CN102298984A - 用于制备敏化太阳电池中硫化亚铜对电极的浆料及方法 - Google Patents
用于制备敏化太阳电池中硫化亚铜对电极的浆料及方法 Download PDFInfo
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- CN102298984A CN102298984A CN2010102178621A CN201010217862A CN102298984A CN 102298984 A CN102298984 A CN 102298984A CN 2010102178621 A CN2010102178621 A CN 2010102178621A CN 201010217862 A CN201010217862 A CN 201010217862A CN 102298984 A CN102298984 A CN 102298984A
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- counter electrode
- slurry
- sulfide
- cuprous sulfide
- cuprous
- Prior art date
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- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
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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
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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Abstract
本发明公开了一种用于制备敏化太阳电池中硫化亚铜对电极的浆料,其中含有重量比为0.01%~85%的硫化亚铜、重量比为0%~80%的复合物、重量比为0~25%的添加剂,其余为溶剂,所述复合物选自碳材料或导电聚合物中的至少一种。本发明所用的基于硫化亚铜的对电极制作简便,性能优越,稳定性好,适用于商品化的量子点敏化太阳电池。
Description
技术领域
本发明涉及量子点敏化太阳能电池制造领域,尤其涉及一种以硫化亚铜为主要活性成分的敏化太阳电池对电极及其制作方法。
背景技术
人类进入二十一世纪以来,面临的能源问题日趋严峻,世界范围内都在积极努力地寻求解决办法,可再生能源因此也受到了各国政府的重视,其中太阳能更是以取之不尽、用之不竭的优点备受关注,因而太阳能电池也成为了新能源研究领域内的热点。染料敏化太阳能电池(DSC)作为近年来发展起来的一种新型太阳能电池,以其优良的性能和经济、便捷的制备方法引发了全球范围内的研究热潮。但由于染料价格方面的因素,限制了DSC成本的进一步降低。近一段时间来,作为染料敏化剂的替代品,量子点敏化剂也逐渐受到了各方的重视。半导体量子点不仅具有稳定性好、价格低廉、消光系数大等敏化剂所必需的特点,还可以通过控制其尺寸实现光学带隙的调节,以多种量子点复合敏化来达到对太阳光谱最大化的利用。同时,光激发后发生在量子点内部的多激子效应可以使一个光子产生多个电子空穴对,显著提升太阳电池的量子效率,可以得到更高的光电转换效率。
然而,由于相关研究刚刚起步,量子点敏化太阳电池的效率并没有达到理想的状态。为了进一步提高电池的转换效率,需要对电池的各个组成部分进行优化,其中对电极材料的选择和制备是影响电池效率的关键因素之一。目前常用的对电极包括金对电极(Advanced Functional Materials,19,604,2009)、白金对电极(Applied Physics Letters,96,63501,2010)、碳对电极(Electrochemistry Communications,12,327,2010)以及通过腐蚀铜片得到的硫化亚铜对电极(Nanotechnology,20,295204,2009)。但是,这几种对电极都存在着一定的问题,比如贵金属对电极的成本较高,碳对电极虽然价格低廉但活性仍不能达到满足电池高效率工作的水平,通过腐蚀铜片得到的硫化亚铜对电极尽管克服了成本和活性两方面的问题,但是由于电解液持续不断地腐蚀铜片,使电解液组分产生变化并且也在封装过程中也存在难以密封的问题,从而使电池的性能不稳定,因此很难达到实用化的需要。
发明内容
因此,本发明的目的在于克服上述现有技术存在的缺陷,提供一种能够提高与基底的粘结性及稳定性的用于制备敏化太阳电池中硫化亚铜对电极的浆料及方法。
本发明的目的是通过以下技术方案实现的:
根据本发明的第一方面,提供一种用于制备敏化太阳电池中硫化亚铜对电极的浆料,其中,含有重量比为0.01%~85%的硫化亚铜、重量比为0%~80%的复合物、重量比为0~25%的添加剂,其余为溶剂,所述复合物选自碳材料或导电聚合物中的至少一种。
在上述浆料中,所述硫化亚铜重量比优选为45~85%。
在上述浆料中,所述复合物重量比优选为30%~80%。
在上述浆料中,所述碳材料选自鳞片状石墨、导电炭黑、活性炭、石墨烯、单壁碳纳米管、多壁碳纳米管、球状石墨、硬碳材料或富勒烯及其衍生物中的至少一种。
在上述浆料中,所述导电聚合物选自聚乙炔、聚吡咯、聚噻吩、聚苯胺、聚对苯、聚苯乙烯,聚噻吩乙烯、聚呋喃乙烯、聚苯硫醚、聚苯乙炔、聚硒吩、聚呋喃、聚氮取代苯胺、聚氮取代吡咯、聚联苯胺、聚吲哚、聚噻吩吡咯、聚芴、聚吡啶或聚偏氟乙烯中的至少一种。
在上述浆料中,所述添加剂包括粘结剂、粘度调节剂和表面活性剂中的至少一种。其中,
根据本发明的第二方面,提供一种采用上述浆料制备的硫化亚铜对电极,其中,所述对电极包括衬底及其上的催化活性材料,所述催化活性材料包括硫化亚铜。
在上述对电极中,所述衬底包括导电玻璃、玻璃、有机玻璃、金属、合金、石墨、导电聚合物、聚对苯二甲酸乙二醇酯(PET)、聚萘二甲酸乙二醇酯(PEN)、尼龙(PA)、聚碳酸酯(PC)、聚甲醛(POM)、聚对苯二甲酸丁二醇酯(PBT)、聚苯醚(PPO/PPE)、聚乙烯(PE)或聚丙烯(PP)。
根据本发明的第三方面,提供一种采用上述浆料制备敏化太阳电池中硫化亚铜对电极的方法,该方法包括以下步骤:
将原料按配比配制为浆料,将此浆料通过刮涂、喷涂或丝网印刷的方法沉积于衬底上成膜,再经过热处理。
根据本发明的第四方面,提供一种原位制备敏化太阳电池中硫化亚铜对电极的方法,该方法包括通过使含有铜源和硫源的材料反应,得到附着在导电衬底上的硫化亚铜对电极。
在上述方法中,所述使含有铜源和硫源的材料反应包括同时将含有铜源和硫源的材料作为反应物在导电衬底上进行反应或将导电衬底分别与含有铜源和硫源的体系先后接触。
与现有技术相比,本发明的优点在于:
1、使硫化亚铜与基底粘结更牢固,增强了其稳定性,并便于电池封装;
2、降低了电池的制造成本。
具体实施方式
以下参照具体的实施例来说明本发明。本领域技术人员能够理解,这些实施例仅用于说明本发明的目的,其不以任何方式限制本发明的范围。
[实施例1]:原位制备硫化亚铜对电极
采用溶剂热法在透明导电玻璃表面原位沉积硫化亚铜,反应条件为以乙二醇为溶剂,20mM醋酸铜和10mM硫脲为反应物,在180℃条件下溶剂热沉积5小时;然后取出透明导电玻璃,用纯水冲净后60℃真空干燥12小时,即得到硫化亚铜对电极。
将上述实施例1的对电极组装成电池进行光电转换效率测试,其中光阳极为纳米二氧化钛多孔薄膜,敏化量子点为CdS和CdSe,电解液为1M硫化钠和1M单质硫的水溶液,测试结果如表1所示。作为对比,在导电玻璃上分别沉积了白金(热解法)、黄金(热蒸镀)、碳(刮涂法)对电极及电解液腐蚀铜片所得到的对电极,其光电效率结果如表1所示。结果表明以硫化亚铜作为催化活性成分的对电极,电池的短路电流、填充因子、光电转换效率比现有白金、黄金、碳及腐蚀铜片对电极的更高,是一种更加优良的对电极。
表1
对电极 | 电流密度(mA cm-2) | 开路电压(mV) | 填充因子 | 光电转换效率(%) |
硫化亚铜 | 10.68 | 497 | 0.581 | 3.08 |
金 | 7.57 | 484 | 0.269 | 0.98 |
白金 | 6.73 | 374 | 0.271 | 0.68 |
碳 | 6.48 | 387 | 0.495 | 1.24 |
腐蚀铜片所得对电极 | 9.39 | 501 | 0.489 | 2.3 |
由上述方法得到的量子点敏化太阳电池对电极,其催化活性显著优于其它目前使用的对电极,因此提升了电池的电流密度、开路电压、填充因子及光电转化效率。
[实施例2~51]:采用含有硫化亚铜的浆料制备硫化亚铜对电极
将硫化亚铜按表2中所示的不同质量分数分散于不同类型及含量的溶剂中,配制成浆料;然后采用高压喷涂的方式将该浆料沉积于加热到120℃的石墨纸表面上,得到对电极。将对电极按上述实施例1的方法组装成电池测试其电池效率,结果如下。
表2
从以上结果可以看出,当硫化亚铜沉积在石墨衬底上作为对电极时电池性能出色,且优选是质量百分比为45%~85%时,更优选为55%~65%。
[实施例52~69]:采用含有硫化亚铜、粘结剂和表面活性剂的浆料制备硫化亚铜对电极
按表2中的配比,以丙三醇为溶剂,配制浆料,然后将其丝网印刷在柔性ITO/PET上,80℃干燥后制得硫化亚铜对电极。按上述实施例1的方法组装成电池进行电池效率测试,测试结果如下所示。
表3
上述Tx-100为商品可得的由Sigma-Aldrich公司制造的表面活性剂TritonX 100的缩写。上述数据表明,低温条件下制备的对电极同样具备良好的性能,该方法尤其适用于难以经受高温处理的柔性衬底,同时由于粘结剂的存在,使对电极与衬底的粘结更加牢固,拓展了对电极的应用范围。
[实施例70~99]:采用含有硫化亚铜、导电复合物、粘结剂的浆料制备硫化亚铜对电极
按表4中的配比,以松油醇为溶剂,配制浆料,然后采用刮涂法将其沉积于普通玻璃上。同样按上述实施例1的方法组装成电池进行电池效率测试,测试结果如下所示。
表4
从以上结果可以看出,利用上述沉积在绝缘衬底上的对电极制备的电池的效率也比现有白金、黄金、碳及硫化亚铜对电极的光电转换效率高。复合物的质量百分比优选为30%~80%,更优选为40%~60%。复合浆料的催化活性和导电性均能满足使用需要。
[实施例100~122]:采用包括硫化亚铜、复合物、粘结剂、粘度调节剂和表面活性剂的浆料制备硫化亚铜对电极
按表5中的配比,以丙三醇为溶剂,复合物为石墨与炭黑(质量比8∶2)的混合物,钛酸四异丙酯为粘结剂(质量分数2%),制备浆料,然后采用丝网印刷法将其沉积于普通玻璃上,400℃热处理30分钟后得到对电极。同样按上述实施例1的方法组装成电池进行电池效率测试,测试结果如下所示。
表5
从以上结果可以看出,利用简便易行的丝网印刷法,可以方便地制备性能优异的对电极,适合于商业化生产的需要。
从以上实施例1~122可以看出,本发明的用于制备量子点敏化太阳能电池的硫化亚铜对电极的方法基本包括两类:
第一类为在导电衬底上原位生长硫化亚铜(如实施例1)。然而,在上述实施例1中通过醋酸铜和硫脲配制硫化亚铜的方法仅为示意性的,在本发明的其他实施例中,还可以采用诸如氯化亚铜的乙腈溶液和硫化氢的水溶液等不同的铜源和硫源作为反应物在导电衬底上进行反应,使包括硫化亚铜在内的反应产物附着在衬底上得到对电极,或者将导电衬底分别与含有铜源和硫源的材料先后接触(例如先后浸沾到含有铜源和硫源的反应液中),得到附着在衬底上的硫化亚铜对电极。另外,也可以使用离子层气体反应法、浸渍法等来替代溶剂热法,由于这些方法都是在反应过程中,硫化亚铜直接生长在透明导电层表面,无需经过进一步处理即可直接组装电池,不仅提高了电池转换效率,还大大方便使用。
第二类为配制成浆料通过诸如刮涂、丝网印刷、高压喷涂、电喷涂和超声喷雾等方法将该浆料沉积于衬底之上,然后经过一定温度下的热处理。在本发明的实施例中,所述浆料包括0.01%~85%(重量)的硫化亚铜、0%~80%(重量)的复合物、0~25%(重量)的添加剂,其余为溶剂,其中复合物选自碳材料或导电聚合物中的至少一种,所述碳材料和导电聚合物可以以任意比例混合。在一个实施例中,所述硫化亚铜优选为45%~85%(重量),更优选为55%~65%。在另一个实施例中,所述复合物优选为30%~80%(重量),更优选为40%~60%。在本发明的再一个实施例中,热处理温度在20至500℃之间。以下详细列出各具体材料。
碳材料选自鳞片状石墨、导电炭黑、活性炭、石墨烯、单壁碳纳米管、多壁碳纳米管、球状石墨、硬碳材料或富勒烯及其衍生物中的至少一种。
导电聚合物选自聚乙炔、聚吡咯、聚噻吩、聚苯胺、聚对苯、聚苯乙烯,聚噻吩乙烯、聚呋喃乙烯、聚苯硫醚、聚苯乙炔、聚硒吩、聚呋喃、聚氮取代苯胺、聚氮取代吡咯、聚联苯胺、聚吲哚、聚噻吩吡咯、聚芴、聚吡啶或聚偏氟乙烯中的至少一种。
添加剂包括粘结剂、粘度调节剂和表面活性剂中的至少一种。进一步地,粘结剂选自固相粘结剂或液相粘结剂中的至少一种,其中固相粘结剂选自二氧化钛、氧化锌、三氧化二铝、氧化镁、二氧化锡、氧化镍、五氧化二钒、五氧化二铌、二氧化锆、三氧化二铬中的至少一种,液相粘结剂选自钛酸四异丙酯、钛酸四丁酯、四氯化钛、硫酸钛、硫酸锌、硝酸锌、醋酸锌、氯化锌、硬脂酸锌、乙酰丙醇锌、四氯化锡、硝酸锡、硝酸镁、氯化镁中的至少一种。粘度调节剂选自淀粉、甲基纤维素、乙基纤维素、纤维素醋酸酯、羧甲基纤维素钠、苯乙烯、聚乙二醇、聚丙二醇、聚丙三醇中的至少一种。表面活性剂选自商品TritonX 100,TritonX 405,TritonX 114,TritonCF 10,TritonDF 20,Triton 15-S-7,Triton 15-S-9中的一种或多种。在本发明的一个实施例中,粘结剂在浆料中的质量分数为0%~10%,粘度调节剂在浆料中的质量分数为0%~5%,表面活性剂在浆料中的质量分数为0%~10%
溶剂包括水或有机溶剂,其中有机溶剂选自松油醇、一缩二乙二醇、甲醇、乙醇、正丙醇、异丙醇、正丁醇、异丁醇、叔丁醇、正戊醇、异戊醇、正己醇、正庚醇、乙二醇、丙二醇、丙三醇、丙酮、环己烷、环己酮、戊烷、己烷、辛烷、醋酸甲酯、醋酸乙酯、醋酸丙酯、乙腈、吡啶、苯、苯酚、甲苯、二甲苯、薄荷酮、薄荷醇、N-甲基吡咯烷酮中的至少一种。
衬底可以包括导电玻璃、玻璃、有机玻璃、金属、合金、石墨、导电聚合物、聚对苯二甲酸乙二醇酯(PET)、聚萘二甲酸乙二醇酯(PEN)、尼龙(PA)、聚碳酸酯(PC)、聚甲醛(POM)、聚对苯二甲酸丁二醇酯(PBT)、聚苯醚(PPO/PPE)、聚乙烯(PE)或聚丙烯(PP)等。
对于本领域普通技术人员来说,应该理解,为了增加所沉积电极的粘附性和稳定性,可在浆料中加入添加剂,但这不是必需的。添加复合物的目的是使制备的对电极同时具有催化活性和导电性,这样就可以将浆料沉积在绝缘的衬底上,不仅节省了此前制备导电层的成本,还大大拓展了此种对电极的使用范围,为其今后的商业化生产提供了可能。
综上所述,本发明通过刮涂、丝网印刷、喷涂等方法使硫化亚铜简便牢固地沉积在各种衬底上的方法,不仅可以使电池获得很高的光电转换效率,而且方便了电池封装,同时具有良好的稳定性,为量子点敏化太阳电池的实用化提供了可能。此外,还可以通过适当调节所添加的复合物等,将此对电极沉积于各种导电或绝缘衬底之上,或者在低温下沉积于不耐高温的衬底之上,丰富了对电极的适用场合,这将有利地促进量子点敏化太阳电池的实用化。
尽管参照上述的实施例已对本发明作出具体描述,但是对于本领域的普通技术人员来说,应该理解可以在不脱离本发明的精神以及范围之内基于本发明公开的内容进行修改或改进,这些修改和改进都在本发明的精神以及范围之内。
Claims (10)
1.一种用于制备敏化太阳电池中硫化亚铜对电极的浆料,其特征在于含有重量比为0.01%~85%的硫化亚铜、重量比为0%~80%的复合物、重量比为0~25%的添加剂,其余为溶剂,其中所述复合物选自碳材料或导电聚合物中的至少一种。
2.根据权利要求1所述的浆料,其特征在于,所述硫化亚铜重量比为45~85%。
3.根据权利要求1所述的浆料,其特征在于,所述复合物重量比为30%~80%。
4.根据权利要求1所述的浆料,其特征在于,所述碳材料选自鳞片状石墨、导电炭黑、活性炭、石墨烯、单壁碳纳米管、多壁碳纳米管、球状石墨、硬碳材料或富勒烯及其衍生物中的至少一种。
5.根据权利要求1所述的浆料,其特征在于,所述导电聚合物选自聚乙炔、聚吡咯、聚噻吩、聚苯胺、聚对苯、聚苯乙烯,聚噻吩乙烯、聚呋喃乙烯、聚苯硫醚、聚苯乙炔、聚硒吩、聚呋喃、聚氮取代苯胺、聚氮取代吡咯、聚联苯胺、聚吲哚、聚噻吩吡咯、聚芴、聚吡啶或聚偏氟乙烯中的至少一种。
6.根据权利要求1所述的浆料,其特征在于,所述添加剂包括粘结剂、粘度调节剂和表面活性剂中的至少一种。
7.一种采用权利要求1至6中任一项所述浆料制备的硫化亚铜对电极,其特征在于,所述对电极包括衬底及其上的催化活性材料,所述催化活性材料包括硫化亚铜。
8.一种采用权利要求1至6中任一项所述浆料制备敏化太阳电池中硫化亚铜对电极的方法,该方法包括以下步骤:
将原料按配比配制为浆料,将此浆料通过刮涂、喷涂或丝网印刷的方法沉积于衬底上成膜,再经过热处理。
9.一种原位制备敏化太阳电池硫化亚铜对电极的方法,方法包括通过与含有铜源和硫源的体系反应,得到附着在导电衬底上的硫化亚铜对电极。
10.根据权利要求9所述的方法,其特征在于,所述与含有铜源和硫源的材料反应包括同时将含有铜源和硫源的材料作为反应物在导电衬底上进行反应或将导电衬底分别与含有铜源和硫源的体系先后接触得到。
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