CN106920856A - A kind of electroluminescent and photovoltaic double-function device and preparation method thereof - Google Patents
A kind of electroluminescent and photovoltaic double-function device and preparation method thereof Download PDFInfo
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Abstract
Description
技术领域technical field
本发明涉及一种电致发光和光伏双功能器件及其制备方法，属于半导体光电子器件技术领域。The invention relates to an electroluminescent and photovoltaic dual-function device and a preparation method thereof, belonging to the technical field of semiconductor optoelectronic devices.
背景技术Background technique
钙钛矿太阳能电池具有制备工艺简单、成本低、效率高等优点。自从2012年PARK课题组首次报道寿命500小时以上、效率达到9.7%的全固态钙钛矿太阳能电池以来，钙钛矿太阳能电池受到了学界和产业界的极大关注，发展迅速，还被《Science》评选为2013年十大科学突破之一。钙钛矿太阳能电池在短短几年里发展迅速，目前报道的钙钛矿太阳能电池的效率已经突破了20%。Perovskite solar cells have the advantages of simple preparation process, low cost and high efficiency. Since the PARK research group first reported an all-solid-state perovskite solar cell with a service life of more than 500 hours and an efficiency of 9.7% in 2012, perovskite solar cells have received great attention from academia and industry, and have developed rapidly. "Selected as one of the top ten scientific breakthroughs in 2013. Perovskite solar cells have developed rapidly in just a few years, and the reported efficiency of perovskite solar cells has exceeded 20%.
钙钛矿太阳能电池的研究方兴未艾，研究人员又发现钙钛矿同时是一种性能优异的发光材料，具备一系列突出的优点： (1)发光效率高。光致发光效率可达 80%以上； (2)带隙和光谱简单可调。通过调节不同卤元素的比例可以轻松实现发光峰从可见覆盖到近红外区； (3)光谱色纯高，发光光谱半峰宽度~20 nm；(4)制备成本低廉、工艺简单，可通过溶液法实现大面积生产。钙钛矿电致发光器件的系列优点及其展现出的优异性能显示出它在照明与平板显示领域中巨大的应用前景。The research on perovskite solar cells is in the ascendant, and researchers have discovered that perovskite is also an excellent light-emitting material with a series of outstanding advantages: (1) High luminous efficiency. The photoluminescent efficiency can reach more than 80%; (2) The band gap and spectrum are easily adjustable. By adjusting the ratio of different halogen elements, the luminescence peak can be easily covered from the visible to the near-infrared region; (3) The spectral color purity is high, and the half-peak width of the luminescence spectrum is ~20 nm; (4) The preparation cost is low, the process is simple, and it can be obtained by solution method to achieve large-scale production. The series of advantages and excellent performance of perovskite electroluminescent devices show its great application prospects in the field of lighting and flat panel display.
虽然已经证明钙钛矿同时是一种性能优异的光伏和发光材料，但是传统的钙钛矿器件绝大多数为单一功能器件，只能提供发光或者光伏中的单一功能，器件集成度差。开发兼顾发光和光伏功的双功能器件对于研究钙钛矿器件研究和产业化应用都具有重要的意义。Although it has been proved that perovskite is a photovoltaic and light-emitting material with excellent performance at the same time, most of the traditional perovskite devices are single-function devices, which can only provide a single function in light-emitting or photovoltaic, and the device integration is poor. The development of dual-functional devices that take into account both luminescence and photovoltaic power is of great significance for the research and industrial application of perovskite devices.
发明内容Contents of the invention
为了解决背景技术中所述的问题，本发明提供了一种电致发光和光伏双功能器件及其制备方法。为了实现上述目的，本发明提出以下技术方案：In order to solve the problems described in the background technology, the present invention provides an electroluminescent and photovoltaic dual-function device and a preparation method thereof. In order to achieve the above object, the present invention proposes the following technical solutions:
一种电致发光和光伏双功能器件及其制备方法，其特征在于，器件结构由下到上依次包括透明导电衬底、第一修饰层、钙钛矿活性层、第二修饰层和反射电极组成。An electroluminescent and photovoltaic dual-function device and its preparation method, characterized in that the device structure sequentially includes a transparent conductive substrate, a first modification layer, a perovskite active layer, a second modification layer and a reflective electrode from bottom to top composition.
进一步的，所述的透明导电衬底为生长有ITO的玻璃衬底，方块电阻10-20Ω，透过率在80-90%。Further, the transparent conductive substrate is a glass substrate grown with ITO, the sheet resistance is 10-20Ω, and the transmittance is 80-90%.
进一步的，所述的第一修饰层为PEDOT:PSS，PEDOT:PSS通过溶液旋转涂覆的方法制备，厚度在30-50 nm。Further, the first modification layer is PEDOT:PSS, and PEDOT:PSS is prepared by solution spin coating, with a thickness of 30-50 nm.
进一步的，所述的钙钛矿活性层为CsPbBr3和CH3NH3PbBr3中的一种， 钙钛矿活性层通过溶液旋转涂覆的方法制备，厚度在50-300 nm。Further, the perovskite active layer is one of CsPbBr 3 and CH 3 NH 3 PbBr 3 , and the perovskite active layer is prepared by solution spin coating with a thickness of 50-300 nm.
进一步的，所述的第二修饰层为TPBI、Bphen、BCP中的一种，厚度在10-50 nm。Further, the second modification layer is one of TPBI, Bphen, and BCP, with a thickness of 10-50 nm.
进一步的，所述的反射电极为Au、Ag、Al或者它们的合金中的一种，反射电极厚度在50-200 nm。Further, the reflective electrode is one of Au, Ag, Al or their alloys, and the thickness of the reflective electrode is 50-200 nm.
进一步的，器件的制备还包括以下步骤：Further, the preparation of the device also includes the following steps:
(1) 透明导电衬底处理：透明导电衬底采用丙酮、玻璃清洗剂依次清洗，然后在丙酮、去离子水、异丙醇中各超声处理10分钟，用氮气吹干后紫外灯照射处理10分钟待用；(1) Treatment of transparent conductive substrate: The transparent conductive substrate was cleaned with acetone and glass cleaning agent in sequence, then ultrasonically treated in acetone, deionized water, and isopropanol for 10 minutes, dried with nitrogen, and then irradiated with ultraviolet light for 10 minutes. minutes to use;
(2)第一修饰层制备：在透明导电衬底上旋转涂覆PEDOT:PSS的水溶液，转速为低俗500rpm，旋转5秒，高速3000-4000rpm，旋转30-50秒；涂覆完毕后，在120摄氏度的加热板上加热退火处理20分钟；(2) Preparation of the first modification layer: Spin-coat the aqueous solution of PEDOT:PSS on the transparent conductive substrate at a low speed of 500rpm for 5 seconds, and at a high speed of 3000-4000rpm for 30-50 seconds; Heat annealing treatment on a heating plate at 120 degrees Celsius for 20 minutes;
(3)钙钛矿光敏层制备：室温下配置有机无机杂化钙钛矿前驱体溶液，将定量的CsPbBr3或者CH3NH3PbBr3在二甲基亚砜(DMSO)中溶解，60℃条件下加热12小时至溶解充分，得到钙钛矿前驱体溶液；利用匀胶机将前驱体溶液旋转涂覆在第一修饰层上；转速2000-3000rpm，旋转时间40-60秒；钙钛矿活性层旋转涂覆完毕的瞬间，在钙钛矿活性层上滴加20ml的氯仿溶液继续旋转涂覆，转速2000-3000rpm，旋转时间20-30秒；完成后将器件转移至90℃的加热板上退火10-30分钟；(3) Preparation of perovskite photosensitive layer: prepare an organic-inorganic hybrid perovskite precursor solution at room temperature, dissolve quantitative CsPbBr 3 or CH 3 NH 3 PbBr 3 in dimethyl sulfoxide (DMSO), and heat at 60°C Heating under the conditions for 12 hours until fully dissolved to obtain a perovskite precursor solution; use a homogenizer to spin coat the precursor solution on the first modification layer; the rotation speed is 2000-3000rpm, and the rotation time is 40-60 seconds; the perovskite At the moment when the spin coating of the active layer is completed, add 20ml of chloroform solution dropwise on the perovskite active layer to continue the spin coating, the rotation speed is 2000-3000rpm, and the rotation time is 20-30 seconds; after completion, transfer the device to a heating plate at 90°C Upper annealing for 10-30 minutes;
(4)第二修饰层制备：完成后将器件转移至真空镀膜机中，待真空度小于5×10-4Pa的条件下后，通过热蒸发的方法继续沉积第二修饰层；(4) Preparation of the second modification layer: after completion, transfer the device to a vacuum coating machine, and continue to deposit the second modification layer by thermal evaporation after the vacuum degree is less than 5×10 -4 Pa;
(5)制备反射电极：在第二修饰层上通过热蒸发的方法沉积一层的Al、Ag或者Au作为反射电极，获得钙钛矿电致发光和光伏双功能器件。(5) Preparation of reflective electrode: a layer of Al, Ag or Au is deposited on the second modified layer by thermal evaporation as a reflective electrode to obtain a perovskite electroluminescent and photovoltaic dual-function device.
附图说明Description of drawings
图1为本发明的电致发光和光伏双功能器件结构示意图Fig. 1 is the structure schematic diagram of electroluminescent and photovoltaic bifunctional device of the present invention
具体实施方式detailed description
实例一：一种电致发光和光伏双功能器件及其制备方法，器件结构示意如图1所示，器件结构由下到上依次包括透明导电衬底、第一修饰层、钙钛矿活性层、第二修饰层和反射电极组成。具体地，器件结构为ITO（方块电阻10Ω，透过率在85%）/PEDOT:PSS（40 nm）/CsPbBr3 （200 nm）/TPBI （20）/Al （100 nm），器件的制备包括步骤：Example 1: An electroluminescent and photovoltaic dual-function device and its preparation method. The device structure is shown in Figure 1. The device structure includes a transparent conductive substrate, a first modification layer, and a perovskite active layer from bottom to top. , a second modification layer and a reflective electrode. Specifically, the device structure is ITO (sheet resistance 10Ω, transmittance 85%)/PEDOT:PSS (40 nm)/CsPbBr 3 (200 nm)/TPBI (20)/Al (100 nm), and the preparation of the device includes step:
第一步、基底清洗：The first step, base cleaning:
透明导电衬底使用丙酮、玻璃清洗剂依次清洗，丙酮、去离子水、异丙醇中各超声处理10分钟，氮气吹干后紫外灯照射处理10分钟；The transparent conductive substrate is cleaned with acetone and glass cleaner in sequence, ultrasonically treated in acetone, deionized water, and isopropanol for 10 minutes, and then dried with nitrogen and then irradiated with ultraviolet light for 10 minutes;
第二步、第一修饰层制备：The second step, preparation of the first modification layer:
在透明导电衬底上旋转涂覆PEDOT:PSS的水溶液，转速为低俗500rpm，旋转5秒，高速3500rpm，旋转35秒；涂覆完毕后，在120℃的加热板上加热退火处理20分钟；Spin-coat the aqueous solution of PEDOT:PSS on the transparent conductive substrate at a low speed of 500rpm for 5 seconds, and at a high speed of 3500rpm for 35 seconds; after coating, heat and anneal on a heating plate at 120°C for 20 minutes;
第三步、钙钛矿光敏层制备：The third step, preparation of perovskite photosensitive layer:
室温下配置无机钙钛矿前驱体溶液，将定量的CsPbBr3在DMSO中溶解，浓度为1 M ,60℃条件下加热12小时至溶解充分，得到CsPbBr3钙钛矿前驱体溶液；利用匀胶机将前驱体溶液旋转涂覆在第一修饰层上；转速2000rpm，旋转时间60秒；钙钛矿活性层旋转涂覆完毕的瞬间，在钙钛矿活性层上滴加20ml的氯仿溶液继续旋转涂覆，转速2000rpm，旋转时间20秒；完成后将器件转移至90℃的加热板上退火10分钟，去除多余的溶剂，形成结晶性能良好的CsPbBr3钙钛矿薄膜；Prepare an inorganic perovskite precursor solution at room temperature, dissolve a certain amount of CsPbBr 3 in DMSO with a concentration of 1 M, and heat at 60°C for 12 hours until fully dissolved to obtain a CsPbBr 3 perovskite precursor solution; The machine spin-coats the precursor solution on the first modification layer; the rotation speed is 2000rpm, and the rotation time is 60 seconds; the moment the perovskite active layer is spin-coated, 20ml of chloroform solution is dripped on the perovskite active layer and continues to rotate Coating, rotation speed 2000rpm, rotation time 20 seconds; after completion, transfer the device to a heating plate at 90°C for annealing for 10 minutes, remove excess solvent, and form a CsPbBr 3 perovskite film with good crystallization properties;
第四步、第二修饰层制备：The fourth step, preparation of the second modification layer:
生长上述器件转移至真空镀膜机中，待真空度小于5×10-4Pa的条件下后，通过热蒸发的方法继续沉积20nm的TPBI作为第二修饰层；The above-mentioned devices are grown and transferred to a vacuum coating machine. After the vacuum degree is less than 5×10-4Pa, continue to deposit 20nm TPBI as the second modification layer by thermal evaporation;
第五步：制备反射电极：Step 5: Prepare reflective electrodes:
制备反射电极：真空度小于5×10-4的真空条件下，在第二修饰层上通过热蒸发的方法沉积一层100 nm的Al作为反射电极，获得钙钛矿电致发光和光伏双功能器件；Preparation of reflective electrode: Under vacuum conditions with a vacuum degree of less than 5×10-4, a layer of 100 nm Al is deposited on the second modified layer by thermal evaporation as a reflective electrode to obtain perovskite electroluminescence and photovoltaic dual functions device;
第六步、测试：Step 6. Test:
在AM1.5模拟太阳能光照射下测得钙钛矿电致发光和光伏双功能器件的开路电压1.3V，填充因子0.40，短路电流2.8mA/cm2，能量转换效率为1.45%。加电条件下，测得器件启亮电压为3.2V，最大亮度为2870cd/cm2，发光峰位于527nm左右，半峰宽为21nm。器件实现电致发光和光伏的双功能。Under AM1.5 simulated solar light irradiation, the open-circuit voltage of the perovskite electroluminescent and photovoltaic dual-function device is 1.3V, the fill factor is 0.40, the short-circuit current is 2.8mA/cm 2 , and the energy conversion efficiency is 1.45%. Under the power-on condition, the measured turn-on voltage of the device is 3.2V, the maximum brightness is 2870cd/cm 2 , the luminescence peak is located at about 527nm, and the half-peak width is 21nm. The device realizes the dual functions of electroluminescence and photovoltaic.
实例二：一种电致发光和光伏双功能器件及其制备方法，器件结构由下到上依次包括透明导电衬底、第一修饰层、钙钛矿活性层、第二修饰层和反射电极组成。具体地，器件结构为ITO（方块电阻10Ω，透过率在85%）/PEDOT:PSS（40 nm）/ CH3NH3PbBr3（300 nm）/Bphen (20 nm) /Ag （100 nm），器件的制备包括步骤：Example 2: An electroluminescence and photovoltaic dual-function device and its preparation method. The device structure consists of a transparent conductive substrate, a first modification layer, a perovskite active layer, a second modification layer and a reflective electrode from bottom to top. . Specifically, the device structure is ITO (sheet resistance 10Ω, transmittance 85%)/PEDOT:PSS (40 nm)/ CH 3 NH 3 PbBr 3 (300 nm)/Bphen (20 nm) /Ag (100 nm) , the preparation of the device includes the steps:
第一步、基底清洗：同实例一；The first step, substrate cleaning: same as Example 1;
第二步、第一修饰层制备：同实例一；The second step, preparation of the first modification layer: same as Example 1;
第三步、钙钛矿光敏层制备：The third step, preparation of perovskite photosensitive layer:
室温下配置有机无机杂化钙钛矿前驱体溶液，将定量的CH3NH3PbBr3在DMSO中溶解，浓度为1.2 M, 60℃条件下加热12小时至溶解充分，得到CH3NH3PbBr3钙钛矿前驱体溶液；利用匀胶机将前驱体溶液旋转涂覆在第一修饰层上；转速2500rpm，旋转时间50秒；钙钛矿活性层旋转涂覆完毕的瞬间，在钙钛矿活性层上滴加20ml的氯仿溶液继续旋转涂覆，转速2000转，旋转时间30秒；完成后将器件转移至90℃的加热板上退火15分钟，去除多余的溶剂，形成结晶性能良好的CH3NH3PbBr3钙钛矿薄膜；Prepare an organic-inorganic hybrid perovskite precursor solution at room temperature, dissolve quantitative CH 3 NH 3 PbBr 3 in DMSO with a concentration of 1.2 M, and heat at 60°C for 12 hours until fully dissolved to obtain CH 3 NH 3 PbBr 3. Perovskite precursor solution; Spin coat the precursor solution on the first modification layer by using a homogenizer; the rotation speed is 2500rpm, and the spin time is 50 seconds; Add 20ml of chloroform solution dropwise on the active layer and continue to spin coating at a speed of 2000 rpm for 30 seconds; after completion, transfer the device to a heating plate at 90°C for annealing for 15 minutes to remove excess solvent and form CH with good crystallization properties. 3 NH 3 PbBr 3 perovskite film;
第四步、第二修饰层制备：The fourth step, preparation of the second modification layer:
生长上述器件转移至真空镀膜机中，待真空度小于5×10-4Pa的条件下后，通过热蒸发的方法继续沉积20nm的Bphen作为第二修饰层；The above-mentioned devices were grown and transferred to a vacuum coating machine. After the vacuum degree was less than 5×10 -4 Pa, continue to deposit 20nm of Bphen as the second modification layer by thermal evaporation;
第五步：制备反射电极：Step 5: Prepare reflective electrodes:
制备反射电极：真空度小于5×10-4的真空条件下，在第二修饰层上通过热蒸发的方法沉积一层100 nm的Ag作为反射电极，获得钙钛矿电致发光和光伏双功能器件；Preparation of reflective electrode: Under vacuum conditions with a vacuum degree of less than 5×10 -4 , a layer of 100 nm Ag is deposited on the second modified layer by thermal evaporation as a reflective electrode to obtain perovskite electroluminescence and photovoltaic dual functions device;
第六步、测试：Step 6. Test:
在AM1.5模拟太阳能光照射下测得钙钛矿电致发光和光伏双功能器件的开路电压1.25V，填充因子0.32，短路电流3.2mA/cm2，能量转换效率为1.28%。加电条件下，测得器件启亮电压为3.3V，最大亮度为3870cd/cm2，发光峰位于525nm左右，半峰宽为20nm。器件实现电致发光和光伏的双功能。Under AM1.5 simulated solar light irradiation, the open circuit voltage of the perovskite electroluminescent and photovoltaic dual-function device is 1.25V, the fill factor is 0.32, the short circuit current is 3.2mA/cm 2 , and the energy conversion efficiency is 1.28%. Under the power-on condition, the measured turn-on voltage of the device is 3.3V, the maximum brightness is 3870cd/cm 2 , the luminescence peak is at about 525nm, and the half-peak width is 20nm. The device realizes the dual functions of electroluminescence and photovoltaic.
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