KR101316096B1 - Organic-inorganic hybrid tandem multijuntion photovoltaics with an interlayer and preparing method for thereof - Google Patents
Organic-inorganic hybrid tandem multijuntion photovoltaics with an interlayer and preparing method for thereof Download PDFInfo
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Abstract
Description
본 발명은 중간층이 삽입된 유·무기 복합 탠덤 태양전지 및 이의 제조방법에 관한 것이다.
The present invention relates to an organic-inorganic composite tandem solar cell having an intermediate layer inserted therein and a method of manufacturing the same.
최근 대체에너지 개발에 대한 관심이 높아지면서 태양전지 개발에도 많은 연구가 이루어지고 있다. 태양전지는 빛에너지를 직접 전기 에너지로 변환시키는 반도체 소자로서, 빛을 흡수하는 두 개 이상의 반도체물질 층으로 구성된다. 상기 태양전지는 p-n 접합을 이루는 반도체 다이오드에 빛을 조사하면 광자가 흡수되어 전자/정공쌍이 생성되고 두 개의 다른 물질의 접합부에서 전위차가 발생함으로써 전류가 흐르게 된다.
Recently, as interest in developing alternative energy increases, many researches are being conducted on solar cell development. Solar cells are semiconductor devices that convert light energy directly into electrical energy and are composed of two or more layers of semiconductor material that absorb light. In the solar cell, when light is irradiated to a semiconductor diode forming a pn junction, photons are absorbed to generate electron / hole pairs, and a current flows by generating a potential difference at a junction of two different materials.
태양전지는 광활성층의 구성 물질에 따라 크게 무기물 태양전지 또는 유기물 태양전지로 구분할 수 있다. 종래 태양전지는 단결정 또는 다결정 실리콘 태양전지가 대부분이었으나, 최근 실리콘 소재의 공급 불안정화가 심화되어, 수급 불균형에 따른 고비용 문제가 발생하고 있어 이를 대체하기 위한 새로운 태양전지를 개발하게 되었다.
Solar cells can be classified into inorganic solar cells or organic solar cells according to the material of the photoactive layer. Conventional solar cells were mostly monocrystalline or polycrystalline silicon solar cells, but recently, the destabilization of supply of silicon material has been intensified, resulting in high cost problems due to supply and demand imbalance, and thus, new solar cells have been developed to replace them.
탠덤 태양전지(Tandem solar cell)는 서로 다른 광학 밴드갭(Optical Bandgap)을 갖는 물질을 2층 이상으로 형성한 구조를 갖는다. 탠덤 태양전지는 빛의 입사면에서 가까운 부분에 넓은 밴드갭을 갖는 물질로 이루어진 반도체층(Top Cell)이 구비되고, 빛의 입사면에서 먼 부분에 상대적으로 좁은 밴드갭을 갖는 물질로 이루어진 반도체층(Bottom Cell)이 삽입된 구조를 갖는다.
Tandem solar cells have a structure in which two or more layers of materials having different optical bandgaps are formed. Tandem solar cells are provided with a semiconductor layer (Top Cell) made of a material having a wide bandgap at a portion close to the incident surface of light, and a semiconductor layer made of a material having a relatively narrow bandgap at a portion far from the incident surface of light. (Bottom Cell) has a structure inserted.
예를 들면, 유·무기 복합 탠덤 태양전지는 유기재료와 무기재료를 혼용한 이종접합 구조를 가지며, 유기물질 및 무기물질의 장점에 의해 각각의 단점을 상호 보완함으로써 태양전지의 광전변환효율 및 사용수명을 향상시킬 수 있는 장점이 있다.
For example, organic / inorganic composite tandem solar cells have a heterojunction structure in which organic and inorganic materials are mixed, and each photoelectric conversion efficiency and use of solar cells are complemented by mutually compensating the disadvantages of the organic and inorganic materials. There is an advantage to improve the service life.
탠덤 태양전지는 다른 흡수 대역을 가진 셀을 사용함으로써 태양광의 스펙트럼을 효율적으로 흡수하여 태양전지의 광전변환효율을 향상시키지만, 실제로 다른 흡수 대역을 가진 셀을 단순히 조합하는 것만으로는 광전변환효율을 향상시키는데 어려움이 있어 두 셀의 결합일치 정도, 계면 혼합층 유무, 셀간의 조합 등을 고려하여야 한다.
Tandem solar cells improve the photovoltaic efficiency of solar cells by efficiently absorbing the spectrum of sunlight by using cells with different absorption bands, but in fact, simply combining cells with different absorption bands improves the photoelectric conversion efficiency. In order to solve the problem, the degree of coupling between two cells, the presence or absence of interfacial mixture layer, and the combination between cells should be considered.
종래 유·무기 복합 탠덤 태양전지의 효율을 향상시키는 방법으로는 다양한 방법들이 공지되어있다.
Various methods are known as methods for improving the efficiency of conventional organic-inorganic composite tandem solar cells.
대한민국등록특허 제10-1018319호(등록일:2011.02.22)는 유·무기 복합 적층형 태양전지의 제조방법에 관한 것이다. 상기 특허문헌에서는 무기태양전지와 유기태양전지 사이에 중간전극층으로 PEDOT:PSS 박막을 형성시키는 방법에 대하여 개시하고 있다(특허문헌 1). 일반적으로 상기 PEDOT:PSS는 정공수송층으로 사용되며, 유·무기 복합 탠덤 태양전지의 태양광 흡수율을 향상시키기 위하여 도입되는 것이나, 상기 PEDOT:PSS는 흡습성이 있어 제조되는 유·무기 복합 탠덤 태양전지의 장기간 안정성이 낮은 단점이 있다.
Republic of Korea Patent No. 10-1018319 (Registration Date: 2011.02.22) relates to a manufacturing method of the organic-inorganic composite laminated solar cell. The patent document discloses a method of forming a PEDOT: PSS thin film as an intermediate electrode layer between an inorganic solar cell and an organic solar cell (Patent Document 1). In general, the PEDOT: PSS is used as a hole transport layer, and is introduced to improve the solar absorption rate of the organic / inorganic composite tandem solar cell, but the PEDOT: PSS is an organic / inorganic composite tandem solar cell manufactured by being hygroscopic. The long term stability is low.
또한, 대한민국공개특허 제10-2011-0029732호(공개일:2011.03.23)는 복수의 태양전지 모듈을 적층 구조로 배치하여 모듈 사이에 확산재층을 형성하여 태양광에 의한 발전효율을 극대화시킨 적층형 태양전지에 관한 것으로서, 상기 특허문헌에서는 무기태양전지와 유기태양전지 사이에 확산수지재로서 폴리카보네이트, 폴리에스테르수지 중 하나를 사용하여 태양전지의 태양광 흡수율을 향상시키는 방법에 대하여 개시하고 있다(특허문헌 2). 그러나, 상기 폴리카보네이트, 폴리에스테르수지는 내열성 수지이긴 하나 고분자 특성상 흡습성이 있어 제조되는 유·무기 복합 탠덤 태양전지의 장기간 안정성이 낮은 단점이 있다.
In addition, Korean Patent Publication No. 10-2011-0029732 (published: 2011.03.23) is a laminated type in which a plurality of solar cell modules are arranged in a stacked structure to form a diffuser layer between the modules to maximize power generation efficiency due to sunlight. The present invention relates to a solar cell, and the patent document discloses a method of improving the solar absorption rate of a solar cell by using one of a polycarbonate and a polyester resin as a diffusion resin material between an inorganic solar cell and an organic solar cell ( Patent document 2). However, although the polycarbonate and the polyester resin are heat-resistant resins, there is a disadvantage in that the long-term stability of the organic-inorganic composite tandem solar cell manufactured due to hygroscopicity is low.
한편, 그래핀은 이차원의 판상 구조 형태를 갖는 넓은 표면적을 가진 물질로서, sp2 혼성 탄소를 포함하여 전기적, 열적, 기계적 특성이 매우 뛰어나 초고용량 캐패시터(capacitor), 이차전지, 수소저장 물질과 같은 에너지 저장물질, 트랜지스터, 센서, 투명전극 및 고분자 복합체 등 다양한 분야에서 각광받고 있는 물질이다.
On the other hand, graphene is a material having a large surface area having a two-dimensional plate-like structure, and has excellent electrical, thermal, and mechanical properties including sp 2 hybrid carbon, such as ultracapacitors, secondary batteries, and hydrogen storage materials. It is a material that is attracting attention in various fields such as energy storage materials, transistors, sensors, transparent electrodes, and polymer composites.
일반적으로 그래핀은 대량생산이 어렵고, 제조단가가 높아 일반적으로 그래핀 옥사이드를 대량생산하여 이를 열 또는 화학적으로 처리하여 물리적특성을 제어하여 사용한다.
In general, graphene is difficult to mass-produce, and manufacturing costs are high, and in general, graphene oxide is mass-produced and thermally or chemically processed to control physical properties.
예를 들면, 화학적 박리법을 이용하여 그래핀 옥사이드를 제조하는 방법은 흑연을 산화시켜 그라파이트 옥사이드(graphite oxide)를 제조한 후, 간단한 초음파 처리를 통해 수용액 상에서 한 장의 그래핀 옥사이드(graphene oxide) 서스펜션을 만드는 방법이다. 그러나, 상기 화학적 박리법을 이용하여 제조된 그래핀 옥사이드는 산화 및 초음파 처리 과정 중 물리적 성질이 저하되는 문제가 있다. 구체적으로, 흑연을 산화시키는 과정 중에 산소를 포함하는 작용기들이 그래핀 표면에 결합하게 되며, 이로 인해 친수성 그룹들이 부착됨으로써 그래핀 층간 거리가 멀어지게 되어 그 결과 그래핀의 물성을 좌우하는 sp2 혼성 탄소가 파괴된다.
For example, a method of preparing graphene oxide using chemical exfoliation method is to prepare graphite oxide by oxidizing graphite and then to prepare a single graphene oxide suspension in an aqueous solution through simple sonication. How to make it. However, graphene oxide prepared using the chemical exfoliation method has a problem in that physical properties are degraded during oxidation and sonication. Specifically, oxygen-containing functional groups are bonded to the surface of graphene during oxidation of graphite, which causes hydrophilic groups to be attached, thereby increasing the distance between graphene layers, resulting in sp 2 hybrids that influence the properties of graphene. Carbon is destroyed
이와 같이 그래핀 옥사이드는 제조과정에서 산소를 포함하는 작용기들이 결합되어 있으므로, 이를 열처리하거나 환원제를 사용하여 이를 환원시킴으로써 물리적 특성을 보완한다.
As described above, since graphene oxide is bonded to functional groups containing oxygen in the manufacturing process, the graphene oxide is supplemented with physical properties by heat treatment or reduction thereof using a reducing agent.
상기 그래핀 옥사이드는 고투명성을 갖고, 용액공정이 가능하여 대면적 코팅이 가능하고, 금속촉매를 필요로 하지 않으며, 저온공정이 가능하고, 전기적특성을 조절하기가 용이할 뿐만 아니라, 기계적으로 유연한 장점이 있다.
The graphene oxide has a high transparency, can be a solution process can be a large area coating, does not require a metal catalyst, low temperature process, easy to control the electrical properties, mechanically flexible There is an advantage.
이에, 본 발명자들은 유·무기 복합 탠덤 태양전지의 광전변환효율을 향상시키기 위한 방법을 연구하던 중, 무기계 광활성층 및 유기계 광활성층 사이에 삽입된 산화인듐주석 전자수송층/그래핀 옥사이드 정공수송층으로 이루어진 중간층(interlayer)이 무기계 광활성층에서 생성되는 전자와 유기계 광활성층에서 생성되는 정공이 재결합할 수 있는 영역을 효율적으로 제공할 수 있어 유·무기 복합 탠덤 태양전지의 광전변환효율을 향상시킬 수 있을 뿐만 아니라 장기간 안정성을 향상시킬 수 있음을 알아내고 본 발명을 완성하였다.
Thus, the inventors of the present invention while studying a method for improving the photoelectric conversion efficiency of the organic-inorganic composite tandem solar cell, consisting of an indium tin oxide electron transport layer / graphene oxide hole transport layer interposed between the inorganic photoactive layer and the organic photoactive layer The interlayer can efficiently provide the recombination region between the electrons generated in the inorganic photoactive layer and the holes generated in the organic photoactive layer, thereby improving the photoelectric conversion efficiency of the organic / inorganic composite tandem solar cell. It has been found that the long term stability can be improved and the present invention has been completed.
본 발명의 목적은 중간층이 삽입된 유·무기 복합 탠덤 태양전지 및 이의 제조방법을 제공하는 데 있다.
It is an object of the present invention to provide an organic-inorganic composite tandem solar cell having an intermediate layer inserted therein and a method of manufacturing the same.
상기 과제를 해결하기 위해, 본 발명은,In order to solve the above problems,
기판;Board;
상기 기판상에 형성된 투명전극층;A transparent electrode layer formed on the substrate;
상기 투명전극층상에 적층된 무기계 광활성층;An inorganic photoactive layer stacked on the transparent electrode layer;
상기 무기계 광활성층상에 적층된 산화인듐주석 전자수송층;An indium tin oxide electron transport layer laminated on the inorganic photoactive layer;
상기 전자수송층상에 적층된 그래핀 옥사이드 정공수송층; A graphene oxide hole transport layer stacked on the electron transport layer;
상기 정공수송층상에 적층된 유기계 광활성층; 및An organic photoactive layer laminated on the hole transport layer; And
상기 유기계 광활성층상에 적층된 후면전극층을 포함하는 중간층이 삽입된 유·무기 복합 탠덤 태양전지를 제공한다.
Provided is an organic-inorganic composite tandem solar cell having an intermediate layer including a rear electrode layer stacked on the organic photoactive layer.
또한, 본 발명은,Further, according to the present invention,
기판상에 투명전극층을 코팅하는 단계(단계 1);Coating a transparent electrode layer on the substrate (step 1);
상기 투명전극층 상부에 무기계 광활성층을 적층하는 단계(단계 2);Stacking an inorganic photoactive layer on the transparent electrode layer (step 2);
상기 무기계 광활성층 상부에 산화인듐주석 전자수송층을 적층하는 단계(단계 3);Stacking an indium tin oxide electron transport layer on the inorganic photoactive layer (step 3);
상기 전자수송층 상부에 그래핀 옥사이드 정공수송층을 적층하는 단계(단계 4);Stacking a graphene oxide hole transport layer on the electron transport layer (step 4);
상기 정공수송층 상부에 유기계 광활성층을 적층하는 단계(단계 5); 및Stacking an organic photoactive layer on the hole transport layer (step 5); And
상기 유기계 광활성층 상부에 후면전극층을 적층하는 단계(단계 6)를 포함하는 것을 특징으로 하는 중간층이 삽입된 유·무기 복합형 탠덤 태양전지의 제조방법.A method of manufacturing an organic / inorganic hybrid tandem solar cell in which an intermediate layer is inserted, comprising the step (step 6) of stacking a rear electrode layer on the organic photoactive layer.
본 발명에 따른 유·무기 복합 탠덤 태양전지의 무기계 광활성층 및 유기계 광활성층 사이에 삽입된 산화인듐주석 전자수송층/그래핀 옥사이드 정공수송층으로 이루어진 중간층은 무기계 광활성층에서 생성되는 전자와 유기계 광활성층에서 생성되는 정공이 재결합할 수 있는 영역을 효율적으로 제공하여, 유·무기 복합 탠덤 태양전지의 광전변환효율을 향상시킬 수 있을 뿐만 아니라 장기간 안정성을 향상시킬 수 있는 효과가 있다.
The intermediate layer consisting of an indium tin oxide electron transport layer / graphene oxide hole transport layer inserted between an inorganic photoactive layer and an organic photoactive layer of the organic / inorganic composite tandem solar cell according to the present invention is used in the electron and organic photoactive layer generated in the inorganic photoactive layer. By efficiently providing a region where holes can be recombined, the photoelectric conversion efficiency of the organic / inorganic composite tandem solar cell can be improved as well as the long-term stability can be improved.
도 1은 본 발명에 따른 중간층이 삽입된 유·무기 복합 탠덤 태양전지를 나타낸 모식도이다.
도 2는 본 발명에 따른 실시예 1 및 실시예 2의 중간층이 삽입된 유·무기 복합 탠덤 태양전지 및 비교예 1 ~ 4의 유·무기 복합 탠덤 태양전지의 전압에 대한 전류밀도를 측정한 결과이다.
도 3은 본 발명에 따른 실시예 2 및 비교예 5의 중간층이 삽입된 유·무기 복합 탠덤 태양전지의 시간에 따른 전력변환효율을 측정한 결과이다.1 is a schematic diagram showing an organic-inorganic composite tandem solar cell in which an intermediate layer is inserted according to the present invention.
Figure 2 is a result of measuring the current density with respect to the voltage of the organic-inorganic composite tandem solar cell and the organic-inorganic composite tandem solar cells of Example 1 and Example 2 inserted according to the present invention and Comparative Examples 1 to 4 to be.
3 is a result of measuring the power conversion efficiency with time of the organic-inorganic hybrid tandem solar cell inserted in the intermediate layer of Example 2 and Comparative Example 5 according to the present invention.
본 발명은,According to the present invention,
기판;Board;
상기 기판상에 형성된 투명전극층;A transparent electrode layer formed on the substrate;
상기 투명전극층상에 적층된 무기계 광활성층;An inorganic photoactive layer stacked on the transparent electrode layer;
상기 무기계 광활성층상에 적층된 산화인듐주석 전자수송층;An indium tin oxide electron transport layer laminated on the inorganic photoactive layer;
상기 전자수송층상에 적층된 그래핀 옥사이드 정공수송층; A graphene oxide hole transport layer stacked on the electron transport layer;
상기 정공수송층상에 적층된 유기계 광활성층; 및An organic photoactive layer laminated on the hole transport layer; And
상기 유기계 광활성층상에 적층된 후면전극층을 포함하는 중간층이 삽입된 유·무기 복합 탠덤 태양전지를 제공한다.
Provided is an organic-inorganic composite tandem solar cell having an intermediate layer including a rear electrode layer stacked on the organic photoactive layer.
이하, 본 발명의 중간층이 삽입된 유·무기 복합 탠덤 태양전지에 대하여 상세히 설명한다.
Hereinafter, the organic-inorganic composite tandem solar cell in which the intermediate layer of the present invention is inserted will be described in detail.
본 발명에 따른 중간층이 삽입된 유·무기 복합 탠덤 태양전지에 있어서, 상기 기판으로는 유리, 플라스틱 기판 등을 사용할 수 있다. 상기 기판은 빛이 일차적으로 입사되는 부분으로서 빛의 투과율이 우수함과 동시에 제조되는 유·무기 복합 탠덤 태양전지 내에서의 내부 단락을 방지할 수 있도록 투명절연성 재질을 사용하는 것이 바람직하다.
In the organic / inorganic composite tandem solar cell in which the intermediate layer according to the present invention is inserted, glass, a plastic substrate, or the like may be used as the substrate. Preferably, the substrate is made of a transparent insulating material so as to prevent internal short-circuiting in the organic / inorganic composite tandem solar cell, which is excellent in transmittance of light as a primary incident light.
다음으로, 본 발명에 따른 중간층이 삽입된 유·무기 복합 탠덤 태양전지에 있어서, 상기 투명전극층은 기판 상부에 적층된다. 상기 투명전극층으로는 알루미늄이 도핑된 산화아연(AZO; Aluminium-zinc oxide; ZnO:Al), 산화인듐주석(ITO;indium-tin oxide), 산화아연(ZnO), 산화알루미늄주석(ATO;Aluminium-tin oxide; SnO2:Al), 불소함유 산화주석(FTO: Fluorine-doped tin oxide), 은 나노와이어, 그래핀(graphene), 탄소나노튜브, PEDOT:PSS 등을 단독 또는 이를 혼합하여 사용할 수 있으며, 바람직하게는 알루미늄이 도핑된 산화아연(AZO)를 사용할 수 있다. 상기 투명전극층은 외부로부터 입사되는 빛을 광흡수층으로 통과시키는 역할을 한다.
Next, in the organic-inorganic composite tandem solar cell in which the intermediate layer is inserted according to the present invention, the transparent electrode layer is stacked on the substrate. The transparent electrode layer may be aluminum-doped zinc oxide (AZO), aluminum-zinc oxide (ZnO: Al), indium tin oxide (ITO), zinc oxide (ZnO), or aluminum tin oxide (ATO). tin oxide; SnO 2 : Al), fluorine-doped tin oxide (FTO), silver nanowires, graphene, carbon nanotubes, PEDOT: PSS, etc. may be used alone or in combination thereof. Preferably, aluminum doped zinc oxide (AZO) may be used. The transparent electrode layer serves to pass light incident from the outside to the light absorbing layer.
다음으로, 본 발명에 따른 중간층이 삽입된 유·무기 복합 탠덤 태양전지에 있어서, 상기 무기계 광활성층은 투명전극층 상부에 적층된다. 상기 무기계 광활성층으로는 비정질 실리콘을 사용할 수 있다. 또한, 상기 무기계 광활성층은 p형 비정질 실리콘층/i형 비정질 실리콘층/n형 비정질 실리콘이 순서대로 적층된 구조를 가질 수 있다. 상기 무기계 광활성층은 빛을 받으면 전자 및 정공을 생성한다. 예를 들면, p형/i형/n형 구조는 i층이 p층과 n층에 의해 공핍(depletion)되어 내부에 전기장을 발생하게 되면, 태양광에 의해 생성되는 정공 및 전자가 상기 전기장에 의해 드리프트되어 각각 p층과 n층에서 수집된다. 구체적으로, 상기 공핍은 n층에서 생성된 자유전자가 확산하여 p층의 접합 부근의 정공과 결합함으로써 i층에 장벽전위를 형성하여 n층의 자유전자와 p층의 정공이 확산되지 않는 것을 말한다. 또한, 무기계 광활성층을 사용함으로써, 종래 유기계 광활성층만을 사용했을 때보다 스퍼터링, 동일한 용매를 이용한 유기계 광활성층의 코팅, 플라즈마 또는 자외선과 같은 표면처리과정 중에 셀이 손상되는 것을 방지할 수 있다.
Next, in the organic-inorganic composite tandem solar cell in which the intermediate layer according to the present invention is inserted, the inorganic photoactive layer is stacked on the transparent electrode layer. Amorphous silicon may be used as the inorganic photoactive layer. In addition, the inorganic photoactive layer may have a structure in which a p-type amorphous silicon layer / i-type amorphous silicon layer / n-type amorphous silicon is sequentially stacked. The inorganic photoactive layer generates electrons and holes upon receiving light. For example, in the p-type / i-type / n-type structure, when the i layer is depleted by the p layer and the n layer to generate an electric field therein, holes and electrons generated by sunlight are applied to the electric field. Drift and collect in p and n layers, respectively. Specifically, the depletion means that free electrons generated in the n-layer diffuse and bond with holes near the junction of the p-layer to form a barrier potential in the i-layer so that the free electrons in the n-layer and the p-layer do not diffuse. . In addition, by using the inorganic photoactive layer, it is possible to prevent the cell from being damaged during the sputtering, coating of the organic photoactive layer using the same solvent, surface treatment such as plasma or ultraviolet rays, than using the conventional organic photoactive layer.
다음으로, 본 발명에 따른 중간층이 삽입된 유·무기 복합 탠덤 태양전지에 있어서, 산화인듐주석 전자수송층은 무기계 광활성층 상부에 적층된다. 상기 산화인듐주석 전자수송층은 고투명성을 가져 넓은 밴드갭을 갖는 반도체층(Top Cell)에 도달하는 빛의 세기가 크므로 반도체층의 광전류흐름을 증가시킬 수 있는 특징이 있다.
Next, in the organic-inorganic composite tandem solar cell in which the intermediate layer according to the present invention is inserted, the indium tin oxide electron transport layer is stacked on the inorganic photoactive layer. Since the indium tin oxide electron transport layer has high transparency, the light intensity reaching the semiconductor layer (Top Cell) having a wide bandgap is large, and thus the photocurrent flow of the semiconductor layer may be increased.
다음으로, 본 발명에 따른 중간층이 삽입된 유·무기 복합 탠덤 태양전지에 있어서, 상기 그래핀 옥사이드 정공수송층은 산화인듐주석 전자수송층 상부에 적층된다. 상기 그래핀 옥사이드 정공수송층은 정공을 운반하는데 뛰어난 효과를 나타내며, 높은 전기전도도를 가지므로 소자의 내부 저항을 줄일 수 있을 뿐만 아니라, 적층구조에서 발생하는 직렬 저항에 의한 전력 손실을 줄일 수 있는 장점이 있다. Next, in the organic-inorganic composite tandem solar cell in which the intermediate layer is inserted according to the present invention, the graphene oxide hole transport layer is stacked on the indium tin oxide electron transport layer. The graphene oxide hole transport layer has an excellent effect in transporting holes, and has a high electrical conductivity, which not only reduces the internal resistance of the device, but also reduces the power loss due to the series resistance generated in the stacked structure. have.
또한, 정공수송층으로서 종래 PEDOT:PSS를 사용하는 경우에는 흡습성, 장기간 안정성이 문제가 되었으나, 이를 그래핀 옥사이드로 대체함으로써 제조되는 유·무기 복합 탠덤 태양전지의 장기간 안정성을 향상시킬 수 있는 특징이 있다.
In addition, when using the conventional PEDOT: PSS as a hole transport layer, the hygroscopicity and long-term stability was a problem, but there is a feature that can improve the long-term stability of the organic-inorganic composite tandem solar cell manufactured by replacing it with graphene oxide .
상기 무기계 광활성층 상부에 순서대로 적층되는 산화인듐주석 전자수송층/그래핀 옥사이드 정공수송층은 중간층(interlayer)으로서, 본 발명의 무기계 광활성층에서 생성된 전자와 유기계 광활성층에서 생성된 정공을 받아 전하가 효과적으로 재결합 할 수 있는 공간을 제공해주고, 전하의 수송을 담당하는 역할을 수행할 수 있다. 따라서, 본 발명에 따른 중간층이 삽입된 유·무기 복합 탠덤 태양전지는 상기 산화인듐주석 전자수송층/그래핀 옥사이드 정공수송층으로 이루어진 중간층이 삽입됨으로써 광전변환효율이 향상될 뿐만 아니라, 제조되는 유·무기 복합 태양전지의 장기간 안정성을 향상시킬 수 있는 특징이 있다.
The indium tin oxide electron transport layer / graphene oxide hole transport layer, which is sequentially stacked on the inorganic photoactive layer, is an interlayer, and receives charges generated in the inorganic photoactive layer of the present invention and holes generated in the organic photoactive layer. It can provide a space for effective recombination and play a role in transporting charges. Therefore, the organic-inorganic composite tandem solar cell having the intermediate layer inserted according to the present invention not only improves the photoelectric conversion efficiency by inserting the intermediate layer made of the indium tin oxide electron transport layer / graphene oxide hole transport layer, but also produces organic and inorganic There is a feature that can improve the long-term stability of the composite solar cell.
다음으로, 본 발명에 따른 중간층이 삽입된 유·무기 복합 탠덤 태양전지에 있어서, 상기 유기계 광활성층은 상기 그래핀 옥사이드 정공수송층 상부에 형성된다. 상기 유기계 광활성층으로는 장파장의 빛을 흡수하는 밴드갭이 작은 유기재료를 사용할 수 있으며, PBDTTT-C(poly[4,8-bis-alkyloxybenzo[1,2-b:4,5-b']dithiophene-2,6-diyl-alt-[alkyl thieno[3,4-b]thiophene-2-carboxylate]-2,6-diyl), PTB7 (Poly[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl][3-fluoro-2-[(2-ethylhexyl)carbonyl]thieno[3,4-b]thiophenediyl]]), PCPDTBT (poly[2,6-(4,4-bis-(2-ethylhexyl)-4H-cyclopenta[2,1-b;3,4-b'] dithiophene)-alt-4,7-(2,1,3-benzothiadiazole)]), PC61BM [6,6]-phenyl-C61-butyric acid methyl ester), PC71BM 등을 단독 또는 혼합하여 사용할 수 있다.
Next, in the organic-inorganic composite tandem solar cell in which the intermediate layer is inserted according to the present invention, the organic photoactive layer is formed on the graphene oxide hole transport layer. As the organic photoactive layer, an organic material having a small band gap for absorbing light of a long wavelength can be used, and poly [4,8-bis-alkyloxybenzo [1,2-b: 4,5-b ' 2-carboxylate] -2,6-diyl), PTB7 (Poly [[4,8-bis [(2-ethylhexyl) -2,6-diyl- oxy] benzo [1,2-b: 4,5-b '] dithiophene-2,6-diyl] [3-fluoro-2 - [(2- ethylhexyl) carbonyl] thieno [3,4- b] thiophenediyl] ], PCPDTBT (poly [2,6- (4,4-bis- (2-ethylhexyl) -4H-cyclopenta [2,1- b; 3,4- b '] dithiophene) (2,1,3-benzothiadiazole)], PC 61 BM [6,6] -phenyl-C 61 -butyric acid methyl ester) and PC 71 BM.
다음으로, 본 발명에 따른 중간층이 삽입된 유·무기 복합 탠덤 태양전지에 있어서, 상기 후면전극층은 상기 유기계 광활성층 상부에 형성된다. 상기 후면전극층으로는 알루미늄, 은, 금, 크롬, 팔라듐, 그래핀, 탄소나노튜브, 은 나노와이어 등을 단독으로 사용할 수 있다. 상기 후면전극층은 상기 나열한 각각의 층을 통과한 태양광을 다시 반사시켜 무기계 광활성층으로 재입사시키는 역할을 한다.
Next, in the organic-inorganic composite tandem solar cell in which the intermediate layer according to the present invention is inserted, the back electrode layer is formed on the organic photoactive layer. As the back electrode layer, aluminum, silver, gold, chromium, palladium, graphene, carbon nanotubes, silver nanowires, or the like may be used alone. The back electrode layer serves to reflect back the sunlight passing through each of the above-mentioned layers to re-inject into the inorganic photoactive layer.
또한, 본 발명은, Further, according to the present invention,
기판상에 투명전극층을 적층하는 단계(단계 1);Stacking a transparent electrode layer on the substrate (step 1);
상기 투명전극층 상부에 무기계 광활성층을 적층하는 단계(단계 2);Stacking an inorganic photoactive layer on the transparent electrode layer (step 2);
상기 무기계 광활성층 상부에 산화인듐주석 전자수송층을 적층하는 단계(단계 3);Stacking an indium tin oxide electron transport layer on the inorganic photoactive layer (step 3);
상기 전자수송층 상부에 그래핀 옥사이드 정공수송층을 적층하는 단계(단계 4);Stacking a graphene oxide hole transport layer on the electron transport layer (step 4);
상기 정공수송층 상부에 유기계 광활성층을 적층하는 단계(단계 5); 및Stacking an organic photoactive layer on the hole transport layer (step 5); And
상기 유기계 광활성층 상부에 후면전극층을 적층하는 단계(단계 6)를 포함하는 것을 특징으로 하는 중간층이 삽입된 유·무기 복합 탠덤 태양전지의 제조방법을 제공한다.
It provides a method of manufacturing an organic-inorganic hybrid tandem solar cell is inserted into the intermediate layer, characterized in that it comprises a step (step 6) of stacking a back electrode layer on the organic photoactive layer.
이하, 본 발명의 중간층이 삽입된 유·무기 복합 탠덤 태양전지의 제조방법을 각 단계별로 상세히 설명한다.
Hereinafter, the manufacturing method of the organic-inorganic composite tandem solar cell in which the intermediate layer of the present invention is inserted will be described in detail for each step.
본 발명에 따른 중간층이 삽입된 유·무기 복합 탠덤 태양전지의 제조방법에 있어서, 상기 단계 1은 기판상에 투명전극층을 적층하는 단계이다.
In the method of manufacturing an organic / inorganic hybrid tandem solar cell having an intermediate layer inserted therein, the
상기 기판으로는 유리, 플라스틱 기판 등을 사용할 수 있다. 상기 기판상에 투명전극층을 적층하는 방법으로는 스퍼터링과 같은 통상적인 방법을 사용할 수 있다.
As the substrate, glass, a plastic substrate, or the like can be used. As a method of laminating the transparent electrode layer on the substrate, a conventional method such as sputtering may be used.
상기 기판상에 적층되는 투명전극층은 태양광이 기판쪽에서 조사되므로 투명도가 높은 물질일수록 유리하다. 상기 투명전극층으로는 알루미늄이 도핑된 산화아연(AZO; Aluminium-zinc oxide;ZnO:Al), 산화인듐주석(ITO;indium-tin oxide), 산화아연(ZnO), 산화알루미늄주석(ATO;Aluminium-tin oxide; SnO2:Al), 불소함유 산화주석(FTO: Fluorine-doped tin oxide), 은 나노와이어, 그래핀(graphene), 탄소나노튜브, PEDOT:PSS 등을 단독 또는 이를 혼합하여 사용할 수 있으며, 바람직하게는 알루미늄이 도핑된 산화아연(AZO)를 사용할 수 있다.
The transparent electrode layer laminated on the substrate is advantageous as the material having high transparency because sunlight is irradiated from the substrate side. The transparent electrode layer may be aluminum-doped zinc oxide (AZO), aluminum-zinc oxide (ZnO: Al), indium tin oxide (ITO), zinc oxide (ZnO), or aluminum tin oxide (ATO). tin oxide; SnO 2 : Al), fluorine-doped tin oxide (FTO), silver nanowires, graphene, carbon nanotubes, PEDOT: PSS, etc. may be used alone or in combination thereof. Preferably, aluminum doped zinc oxide (AZO) may be used.
다음으로, 상기 단계 2는 투명전극층 상부에 무기계 광활성층을 적층하는 단계이다.
Next,
상기 투명전극층 상부에 무기계 광활성층을 적층하는 방법으로는 플라즈마화학기상증착법(Plasma-enhanced chemical vapor deposition, PECVD) 등을 사용할 수 있다.
Plasma-enhanced chemical vapor deposition (PECVD) may be used as a method of stacking the inorganic photoactive layer on the transparent electrode layer.
상기 무기계 광활성층은 투명전극층 상부에 p형 비정질 실리콘층, i(intrinsic)형 비정질 실리콘층 및 n형 비정질 실리콘층 각각이 순서대로 적층된 구조일 수 있다. 구체적으로 상기 p형 비정질 실리콘은 3가 원소인 붕소, 칼륨과 같은 원소가 도핑된 비정질 실리콘을 의미하고, i형 비정질 실리콘은 어떠한 불순물도 첨가되지 않은 비정질 실리콘을 의미하고, n형 비정질 실리콘은 5가 원소인 인, 비소, 안티몬과 같은 원소가 도핑된 비정질 실리콘을 의미한다.
The inorganic photoactive layer may have a structure in which a p-type amorphous silicon layer, an i (intrinsic) type amorphous silicon layer, and an n-type amorphous silicon layer are sequentially stacked on the transparent electrode layer. Specifically, the p-type amorphous silicon refers to amorphous silicon doped with elements such as boron and potassium, which are trivalent elements, the i-type amorphous silicon refers to amorphous silicon to which no impurities are added, and the n-type amorphous silicon is 5 It refers to amorphous silicon doped with elements such as phosphorus, arsenic, and antimony.
예를 들면, 상기 무기계 광활성층은 투명전극층 상부에 p형 비정질 실리콘층을 플라즈마화학기상증착법을 이용하여 적층시키고, 상기 p형 비정질 실리콘층 상부에 i형 비정질 실리콘층을 플라즈마화학기상증착법을 이용하여 적층시키고, 상기 i형 비정질 실리콘층 상부에 n형 비정질 실리콘층을 플라즈마화학기상증착법을 이용하여 적층시켜 형성될 수 있다.
For example, the inorganic photoactive layer may be formed by depositing a p-type amorphous silicon layer on the transparent electrode layer using a plasma chemical vapor deposition method, and an i-type amorphous silicon layer on the p-type amorphous silicon layer by using a plasma chemical vapor deposition method. The n-type amorphous silicon layer may be stacked on the i-type amorphous silicon layer by using plasma chemical vapor deposition.
다음으로, 상기 단계 3은 무기계 광활성층 상부에 산화인듐주석 전자수송층을 적층하는 단계이다.
Next,
상기 무기계 광활성층 상부에 산화인듐주석 전자수송층을 적층하는 방법으로는 마그네트론 스퍼터링(magnetron sputtering)과 같은 방법을 사용할 수 있다.
As a method of stacking the indium tin oxide electron transport layer on the inorganic photoactive layer, a method such as magnetron sputtering may be used.
다음으로, 상기 단계 4는 산화인듐주석 전자수송층 상부에 그래핀 옥사이드 정공수송층을 적층하는 단계이다.
Next,
상기 산화인듐주석 전자수송층 상부에 그래핀 옥사이드 정공수송층을 적층하는 방법으로는 스핀코팅과 같은 방법을 사용할 수 있다.
As a method of stacking the graphene oxide hole transport layer on the indium tin oxide electron transport layer, a method such as spin coating may be used.
또한, 본 발명은 상기 단계 4 이후에 100 ~ 300 ℃에서 열처리하는 단계를 더 포함할 수 있다.
In addition, the present invention may further include the step of heat treatment at 100 ~ 300 ℃ after
본 발명에 따른 중간층이 삽입된 유·무기 복합 탠덤 태양전지의 제조방법에 있어서, 상기 열처리는 산화인듐주석 전자수송층 상부에 적층된 그래핀 옥사이드 정공수송층을 환원시키기 위한 공정이다. 상기 열처리를 통해 그래핀 옥사이드 표면에 결합된 산소를 포함하는 작용기들을 환원시켜 그래핀 옥사이드의 제조과정 중에 파괴된 sp2 구조를 복원시킴으로써, 그래핀 옥사이드의 물리적 특성을 향상시킬 수 있다. 따라서, 상기 열처리를 통해 제조되는 유·무기 복합 탠덤 태양전지의 광전변환효율 및 장기간 안정성을 더욱 향상시킬 수 있는 효과가 있다.
In the method of manufacturing an organic-inorganic composite tandem solar cell with an interlayer inserted according to the present invention, the heat treatment is a process for reducing the graphene oxide hole transport layer laminated on the indium tin oxide electron transport layer. Sp 2 destroyed during the production of graphene oxide by reducing functional groups containing oxygen bonded to the surface of graphene oxide through the heat treatment. By restoring the structure, the physical properties of graphene oxide can be improved. Therefore, there is an effect that can further improve the photoelectric conversion efficiency and long-term stability of the organic-inorganic composite tandem solar cell manufactured by the heat treatment.
다음으로, 상기 단계 5는 그래핀 옥사이드 정공수송층 상부에 유기계 광활성층을 적층하는 단계이다.
Next,
상기 그래핀 옥사이드 정공수송층 상부에 유기계 광활성층을 적층하는 방법으로는 스핀코팅과 같은 방법을 사용할 수 있다.
As a method of stacking the organic photoactive layer on the graphene oxide hole transport layer, a method such as spin coating may be used.
상기 그래핀 옥사이드 정공수송층 상부에 적층되는 유기계 광활성층으로는 PBDTTT-C(poly[4,8-bis-alkyloxybenzo[1,2-b:4,5-b']dithiophene-2,6-diyl-alt-[alkyl thieno[3,4-b]thiophene-2-carboxylate]-2,6-diyl), PTB7 (Poly[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl][3-fluoro-2-[(2-ethylhexyl)carbonyl]thieno[3,4-b]thiophenediyl]]), PCPDTBT (poly[2,6-(4,4-bis-(2-ethylhexyl)-4H-cyclopenta[2,1-b;3,4-b'] dithiophene)-alt-4,7-(2,1,3-benzothiadiazole)]), PC61BM [6,6]-phenyl-C61-butyric acid methyl ester), PC71BM 등을 단독 또는 혼합하여 사용할 수 있다.
The organic photoactive layer stacked on the graphene oxide hole transport layer is PBDTTT-C (poly [4,8-bis-alkyloxybenzo [1,2-b: 4,5-b '] dithiophene-2,6-diyl- alt- [alkyl thieno [3,4-b] thiophene-2-carboxylate] -2,6-diyl), PTB7 (Poly [[4,8-bis [(2-ethylhexyl) oxy] benzo [1,2- b: 4,5-b '] dithiophene-2,6-diyl] [3-fluoro-2-[(2-ethylhexyl) carbonyl] thieno [3,4-b] thiophenediyl]]), PCPDTBT (poly [2 , 6- (4,4-bis- (2-ethylhexyl) -4H-cyclopenta [2,1-b; 3,4-b '] dithiophene) -alt-4,7- (2,1,3-benzothiadiazole )]), PC 61 BM [6,6] -phenyl-C 61 -butyric acid methyl ester), PC 71 BM and the like can be used alone or in combination.
다음으로, 상기 단계 6은 유기계 광활성층 상부에 후면전극층을 적층하는 단계이다.
Next,
상기 유기계 광활성층 상부에 후면전극층을 적층하는 방법으로는 열증착법, 진공증착법과 같은 방법을 사용할 수 있다.
As a method of stacking the rear electrode layer on the organic photoactive layer, a method such as thermal deposition or vacuum deposition may be used.
상기 유기계 광활성층 상부에 적층되는 후면전극층으로는 알루미늄, 은, 금, 크롬, 팔라듐, 그래핀, 탄소나노튜브, 은 나노와이어 등을 단독으로 사용할 수 있다.
Aluminum, silver, gold, chromium, palladium, graphene, carbon nanotubes, silver nanowires, and the like may be used as the back electrode layer stacked on the organic photoactive layer.
또한, 본 발명은 상기 제조방법으로 제조되며, 기판상에 투명전극층/무기계 광활성층/산화인듐주석 전자수송층/그래핀 옥사이드 정공수송층/유기계 광활성층/후면전극층이 순서대로 적층된 구조를 갖는 중간층이 삽입된 유·무기 복합 탠덤 태양전지를 제공한다.
In addition, the present invention is manufactured by the above manufacturing method, the intermediate layer having a structure in which a transparent electrode layer / inorganic non-organic photoactive layer / indium tin oxide electron transport layer / graphene oxide hole transport layer / organic photoactive layer / rear electrode layer in order on the substrate Provided is an organic-inorganic composite tandem solar cell inserted.
탠덤태양전지는 하부 투명전극을 통해 태양빛이 조사되면, 밴드갭이 큰 하부 셀에서 단파장의 빛을 흡수하고, 밴드갭이 작은 상부 셀에서 하부 셀을 통과한 장파장 영역의 빛을 흡수한다. 이때, 저항의 증가 없이 이상적으로 두 단위 셀을 직렬 연결하게 되면 광전류는 동일하게 흐르고, 전체 셀의 개방회로전압(Voc)이 증가하여 (Voc = Voc ,1 + Voc ,2) 효율을 크게 향상시킬 수 있다.
When the tandem solar cell is irradiated with sunlight through the lower transparent electrode, the light absorbs short wavelengths in the lower cell having a large band gap, and absorbs light in the long wavelength region passing through the lower cell in the upper cell having a small band gap. At this time, if two unit cells are ideally connected in series without increasing the resistance, the photocurrent flows in the same way, and the open circuit voltage (V oc ) of all the cells increases (V oc = V oc , 1 + V oc , 2 ) efficiency. Can greatly improve.
따라서, 본 발명에 따른 중간층이 삽입된 유·무기 복합 탠덤 태양전지는 무기계 광활성층 및 유기계 광활성층 사이에 산화인듐주석 전자수송층/그래핀 옥사이드 정공수송층으로 이루어진 중간층을 포함함으로써, 무기계 광활성층에서 생성된 전자와 유기계 광활성층에서 생성된 정공이 효과적으로 재결합할 수 있는 공간이 형성되어 제조되는 유·무기 복합 탠덤 태양전지의 광전변환효율이 향상될 뿐만 아니라, 그래핀 옥사이드층이 삽입됨으로써 제조되는 유·무기 복합 태양전지의 장기간 안정성이 우수한 특징이 있다.
Therefore, the organic-inorganic composite tandem solar cell in which the intermediate layer is inserted according to the present invention includes an intermediate layer made of an indium tin oxide electron transport layer / graphene oxide hole transport layer between an inorganic photoactive layer and an organic photoactive layer, thereby creating an inorganic photoactive layer. The photovoltaic conversion efficiency of organic-inorganic composite tandem solar cells manufactured by forming a space for effectively recombining the electrons generated in the organic photoactive layer and the electrons formed in the organic photoactive layer is improved, and the Long term stability of inorganic composite solar cells is excellent.
이하, 본 발명의 실시예를 통해 더욱 상세히 설명한다. 단, 하기 실시예는 본 발명을 예시하는 것일 뿐 본 발명의 내용이 하기 실시예에 의해 한정되는 것은 아니다.
Hereinafter, embodiments of the present invention will be described in more detail. However, the following examples are illustrative of the present invention and are not intended to limit the scope of the present invention.
<< 실시예Example 1> 산화인듐주석 1> Indium Tin Oxide 전자수송층Electron transport layer /Of 그래핀Grapina 옥사이드Oxide 정공수송층으로 이루어진 중간층이 삽입된 유·무기 복합 탠덤 태양전지 Organic / Inorganic Composite Tandem Solar Cell with Interlayer of Hole Transport Layer
단계 1. 기판을 준비하는 단계
알루미늄이 도핑된 산화아연(AZO)이 500 ㎚ ~ 1 ㎛ 두께로 적층된 유리기판을 아세톤 또는 이소프로필 알코올을 이용하여 세척하거나 산소 분위기에서 자외선을 조사하여 표면처리(UVO) 하였다.
A glass substrate on which aluminum-doped zinc oxide (AZO) has been deposited to a thickness of 500 nm to 1 μm was subjected to surface treatment (UVO) by washing with acetone or isopropyl alcohol or irradiating ultraviolet rays in an oxygen atmosphere.
단계 2. 무기계 광활성층을 적층하는 단계
다음으로, 플라즈마화학기상증착법(plasma-enhanced chemical vapor deposition, PECVP)을 이용하여 상기 알루미늄이 도핑된 산화아연층(AZO) 상부에 p형 비정질 실리콘층/i형 비정질 실리콘층/n형 비정질 실리콘층을 각각 5 ㎚/70 ㎚/5 ㎚ 두께로 적층하였다.
Next, p-type amorphous silicon layer / i-type amorphous silicon layer / n-type amorphous silicon layer on the aluminum-doped zinc oxide layer (AZO) using plasma-enhanced chemical vapor deposition (PECVP). Were laminated to a thickness of 5 nm / 70 nm / 5 nm, respectively.
상기 i형 비정질 실리콘층은 실란(SiH4) 및 수소(H2)의 혼합물로부터 얻었고, 상기 i형 비정질 실리콘을 구성하는 혼합물에 수소화붕소(BH4) 및 인화수소(PH3)를 각각 첨가하여 p형 비정질 실리콘 및 n형 비정질 실리콘을 얻었다.
The i-type amorphous silicon layer was obtained from a mixture of silane (SiH 4 ) and hydrogen (H 2 ), boron hydride (BH 4 ) and hydrogen fluoride (PH 3 ) were added to the mixture constituting the i-type amorphous silicon p-type amorphous silicon and n-type amorphous silicon were obtained.
단계 3. 산화인듐주석 전자수송층을 적층하는 단계
다음으로, 마그네트론 스퍼터링법을 이용하여 상기 n형 비정질 실리콘층 상부에 산화인듐주석 전자수송층을 50 ㎚ 두께로 적층하였다.
Next, an indium tin oxide electron transport layer was deposited to a thickness of 50 nm on the n-type amorphous silicon layer by using the magnetron sputtering method.
단계 4. 그래핀 옥사이드 정공수송층을 적층하는 단계
다음으로, 농도가 275 ㎎/ℓ인 그래핀 옥사이드와 물의 혼합용액을 스핀코팅법(5000 rpm, 40 초)을 이용하여 산화인듐주석 전자수송층 상부에 그래핀 옥사이드 정공수송층을 1 ~ 3 ㎚로 적층하였다.
Next, a graphene oxide hole transport layer was laminated at a thickness of 1 to 3 nm on the indium tin oxide electron transport layer using a spin coating method (5000 rpm, 40 seconds) in a mixed solution of graphene oxide and water having a concentration of 275 mg / l. It was.
단계 5. 유기계 광활성층을 적층하는 단계
다음으로, 스핀코팅법을 이용하여 그래핀 옥사이드 정공수송층 상부에 PBDTTT-C:PCBM(중량비, 1:2)과 디클로로벤젠수용액(농도, 2 중량%)과 혼합한 용액을 80 ~ 100 ㎚ 두께로 적층하였다. 상기 단계 완료 후, 상온에서 10 분간 건조시켰다.
Next, a solution of PBDTTT-C: PCBM (weight ratio 1: 2) and dichlorobenzene aqueous solution (concentration, 2 wt%) on the graphene oxide hole transport layer was spin-coated to a thickness of 80 to 100 nm. Laminated. After completion of the above step, it was dried at room temperature for 10 minutes.
단계 6. 후면전극층을 적층하는 단계
다음으로, 열증착법을 이용하여 상기 PBDTTT-C:PCBM 상부에 알루미늄층을 100 ㎚ 두께로 적층하여 산화인듐주석 전자수송층/그래핀 옥사이드 정공수송층으로 이루어진 중간층이 삽입된 유·무기 복합 탠덤 태양전지를 제조하였다(도 1).
Next, an organic-inorganic composite tandem solar cell in which an intermediate layer consisting of an indium tin oxide electron transport layer / graphene oxide hole transport layer was inserted by stacking an aluminum layer on the PBDTTT-C: PCBM layer using a thermal evaporation method. Prepared (FIG. 1).
<< 실시예Example 2> 산화인듐주석 2> indium tin oxide 전자수송층Electron transport layer /Of 그래핀Grapina 옥사이드Oxide 정공수송층으로To the hole transport layer 이루어진 중간층이 삽입된 유·무기 복합 탠덤 태양전지 Organic and inorganic composite tandem solar cell with interlayer
상기 실시예 1 중 상기 단계 4 이후에 200 ℃에서 10 분간 열처리를 더 수행한 것을 제외하고는 실시예 1과 동일한 방법을 사용하여 산화인듐주석 전자수송층/그래핀 옥사이드 정공수송층으로 이루어진 중간층이 삽입된 유·무기 복합 탠덤 태양전지를 제조하였다.
An intermediate layer made of indium tin oxide electron transport layer / graphene oxide hole transport layer was inserted in the same manner as in Example 1 except that heat treatment was further performed at 200 ° C. for 10 minutes after
<< 비교예Comparative Example 1> 중간층이 삽입되지 않은 유·무기 복합 탠덤 태양전지 1> Organic / Inorganic Composite Tandem Solar Cell without Interlayer
상기 실시예 1 중 단계 3 및 단계 4를 수행하지 않은 것을 제외하고는 실시예 1과 동일한 방법을 사용하여 유·무기 복합 탠덤 태양전지를 제조하였다.
An organic-inorganic hybrid tandem solar cell was manufactured in the same manner as in Example 1, except that
<< 비교예Comparative Example 2> 2> 산화인듐주석층이Indium tin oxide layer 단독으로 삽입된 유·무기 복합 탠덤 태양전지 Organic / Inorganic Composite Tandem Solar Cell Inserted Separately
상기 실시예 1 중 단계 4를 수행하지 않은 것을 제외하고는 실시예 1과 동일한 방법을 사용하여 유·무기 복합 탠덤 태양전지를 제조하였다.
An organic-inorganic composite tandem solar cell was manufactured in the same manner as in Example 1, except that
<< 비교예Comparative Example 3> 3> 그래핀Grapina 옥사이드층이Oxide layer 단독으로 삽입된 유·무기 복합 탠덤 태양전지 Organic / Inorganic Composite Tandem Solar Cell Inserted Separately
상기 실시예 1 중 단계 3을 수행하지 않은 것을 제외하고는 실시예 1과 동일한 방법을 사용하여 유·무기 복합 탠덤 태양전지를 제조하였다.
An organic-inorganic composite tandem solar cell was manufactured in the same manner as in Example 1, except that
<< 비교예Comparative Example 4> 4> 그래핀Grapina 옥사이드층이Oxide layer 단독으로 삽입된 유·무기 복합 탠덤 태양전지 Organic / Inorganic Composite Tandem Solar Cell Inserted Separately
상기 실시예 1 중 단계 3을 수행하지 않고, 단계 4 이후에 200 ℃에서 10 분간 열처리를 더 수행한 것을 제외하고는 실시예 1과 동일한 방법을 사용하여 유·무기 복합 탠덤 태양전지를 제조하였다.
An organic-inorganic composite tandem solar cell was manufactured in the same manner as in Example 1, except that
<< 비교예Comparative Example 5> 산화인듐주석 5> Indium Tin Oxide 전자수송층Electron transport layer /Of PEDOTPEDOT :: PSSPSS 정공수송층으로To the hole transport layer 이루어진 중간층이 삽입된 유·무기 복합 탠덤 태양전지 Organic and inorganic composite tandem solar cell with interlayer
상기 실시예 1 중 단계 4에서 그래핀 옥사이드 대신에 폴리(3,4-에틸렌디옥시티오펜):폴리(스티렌설포네이트)(PEDOT:PSS)를 사용한 것을 제외하고는 실시예 1과 동일한 방법을 사용하여 유·무기 복합 탠덤 태양전지를 제조하였다.
The same method as in Example 1, except that poly (3,4-ethylenedioxythiophene): poly (styrenesulfonate) (PEDOT: PSS) was used instead of graphene oxide in
<실험예 1> 전기적특성 분석≪ Experimental Example 1 >
(1) J-V 그래프 분석 (1) J-V graph analysis
본 발명에 따른 산화인듐주석 전자수송층/그래핀 옥사이드 정공수송층으로 이루어진 중간층의 삽입효과를 알아보기 위해, 전압에 대한 전류밀도를 측정하고, 그 결과를 도 2 및 표 1에 나타내었다.In order to determine the insertion effect of the intermediate layer consisting of the indium tin oxide electron transport layer / graphene oxide hole transport layer according to the present invention, the current density against the voltage was measured, and the results are shown in Figure 2 and Table 1.
하기 표 1 중 단락회로전류밀도(Jsc), 개방회로전압(Voc) 및 곡선인자(Fill Factor, FF)는 태양전지의 전력변환효율을 특징 짓는 변수이다.The short circuit current density J sc , the open circuit voltage V oc and the fill factor (FF) in Table 1 are variables that characterize the power conversion efficiency of the solar cell.
상기 단락회로전류밀도는 회로가 단락된 상태로, 외부저항이 없는 상태에서 빛을 받았을 때 나타나는 역방향(음의 값)의 전류밀도이다. 단락회로전류밀도는 입사광의 세기와 파장분포가 결정된 상태에서, 광흡수에 의해 여기된 전자와 정공이 재결합(recombination)하여 손실되지 않고 얼마나 효과적으로 전지 내부에서 외부회로 쪽으로 보내어지는가에 의존한다. 상기 광흡수에 의해 여기된 전자와 정공의 재결합에 의한 손실은 재료의 내부 또는 계면에서 일어날 수 있다.The short circuit current density is a reverse (negative) current density that appears when light is received in the state that the circuit is short-circuited and there is no external resistance. The short circuit current density depends on how effectively the electrons and holes excited by light absorption recombine and are not lost in the state where the intensity of the incident light and the wavelength distribution are determined. Losses due to recombination of electrons and holes excited by the light absorption can occur inside the material or at the interface.
상기 개방회로전압은 무한대의 임피던스가 걸린 상태에서 빛을 받았을 때 태양전지의 양단에 형성되는 전위차이다.The open circuit voltage is a potential difference formed at both ends of the solar cell when light is received in an infinite impedance state.
상기 곡선인자는 최대전력점에서의 전류밀도와 전압의 곱(Jmp×Vmp)을 단락회로전류밀도와 개방회로전압의 곱(Jsc×Voc)으로 나눈 값이다. 상기 곡선인자는 빛이 조사된 상태에서 J - V 곡선의 모양이 사각형에 얼마나 가까운가를 나타내는 지표이다.The curve factor is the product of the current density at the maximum power point and the voltage (J mp × V mp ) divided by the product of the short circuit current density and the open circuit voltage (J sc × V oc ). The curve factor is an indicator of how close the shape of the J-V curve is to the square when the light is irradiated.
태양전지의 전력변환효율(PCE)는 태양전지에 의해 생산된 최대 전력과 입사광 에너지 Pin 사이의 비율이다.
The power conversion efficiency (PCE) of the solar cell is the ratio between the maximum power produced by the solar cell and the incident light energy P in .
(mA/cm2)Short circuit current density
(mA / cm 2 )
(V)Open circuit voltage
(V)
(%)Power conversion efficiency
(%)
상기 표 1을 참조하면, 본 발명에 따른 실시예 1의 산화인듐주석 전자수송층/그래핀 옥사이드 정공수송층으로 이루어진 중간층이 삽입된 유·무기 복합 탠덤 태양전지는 중간층이 없는 유·무기 복합 탠덤 태양전지(비교예 1)보다 약 3.86 배 높은 전력변환효율을 나타내었다.Referring to Table 1, an organic-inorganic composite tandem solar cell having an intermediate layer of an indium tin oxide electron transport layer / graphene oxide hole transport layer of Example 1 according to the present invention inserted therein is not an intermediate layer. It showed about 3.86 times higher power conversion efficiency than (Comparative Example 1).
나아가, 열처리 공정을 더 수행하여 제조된 중간층이 삽입된 유·무기 복합 탠덤 태양전지(실시예 2)는 상기 실시예 1의 중간층이 삽입된 유·무기 복합 탠덤 태양전지보다 3.04 배 높은 전력변환효율을 나타내었다.Furthermore, the organic-inorganic hybrid tandem solar cell having the intermediate layer inserted by performing the heat treatment process (Example 2) was 3.04 times higher in power conversion efficiency than the organic-inorganic hybrid tandem solar cell having the intermediate layer inserted in the first embodiment. Indicated.
또한, 중간층으로서 산화인듐주석층 또는 그래핀 옥사이드층을 단독으로 삽입된 경우보다, 산화인듐주석층/그래핀 옥사이드층으로 이루어진 중간층이 삽입된 경우 제조되는 태양전지의 전력변환효율이 향상됨을 나타내었다. 나아가, 상기 비교예 1의 중간층이 없는 유·무기 복합 탠덤 태양전지는 상대적으로 아주 낮은 광기전성능을 나타내는데, 이로부터 각각의 층들이 전기적으로 연결되어 있지 않다는 것을 알 수 있다.In addition, when the indium tin oxide layer or the graphene oxide layer is inserted alone as an intermediate layer, it is shown that the power conversion efficiency of the solar cell produced when the intermediate layer consisting of indium tin oxide layer / graphene oxide layer is inserted. . Furthermore, the organic-inorganic composite tandem solar cell without the intermediate layer of Comparative Example 1 exhibits relatively low photovoltaic performance, from which the respective layers are not electrically connected.
도 2를 참조하면, 비교예 1의 유·무기 복합 탠덤 태양전지의 J-V 그래프는 S 형 곡선을 나타내므로, 전하의 추출 및 주입에 대하여 에너지 장벽이 매우 높음을 알 수 있다.2, since the J-V graph of the organic-inorganic hybrid tandem solar cell of Comparative Example 1 shows an S-type curve, it can be seen that the energy barrier is very high for extraction and injection of charge.
반면에, 본 발명에 따른 실시예 1 및 2의 중간층이 삽입된 유·무기 복합 탠덤 태양전지의 J-V 그래프는 S 형 곡선을 나타내지 않으며, 열처리 공정을 수행한 실시예 2의 중간층이 삽입된 유·무기 복합 탠덤 태양전지의 곡선인자는 0.46으로 증가한 것을 알 수 있다.On the other hand, the JV graph of the organic-inorganic hybrid tandem solar cell in which the intermediate layers of Examples 1 and 2 were inserted according to the present invention did not show an S-shaped curve, It can be seen that the curve factor of the inorganic composite tandem solar cell increased to 0.46.
이로부터, 본 발명의 유·무기 복합 태양전지는 산화인듐주석 전자수송층/그래핀 옥사이드 정공수송층으로 이루어진 중간층이 삽입됨으로써 전력변환효율을 향상시킬 수 있으며, 이는 상기 중간층이 무기계 광활성층 및 유기계 광활성층 각각에서 생성된 전자와 정공이 재결합할 수 있는 영역을 효율적으로 제공하는 것에 기인하는 것으로 판단할 수 있다.
From this, the organic-inorganic composite solar cell of the present invention can improve the power conversion efficiency by inserting an intermediate layer consisting of an indium tin oxide electron transport layer / graphene oxide hole transport layer, which is an inorganic photoactive layer and an organic photoactive layer It can be judged that it is due to providing efficiently the area | region which can recombine the generated electron and the hole in each.
(2) 장기안정성 실험(2) long-term stability test
본 발명에 따른 산화인듐주석 전자수송층/그래핀 옥사이드 정공수송층으로 이루어진 중간층의 삽입효과를 알아보기 위해, 시간에 따른 전력변환효율을 측정하였고 이를 도 3 및 표 2에 나타내었다.
In order to determine the insertion effect of the intermediate layer consisting of the indium tin oxide electron transport layer / graphene oxide hole transport layer according to the present invention, the power conversion efficiency over time was measured and shown in Figure 3 and Table 2.
(day)Driving time
(day)
(㎃/㎠)Short circuit current density
(MA / cm2)
(V)Open circuit voltage
(V)
(%)Power conversion efficiency
(%)
실시예2
Example 2
비교예5
Comparative Example 5
상기 표 2를 참조하면, 본 발명에 따른 실시예 2의 산화인듐주석 전자수송층/그래핀 옥사이드 정공수송층이 삽입된 유·무기 복합 태양전지는 7 일이 지난 후에 전력변환효율이 약 9 % 정도 감소함을 나타내어, 시간에 따른 전력변환효율의 감소폭이 매우 작은 것을 알 수 있다.Referring to Table 2, the organic-inorganic hybrid solar cell having the indium tin oxide electron transport layer / graphene oxide hole transport layer of Example 2 according to the present invention reduces power conversion efficiency by about 9% after 7 days. It can be seen that the decrease in power conversion efficiency with time is very small.
반면에, 비교예 5의 산화인듐주석 전자수송층/PEDOT:PSS 정공수송층으로 이루어진 중간층이 삽입된 유·무기 복합 태양전지는 초기에는 높은 전력변환효율을 나타내나, 시간에 따라 전력변환효율의 감소폭이 매우 커 7 일이 지난 후에는 거의 태양전지로서 성능을 발휘하지 못하는 것을 알 수 있다.On the other hand, the organic-inorganic hybrid solar cell in which the intermediate layer of the indium tin oxide electron transport layer / PEDOT: PSS hole transport layer of Comparative Example 5 is inserted initially exhibits high power conversion efficiency, but the power conversion efficiency decreases with time. It's very big, and after seven days, it's almost impossible to perform as a solar cell.
이로부터, 본 발명에 따른 유·무기 복합 태양전지는 산화인듐주석 전자수송층/그래핀 옥사이드 정공수송층으로 이루어진 중간층이 삽입됨으로써 장기간 안정성이 향상된 것을 알 수 있다.From this, it can be seen that the organic-inorganic composite solar cell according to the present invention has improved long-term stability by inserting an intermediate layer composed of an indium tin oxide electron transport layer / graphene oxide hole transport layer.
Claims (14)
상기 기판상에 형성된 투명전극층;
상기 투명전극층상에 적층된 무기계 광활성층;
상기 무기계 광활성층상에 적층된 산화인듐주석 전자수송층;
상기 전자수송층상에 적층된 그래핀 옥사이드 정공수송층;
상기 정공수송층상에 적층된 유기계 광활성층; 및
상기 유기계 광활성층상에 적층된 후면전극층을 포함하는 중간층이 삽입된 유·무기 복합 탠덤 태양전지.
Board;
A transparent electrode layer formed on the substrate;
An inorganic photoactive layer stacked on the transparent electrode layer;
An indium tin oxide electron transport layer laminated on the inorganic photoactive layer;
A graphene oxide hole transport layer stacked on the electron transport layer;
An organic photoactive layer laminated on the hole transport layer; And
An organic-inorganic composite tandem solar cell having an intermediate layer including a back electrode layer stacked on the organic photoactive layer.
The organic-inorganic composite tandem solar cell of claim 1, wherein the substrate is a glass or plastic substrate.
The method of claim 1, wherein the transparent electrode layer is aluminum-doped zinc oxide (AZO; Aluminum-zinc oxide; ZnO: Al;), indium tin oxide (ITO; indium-tin oxide), zinc oxide (ZnO), aluminum oxide Groups containing tin (ATO; aluminum-tin oxide; SnO 2 : Al), fluorine-doped tin oxide (FTO), silver nanowires, graphene, carbon nanotubes, and PEDOT: PSS An organic-inorganic composite tandem solar cell having an interlayer inserted therein, characterized in that it is at least one member selected from the group.
The organic-inorganic composite tandem solar cell of claim 1, wherein the inorganic photoactive layer is formed by sequentially stacking an p-type amorphous silicon layer, an i-type amorphous silicon layer, and an n-type amorphous silicon.
The method of claim 1, wherein the organic photoactive layer is PBDTTT-C (poly [4,8-bis-alkyloxybenzo [1,2-b: 4,5-b '] dithiophene-2,6-diyl-alt- [alkyl thieno [3,4-b] thiophene-2-carboxylate] -2,6-diyl), PTB7 (Poly [[4,8-bis [(2-ethylhexyl) oxy] benzo [1,2-b: 4, 5-b '] dithiophene-2,6-diyl] [3-fluoro-2-[(2-ethylhexyl) carbonyl] thieno [3,4-b] thiophenediyl]]), PCPDTBT (poly [2,6- ( 4,4-bis- (2-ethylhexyl) -4H-cyclopenta [2,1-b; 3,4-b '] dithiophene) -alt-4,7- (2,1,3-benzothiadiazole)]), PC 61 BM [6,6] -phenyl-C 61 -butyric acid methyl ester) and an organic-inorganic composite tandem solar cell, characterized in that at least one member selected from the group consisting of PC 71 BM.
The organic-inorganic composite tandem solar cell of claim 1, wherein the back electrode layer is one selected from the group consisting of aluminum, silver, gold, chromium, palladium, graphene, carbon nanotubes, and silver nanowires. .
상기 투명전극층 상부에 무기계 광활성층을 적층하는 단계(단계 2);
상기 무기계 광활성층 상부에 산화인듐주석 전자수송층을 적층하는 단계(단계 3);
상기 전자수송층 상부에 그래핀 옥사이드 정공수송층을 적층하는 단계(단계 4);
상기 정공수송층 상부에 유기계 광활성층을 적층하는 단계(단계 5); 및
상기 유기계 광활성층 상부에 후면전극층을 적층하는 단계(단계 6)를 포함하는 것을 특징으로 하는 중간층이 삽입된 유·무기 복합형 탠덤 태양전지의 제조방법.
Coating a transparent electrode layer on the substrate (step 1);
Stacking an inorganic photoactive layer on the transparent electrode layer (step 2);
Stacking an indium tin oxide electron transport layer on the inorganic photoactive layer (step 3);
Stacking a graphene oxide hole transport layer on the electron transport layer (step 4);
Stacking an organic photoactive layer on the hole transport layer (step 5); And
A method of manufacturing an organic / inorganic hybrid tandem solar cell in which an intermediate layer is inserted, comprising the step (step 6) of stacking a rear electrode layer on the organic photoactive layer.
8. The method of claim 7, wherein the substrate is a glass or plastic substrate.
The method of claim 7, wherein the transparent electrode layer is aluminum-doped zinc oxide (AZO; Aluminum-zinc oxide (ZnO: Al), indium tin oxide (ITO; indium-tin oxide), zinc oxide (ZnO), aluminum tin oxide (ATO; Aluminium-tin oxide; SnO 2 : Al), fluorine-doped tin oxide (FTO), silver nanowires, graphene, carbon nanotubes and PEDOT: PSS The manufacturing method of the organic-inorganic composite tandem solar cell in which the intermediate | middle layer is inserted which is one or more types chosen.
The method of claim 7, wherein the inorganic photoactive layer is a p-type amorphous silicon layer, i-type amorphous silicon layer and n-type amorphous silicon layer, characterized in that the manufacturing of the intermediate layer-inserted organic-inorganic hybrid tandem solar cell Way.
The method of manufacturing an organic-inorganic composite tandem solar cell having an interlayer inserted therein, further comprising a heat treatment at 100 to 300 ° C. after the step 4.
The method of claim 7, wherein the organic photoactive layer is PBDTTT-C (poly [4,8-bis-alkyloxybenzo [1,2-b: 4,5-b '] dithiophene-2,6-diyl-alt- [alkyl thieno [3,4-b] thiophene-2-carboxylate] -2,6-diyl), PTB7 (Poly [[4,8-bis [(2-ethylhexyl) oxy] benzo [1,2-b: 4, 5-b '] dithiophene-2,6-diyl] [3-fluoro-2-[(2-ethylhexyl) carbonyl] thieno [3,4-b] thiophenediyl]]), PCPDTBT (poly [2,6- ( 4,4-bis- (2-ethylhexyl) -4H-cyclopenta [2,1-b; 3,4-b '] dithiophene) -alt-4,7- (2,1,3-benzothiadiazole)]), Preparation of organic-inorganic composite tandem solar cell having an interlayer inserted therein, characterized in that it is at least one selected from the group consisting of PC 61 BM [6,6] -phenyl-C 61 -butyric acid methyl ester) and PC 71 BM. Way.
The organic-inorganic-inorganic intermediate layer of claim 7, wherein the back electrode layer is one selected from the group consisting of aluminum, silver, gold, chromium, palladium, graphene, carbon nanotubes, and silver nanowires. Method for manufacturing a composite tandem solar cell.
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