, 에틸렌글리콜류, 아닐린류, 톨루엔, 클로로포름 중에서 선택되는 하나 또는 2개 이상의 용액인 것을 특징으로 하는 CNT/Pt 복합체 상대전극을 구비한 염료감응형 태양전지 제조방법.The method of claim 1,
The solvent is CNT / Pt, characterized in that one or more solutions selected from ethyl alcohol, methyl alcohol, isopropyl alcohol, acetone, methyl ethyl ketone, ethyl isoketone, ethylene glycol, aniline, toluene, chloroform Dye-sensitized solar cell manufacturing method having a composite counter electrode.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| KR101441890B1 (en) * | 2013-03-04 | 2014-09-22 | 인하대학교 산학협력단 | Menufacture of counter electrodes containing metal/graphene composites |
| KR101575509B1 (en) * | 2014-07-31 | 2015-12-07 | 성균관대학교산학협력단 | Electron collector for solar cell and method of fabricating thererof |
| KR101628575B1 (en) | 2014-12-24 | 2016-06-08 | 현대자동차주식회사 | Method for manufactured tantalum-silver complex electrode of dye-sensitized solar cell(dssc) using ionic liquid electroplating |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
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| KR101441890B1 (en) * | 2013-03-04 | 2014-09-22 | 인하대학교 산학협력단 | Menufacture of counter electrodes containing metal/graphene composites |
| KR101575509B1 (en) * | 2014-07-31 | 2015-12-07 | 성균관대학교산학협력단 | Electron collector for solar cell and method of fabricating thererof |
| KR101628575B1 (en) | 2014-12-24 | 2016-06-08 | 현대자동차주식회사 | Method for manufactured tantalum-silver complex electrode of dye-sensitized solar cell(dssc) using ionic liquid electroplating |
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