聚合物体异质结太阳能电池的器件优化及光伏性能研究
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摘要
随着全球经济发展、人口数量激增,今后全世界能源消费总量将不断提高,而煤、天然气、石油等传统能源消费总量终有一天将会到达极限。能源危机的日益突显,使人类意识到寻找可再生能源的重要性。太阳能作为绿色、环境友好型能源的代表,成为各国学术界和工业界的研究热点。尽管无机硅太阳能电池具有高的光电转换效率,但由于其制造条件苛刻,生产成本高,不易加工及非柔性等缺点限制了其大规模民用化进程。而以聚合物材料为活性层的聚合物体异质结太阳能电池具有材料来源广、成本低、柔性、可大面积器件及制备工艺简单等特点而被人们广泛关注。
聚合物体异质结太阳能电池器件性能与活性层给体材料的能级结构、带隙、对光的吸收、成膜性、分子量、载流子迁移率密切相关,此外还与如活性层复合薄膜表面形貌、活性层与电极的界面接触等器件优化过程密不可分。本论文主要围绕研究上述影响因素与聚合物体异质结太阳能电池器件性能的关系并以此展开工作。通过选择窄带隙宽吸收的共轭聚合物作为给体材料增加其对入射光的俘获,考察其分子结构与器件性能之间的关系；通过对器件活性层和电极界面进行修饰和采用不同溶剂、不同给受体掺杂比例、不同活性层厚度成膜等方法对器件进行优化并研究其与器件性能之间的关系；使用具有表面等离子体增强吸收效应的银圆盘纳米晶对阳极进行修饰,并以提高器件对光的捕获；论文的详细内容如下：
1.在论文的引言部分详细对聚合物体异质结太阳能电池进行综述：包括研究发展历程、工作原理、器件结构、器件性能表征参数与测试仪器、器件性能影响因素等方面的大量研究工作。
2.以噻吩单元代替苯单元作为桥联基团,将给电子基团芴与吸电子基团苯并噻二唑通过Heck偶联反应进行共聚,合成了一种新型的窄带隙聚芴共轭聚合物PF-TBT[poly(fluorenevinylenealt-4,7-dithienyl-2,1,3-benzothiadiazole)]。噻吩单元以其优良的光学性质、高的载流子迁移率、强的给电子能力和高的化学稳定性而被广泛的应用在聚合物体异质结太阳能电池中。PF-TBT具有宽的吸收光谱,其吸收带边接近700nm,光学带隙为1.82eV。我们以聚合物PF-TBT作为给体材料,富勒烯衍生物PC61BM[(6,6)-phenyl-C61-butyric acid methyl ester]为受体材料,制备了器件结构为ITO/poly(3,4-ethylenedioxythiophene):poly(styenesulfonate) (PEDOT:PSS)/PF-TBT:PC6,BM/LiF/Al的聚合物体异质结太阳能电池,系统地研究了PF-TBT的光物理性质,热学性质和电化学性质,利用空间电荷限制电流方法(SCLC)计算了聚合物的空穴载流子迁移率,利用原子力显微镜(AFM)和透射电子显微镜(TEM)分析了PF-TBT与PC61BM共混膜的表面形貌。在光强100mW/cm2AM1.5G模拟太阳光照射下,Jsc=3.97mAcm-2, FF=0.35, Voc=0.86 V,能量转换效率达1.18%。
3.以聚苯撑乙烯类共轭聚合物PP-DBT [poly(phenylenevinylene-alt-4,7-diphenyl-2,1,3-benzothiadiazole)]为给体材料,富勒烯衍生物PC71BM [(6,6)-phenyl-C71-butyric acid methyl ester]为受体材料,制备了器件结构为ITO/PEDOT:PSS/PP-DBT:PC71BM/ZnO/Al的聚合物体异质结太阳能电池。对器件进行了一系列优化：对活性层的厚度、给体材料与受体材料掺杂比例进行调节；选择氯苯、氯仿、邻二氯苯为溶剂,考察其对活性层复合薄膜表面形貌的影响；采用ZnO纳米晶对活性层薄膜与电极界面进行修饰。利用空间电荷限制电流方法(SCLC)计算了聚合物PP-DBT的空穴载流子迁移率,利用透射电子显微镜(TEM)和原子力显微镜(AFM)分析了PP-DBT:PC71BM共混膜的表面形貌。在光强100mW/cm2AM1.5G模拟太阳光照射下,器件的Jsc=7.46mAcm-2, FF=0.50,Voc=0.90 V,能量转换效率达3.36%。
4.利用静电自组装方法将具有局域表面等离子体共振效应的银纳米圆盘组装在ITO基底,并以聚噻吩衍生物P3HT[poly(3-hexylthiophene)]为给体材料,以富勒烯衍生物PC61BM为受体材料,制备了器件结构为[ITO/silver nanodisks/ PEDOT:PSS/P3HT:PC61BM/LiF/Al的太阳能电池,在光强100mW/cm2 AMI.5G模拟太阳光照射下,Jsc=9.24±0.09mAcm-2,FF=0.60±0.01, Voc=0.61±0.01V,能量转换效率达3.46±0.07%。通过银纳米圆盘的等离子体共振效应有效提高聚合物活性层中P3HT对入射光的俘获,与无银纳米圆盘修饰的器件相比,能量转换效率由原来的2.72±0.08%提升至3.46±0.07%。
As the global energy demand continues to increase every year, the limiting supply of today's main energy sources (i.e. oil, coal, natural gas) and their detrimental long-term effects on the natural balance on our planet, force people develop some renewable energy sources. Harvesting energy directly from the sunlight using photovoltaic (PV) technology is being widely recognized as an essential component of future global energy production. Although the photovoltaic cells based on inorganic materials have been proved to convert sunlight to electricity efficiently, the high cost for manufacture limits them to be widely used. Polymer solar cells, based on polymer materials as active layer, possess the advantage of plenty of choices for active layer, low cost, flexibility and easily being large-scale etc., which attracts great attention in recent years.
The photovoltaic performance of devices is strongly dependent on the band gap, energy levels, light harvesting, film forming ability, molecular weight, charge carrier mobility of donor and acceptor materials. In addition, the surface morphology of active composite layer and the interface modification between active layer and electrodes could also influence the power conversion efficiency of the solar cell.
The thesis focus on how the above factors such as the band gap of materials, the surface morphology of active layer, the interface modificaton between active layer and electrodes affect the performance of solar cells. We used a low band gap donor-acceptor (D-A) conjugated polymer as donors and PC61BM as acceptor, meanwhile, we investigated the relation between the molecular structure and their device performance; we optimize the solar cell by interface modification, different acceptor material, solvents and blend ratios; We used the plasmonic silver nanodisks modificate the indium tin oxide (ITO) and fabricate the polymer solar cells. More details are now listed below.
1. First of all, the important steps during the development history of polymer bulk-heterojunction (BHJ) solar cells, work principle, the device structure, characterization and related measure instruments are described, and we also reviewed the recent work focusing on synthesis of materials, device physics and related processing and so on.
2. A new low band gap copolymer containing dialkylfluorene and 4,7-dithienyl-2,1,3-benzothiadiazole (TBT), poly(fluorenevinylene-alt-4,7-dithienyl-2,1,3-benzothiadiazole) (PF-TBT) was synthesized by Heck cross-coupling polymerization. The copolymer exhibited broad absorption band with an absorption edge close to 700 nm and optical band gap of 1.82 eV. Cyclic voltammetric study indicated that the relatively low HOMO energy level assured a higher open circuit voltage (Voc) when PF-TBT is used as donor material in photovoltaic cell. The Bulk heterojunction (BHJ) solar cell by using PF-TBT as donor and [6,6]-phenyl C61-butyric acid methyl ester (PCBM) as acceptor with the structure of ITO/ [poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)](PEDOT:PSS)/copolymer: PC61BM/LiF/Al exhibited a Voc of 0.86 V, short-circuit current (Jsc) of 3.97 mA/cm2, fill factor (FF) of 0.35, and power conversion efficiency (PCE) of 1.18% under one sun of AM 1.5 solar simulator illumination (100mW/cm2).
3. Bulk heterojunction organic photovoltaic cells using blends of [poly(phenylenevinylene-alt-4,7-diphenyl-2,1,3-benzothiadiazole)] and [6.6]-phenyl-C71-butyric acid methyl ester (PC71BM) as electron donor and acceptor were fabricated and characterized. By optimizing the donor/acceptor ratio and the thickness of the active layer, the choice of solvent (1,2-dichlorobenzene, chloroform and chlorobenzene) and using the interface modification of ZnO nanoparticles, the solar cells with the structure of ITO/PEDOT:PSS/PP-DBT:PC71BM/ZnO/Al exhibited a Voc of 0.96 V, short-circuit current (Jsc) of 7.46 mA/cm2, fill factor (FF) of 0.50, and power conversion efficiency (PCE) of 3.36% under one sun of AM 1.5 solar simulator illumination (100mW/cm2).
4. We report the efficiency enhancement of polymer solar cells by incorporating a silver nanodisks self-assembled layer which was grown on the indium tin oxide (ITO) surface by the electrostatic interaction between the silver particles and modified ITO. Polymer solar cells with a structure of ITO (silver nanodisks)/PEDOT:PSS/ poly(3-hexylthiophene)(P3HT):PC6iBM)/LiF/Al exhibited an open circuit voltage (Voc) of 0.61±0.01V, short-circuit current density (Jsc) of 9.24±0.09mAcm-2, fill factor (FF) of 0.60±0.01, and power conversion efficiency (PCE) of 3.46±0.07% under one sun of simulated air mass 1.5 global (AM 1.5 G) irradiation (100mW/cm2). The PCE was increased from 2.72±0.08% to 3.46±0.07% as compared to the devices without silver nanodisks self-assembled layer, mainly resulting from the improved photocurrent density as a result of the excited localized surface plasmon resonance induced by the silver nanodisks.
聚合物体异质结太阳能电池器件性能与活性层给体材料的能级结构、带隙、对光的吸收、成膜性、分子量、载流子迁移率密切相关,此外还与如活性层复合薄膜表面形貌、活性层与电极的界面接触等器件优化过程密不可分。本论文主要围绕研究上述影响因素与聚合物体异质结太阳能电池器件性能的关系并以此展开工作。通过选择窄带隙宽吸收的共轭聚合物作为给体材料增加其对入射光的俘获,考察其分子结构与器件性能之间的关系；通过对器件活性层和电极界面进行修饰和采用不同溶剂、不同给受体掺杂比例、不同活性层厚度成膜等方法对器件进行优化并研究其与器件性能之间的关系；使用具有表面等离子体增强吸收效应的银圆盘纳米晶对阳极进行修饰,并以提高器件对光的捕获；论文的详细内容如下：
1.在论文的引言部分详细对聚合物体异质结太阳能电池进行综述：包括研究发展历程、工作原理、器件结构、器件性能表征参数与测试仪器、器件性能影响因素等方面的大量研究工作。
2.以噻吩单元代替苯单元作为桥联基团,将给电子基团芴与吸电子基团苯并噻二唑通过Heck偶联反应进行共聚,合成了一种新型的窄带隙聚芴共轭聚合物PF-TBT[poly(fluorenevinylenealt-4,7-dithienyl-2,1,3-benzothiadiazole)]。噻吩单元以其优良的光学性质、高的载流子迁移率、强的给电子能力和高的化学稳定性而被广泛的应用在聚合物体异质结太阳能电池中。PF-TBT具有宽的吸收光谱,其吸收带边接近700nm,光学带隙为1.82eV。我们以聚合物PF-TBT作为给体材料,富勒烯衍生物PC61BM[(6,6)-phenyl-C61-butyric acid methyl ester]为受体材料,制备了器件结构为ITO/poly(3,4-ethylenedioxythiophene):poly(styenesulfonate) (PEDOT:PSS)/PF-TBT:PC6,BM/LiF/Al的聚合物体异质结太阳能电池,系统地研究了PF-TBT的光物理性质,热学性质和电化学性质,利用空间电荷限制电流方法(SCLC)计算了聚合物的空穴载流子迁移率,利用原子力显微镜(AFM)和透射电子显微镜(TEM)分析了PF-TBT与PC61BM共混膜的表面形貌。在光强100mW/cm2AM1.5G模拟太阳光照射下,Jsc=3.97mAcm-2, FF=0.35, Voc=0.86 V,能量转换效率达1.18%。
3.以聚苯撑乙烯类共轭聚合物PP-DBT [poly(phenylenevinylene-alt-4,7-diphenyl-2,1,3-benzothiadiazole)]为给体材料,富勒烯衍生物PC71BM [(6,6)-phenyl-C71-butyric acid methyl ester]为受体材料,制备了器件结构为ITO/PEDOT:PSS/PP-DBT:PC71BM/ZnO/Al的聚合物体异质结太阳能电池。对器件进行了一系列优化：对活性层的厚度、给体材料与受体材料掺杂比例进行调节；选择氯苯、氯仿、邻二氯苯为溶剂,考察其对活性层复合薄膜表面形貌的影响；采用ZnO纳米晶对活性层薄膜与电极界面进行修饰。利用空间电荷限制电流方法(SCLC)计算了聚合物PP-DBT的空穴载流子迁移率,利用透射电子显微镜(TEM)和原子力显微镜(AFM)分析了PP-DBT:PC71BM共混膜的表面形貌。在光强100mW/cm2AM1.5G模拟太阳光照射下,器件的Jsc=7.46mAcm-2, FF=0.50,Voc=0.90 V,能量转换效率达3.36%。
4.利用静电自组装方法将具有局域表面等离子体共振效应的银纳米圆盘组装在ITO基底,并以聚噻吩衍生物P3HT[poly(3-hexylthiophene)]为给体材料,以富勒烯衍生物PC61BM为受体材料,制备了器件结构为[ITO/silver nanodisks/ PEDOT:PSS/P3HT:PC61BM/LiF/Al的太阳能电池,在光强100mW/cm2 AMI.5G模拟太阳光照射下,Jsc=9.24±0.09mAcm-2,FF=0.60±0.01, Voc=0.61±0.01V,能量转换效率达3.46±0.07%。通过银纳米圆盘的等离子体共振效应有效提高聚合物活性层中P3HT对入射光的俘获,与无银纳米圆盘修饰的器件相比,能量转换效率由原来的2.72±0.08%提升至3.46±0.07%。
As the global energy demand continues to increase every year, the limiting supply of today's main energy sources (i.e. oil, coal, natural gas) and their detrimental long-term effects on the natural balance on our planet, force people develop some renewable energy sources. Harvesting energy directly from the sunlight using photovoltaic (PV) technology is being widely recognized as an essential component of future global energy production. Although the photovoltaic cells based on inorganic materials have been proved to convert sunlight to electricity efficiently, the high cost for manufacture limits them to be widely used. Polymer solar cells, based on polymer materials as active layer, possess the advantage of plenty of choices for active layer, low cost, flexibility and easily being large-scale etc., which attracts great attention in recent years.
The photovoltaic performance of devices is strongly dependent on the band gap, energy levels, light harvesting, film forming ability, molecular weight, charge carrier mobility of donor and acceptor materials. In addition, the surface morphology of active composite layer and the interface modification between active layer and electrodes could also influence the power conversion efficiency of the solar cell.
The thesis focus on how the above factors such as the band gap of materials, the surface morphology of active layer, the interface modificaton between active layer and electrodes affect the performance of solar cells. We used a low band gap donor-acceptor (D-A) conjugated polymer as donors and PC61BM as acceptor, meanwhile, we investigated the relation between the molecular structure and their device performance; we optimize the solar cell by interface modification, different acceptor material, solvents and blend ratios; We used the plasmonic silver nanodisks modificate the indium tin oxide (ITO) and fabricate the polymer solar cells. More details are now listed below.
1. First of all, the important steps during the development history of polymer bulk-heterojunction (BHJ) solar cells, work principle, the device structure, characterization and related measure instruments are described, and we also reviewed the recent work focusing on synthesis of materials, device physics and related processing and so on.
2. A new low band gap copolymer containing dialkylfluorene and 4,7-dithienyl-2,1,3-benzothiadiazole (TBT), poly(fluorenevinylene-alt-4,7-dithienyl-2,1,3-benzothiadiazole) (PF-TBT) was synthesized by Heck cross-coupling polymerization. The copolymer exhibited broad absorption band with an absorption edge close to 700 nm and optical band gap of 1.82 eV. Cyclic voltammetric study indicated that the relatively low HOMO energy level assured a higher open circuit voltage (Voc) when PF-TBT is used as donor material in photovoltaic cell. The Bulk heterojunction (BHJ) solar cell by using PF-TBT as donor and [6,6]-phenyl C61-butyric acid methyl ester (PCBM) as acceptor with the structure of ITO/ [poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)](PEDOT:PSS)/copolymer: PC61BM/LiF/Al exhibited a Voc of 0.86 V, short-circuit current (Jsc) of 3.97 mA/cm2, fill factor (FF) of 0.35, and power conversion efficiency (PCE) of 1.18% under one sun of AM 1.5 solar simulator illumination (100mW/cm2).
3. Bulk heterojunction organic photovoltaic cells using blends of [poly(phenylenevinylene-alt-4,7-diphenyl-2,1,3-benzothiadiazole)] and [6.6]-phenyl-C71-butyric acid methyl ester (PC71BM) as electron donor and acceptor were fabricated and characterized. By optimizing the donor/acceptor ratio and the thickness of the active layer, the choice of solvent (1,2-dichlorobenzene, chloroform and chlorobenzene) and using the interface modification of ZnO nanoparticles, the solar cells with the structure of ITO/PEDOT:PSS/PP-DBT:PC71BM/ZnO/Al exhibited a Voc of 0.96 V, short-circuit current (Jsc) of 7.46 mA/cm2, fill factor (FF) of 0.50, and power conversion efficiency (PCE) of 3.36% under one sun of AM 1.5 solar simulator illumination (100mW/cm2).
4. We report the efficiency enhancement of polymer solar cells by incorporating a silver nanodisks self-assembled layer which was grown on the indium tin oxide (ITO) surface by the electrostatic interaction between the silver particles and modified ITO. Polymer solar cells with a structure of ITO (silver nanodisks)/PEDOT:PSS/ poly(3-hexylthiophene)(P3HT):PC6iBM)/LiF/Al exhibited an open circuit voltage (Voc) of 0.61±0.01V, short-circuit current density (Jsc) of 9.24±0.09mAcm-2, fill factor (FF) of 0.60±0.01, and power conversion efficiency (PCE) of 3.46±0.07% under one sun of simulated air mass 1.5 global (AM 1.5 G) irradiation (100mW/cm2). The PCE was increased from 2.72±0.08% to 3.46±0.07% as compared to the devices without silver nanodisks self-assembled layer, mainly resulting from the improved photocurrent density as a result of the excited localized surface plasmon resonance induced by the silver nanodisks.
引文
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