CN110061244A - 一种柔性的无隔膜的线型燃料电池的制备方法 - Google Patents
一种柔性的无隔膜的线型燃料电池的制备方法 Download PDFInfo
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Abstract
本发明属于线型燃料电池技术领域,具体涉及一种柔性的无隔膜的线型燃料电池的制备方法。通过碳纳米管膜加捻负载催化剂得到(CNT)@Fe3[Co(CN)6]2阴极电极,碳纳米管膜加捻包覆镍粉得到CNT@镍颗粒阳极电极,与H2O2的燃料电解液集成在硅胶管中制备成柔性线型燃料电池。本发明的柔性线型燃料电池,可产生0.88V的开路电压,同时具有非常好的柔性,可编织进衣物等纺织品中,在便携式供能领域具有非常好的应用前景。
Description
技术领域
本发明属于线型燃料电池技术领域,具体涉及一种柔性的无隔膜的线型燃料电池的制备方法。
背景技术
可穿戴电子产品因其在健康监测、智能皮肤和传感器等领域的广阔前景而备受关注。为了给这些可穿戴电子设备提供动力,灵活的电源是必不可少的。线状储能系统是可穿戴电子产品的理想储能系统,因为纤维和/或纱线重量轻、柔韧和可编织。因此,线状储能器件的研究也付出了巨大的努力,包括线状锂离子电池、超级电容器、太阳能电池等。然而,由于线状可穿戴燃料电池在组装、膜、电解液、催化剂等方面的困难,目前开展的研究很少。
燃料电池是一类转换效率高、能量高的动力装置,它通过阴极和阳极表面的还原和氧化反应将化学能转化为电能。因此,实现柔性线形燃料电池在柔性可穿戴电子和纺织领域具有重要意义。然而,传统燃料电池的流场和集流器通常是刚性的、沉重的、不灵活的,如金属板或石墨板,不能集成或编织成柔性电子或纺织品。同时,传统燃料电池的膜结构对线形器件的设计也缺乏可靠性和难度。为此,我们希望从以下两个方面来设计和制造一种线状柔性燃料电池:一是制备一种负载纳米催化颗粒的线状柔性集电极;另一种是探索基于无膜单室燃料电池的反应机理。
发明内容
本发明要解决的技术问题是:实现燃料电池的线型化,微型化,可便携化等技术问题,从而提供一种柔性的无隔膜的线型燃料电池的制备方法。
本发明解决其技术问题所采用的技术方案是将催化剂负载在碳纳米管纱线上,利用双氧水既能充当还化剂燃料又能充当氧化剂的特性,使得阴阳极可以在同一个腔室内从而避免使用隔膜,同时使用包覆间隔纱线的方式来避免阴阳极短路。
上述柔性的无隔膜的线型燃料电池的制备方法包括如下步骤:
(1)称取FeSO4·7H2O和K3[Co(CN)6]试剂分别配制成水溶液,混合后在磁力搅拌下得到悬浮液,过滤留下沉淀,用去离子水洗涤沉淀,真空低温烘干得到催化剂Fe3[Co(CN)6]2。
(2)将碳纳米管膜从碳纳米管森林上拉出来,叠上不同的层数后,卷成圆柱状,将步骤(1)中所述的催化剂Fe3[Co(CN)6]2与乙醇溶液配成一定浓度的溶液,然后将所述的催化剂溶液均匀的滴涂到圆柱状的碳膜上,然后在电机的辅助下,加捻成均匀的(CNT)@Fe3[Co(CN)6]2阴极电极纱线。
(3)将所述的碳纳米管膜铺在玻璃片上,然后将纳米镍粉超声分散在DMF溶液中,然后将所得分散液均匀滴涂到纳米碳膜上,在电机的辅助下,加捻制成CNT@镍颗粒阳极电极纱线。
(4)等CNT@镍颗粒阳极电极纱线自然烘干后,在两个同步电机辅助下,在CNT@镍颗粒阳极电极纱线表面包覆一层聚丙烯(PP)单丝,得到CNT@镍@PP电极。
(5)称取双氧水溶液,高氯酸溶液,氯化钠盐,配制成燃料电解液。
(6)将所述的(CNT)@Fe3[Co(CN)6]2阴极电极纱线和CNT@镍@PP电极加捻在一起,装进硅胶管中注入电解液,从而制备成柔性的线型的双氧水燃料电池。
作为本发明的一个优选的实施例,步骤(1)中FeSO4·7H2O和K3[Co(CN)6]水溶液的浓度分别为0.2mol/l和0.15mol/l。所述的混合体积比1:1,所述的磁力搅拌转速为240转/分钟。所述的真空低温烘干的时间为6-10小时,所述的真空低温烘干的温度为40℃。
作为本发明的一个优选的实施例,步骤(2)中所述的碳纳米管膜的长度为15cm,宽度为2.5cm,层数为10层。所述的催化剂的浓度为5mg/ml,所述的滴加的催化剂溶液的量为1ml。所述的电机加捻的转速为100转/分钟,所述的加捻时间为1min。
作为本发明的一个优选的实施例,步骤(3)中所述的碳纳米管膜的长度为15cm,宽度为2.5cm,层数为10层。所述的分散液中,纳米镍粉的浓度为20mg/ml,所滴加的量为2ml。所述的电机加捻的转速为100转/分钟,所述的加捻时间为1min。
作为本发明的一个优选的实施例,步骤(4)中所述的两个同步电机的转数为50转/分钟,所述的PP单丝的直径为100微米。
作为本发明的一个优选的实施例,步骤(5)中所述的双氧水的浓度为0.03mol/l,所述的高氯酸溶液的浓度0.15mol/l,所述的氯化钠溶液为0.1mol/l,所述的3种溶液的混合体积比1:1:1。
作为本发明的一个优选的实施例,步骤(6)中所述的硅胶管的内径为0.1mm,长度为10-20cm。
本发明的有益效果是:方法简单,效率高,稳定性好,有利于实现工业化大生产。
具体表现为:
1.利用碳纳米管薄膜紧紧包覆着催化剂颗粒,加捻后的纱线,在弯折的过程中也会保持非常好的柔性和稳定性。
2.绝缘的聚丙烯间隔纱的使用保证了线型燃料电池在弯折过程中不会出现阴阳极接触短路的现象。
3.线型燃料电池的可编织性,使得便携式燃料电池在纺织品应用成为可能。
4.硅胶管的封装保证了电池的抗酸碱能力和安全性。
附图说明
图1本发明所制备的阳极电极的SEM图。
图2本发明所制备的阴极电极的SEM图。
图3本发明所制备的线型燃料电池的示意图。
图4本发明所制备的线型燃料电池的器件图。
图5本发明所制备的线型燃料电池的性能图。
具体实施方式
为使本发明的上述目的、特征和优点能够更加明显易懂,下面结合附图和具体实施方式对本发明作进一步详细的说明。
此处所称的“一个实施例”或“实施例”是指可包含于本发明至少一个实现方式中的特定特征、结构或特性。在本说明书中不同地方出现的“在一个实施例中”并非均指同一个实施例,也不是单独的或选择性的与其他实施例互相排斥的实施例。另外,需要说明的是,FeSO4·7H2O、K3[Co(CN)6]和NaCl,质量分数纯度为99.99%wt,高氯酸和乙醇(分析纯AR)双氧水的浓度为30%wt。DMF表示N甲基吡咯烷酮(分析纯AR)。
实施例1
(1)称取FeSO4·7H2O和K3[Co(CN)6]试剂分别配制成0.2mol/L和0.15mol/L的20ml水溶液,将FeSO4·7H2O水溶液缓慢加入到K3[Co(CN)6]水溶液中在240转/分钟的磁力搅拌下得到悬浮液,过滤留下沉淀,将沉淀用用去离子水离心洗涤3-5次后,在40℃的真空烘箱中烘干8h得到催化剂Fe3[Co(CN)6]2。
(2)将碳纳米管膜从碳纳米管森林上拉出来,长度为15cm,宽度为2.5cm,叠上10层数后,卷成圆柱状,将步骤(1)中所述的催化剂与乙醇溶液配成一定5mg/mL的溶液,然后量取1ml所述的催化剂溶液均匀的滴涂到圆柱状的碳膜上,然后在100转/分钟的电机的辅助下,加捻1min,加捻成均匀的(CNT)@Fe3[Co(CN)6]2阴极电极纱线。
(3)将碳纳米管膜铺在玻璃片上,长度为15cm,宽度为2.5cm,叠上10层,然后将纳米镍粉超声分散在DMF溶液中,制备成20mg/ml的分散液,然后称取2ml所述分散液均匀滴涂到纳米碳膜上,在100转/分钟电机的加捻下,加捻1min制成CNT@镍颗粒阳极电极纱线。
(4)等CNT@镍颗粒纱线自然烘干后,在两个转数为50转/分钟的同步电机辅助下,将一根直径100微米的聚丙烯(PP)单丝包覆在其表面。得到CNT@镍@PP电极。
(5)称取配制0.3mol/l双氧水,0.15mol/l高氯酸,0.1mol/l氯化钠混合水溶液,3种溶液的混合体积比1:1:1,配制成燃料电解液。
(6)将所述的(CNT)@Fe3[Co(CN)6]2和CNT@镍@PP电极加捻在一起,装进硅胶管中注入电解液,从而制备成柔性的线型的双氧水燃料电池。
实施例2
(1)称取FeSO4·7H2O和K3[Co(CN)6]试剂分别配制成0.20mol/L和0.15mol/L的20ml水溶液,将FeSO4·7H2O水溶液缓慢加入到K3[Co(CN)6]水溶液中在240转/分钟的磁力搅拌下得到悬浮液,过滤留下沉淀,将沉淀用用去离子水离心洗涤3-5次后,在25℃的真空烘箱中烘干8h得到催化剂Fe3[Co(CN)6]2。
(2)将碳纳米管膜从碳纳米管森林上拉出来,长度为15cm,宽度为3cm,叠上15层数后,卷成圆柱状,将步骤(1)中所述的催化剂与乙醇溶液配成一定5mg/mL的溶液,然后量取1ml所述的催化剂溶液均匀的滴涂到圆柱状的碳膜上,然后在100转/分钟的电机的辅助下,加捻2min,加捻成均匀的(CNT)@Fe3[Co(CN)6]2阴极电极纱线。
(3)将碳纳米管膜铺在玻璃片上,长度为15cm,宽度为3cm,叠上10层,然后将纳米镍粉超声分散在DMF溶液中,制备成20mg/ml的分散液,然后称取2ml所述分散液均匀滴涂到纳米碳膜上,在100转/分钟电机的加捻下,加捻1min制成CNT@镍颗粒阳极电极纱线。
(4)等CNT@镍颗粒纱线自然烘干后,在两个转数为25转/分钟的同步电机辅助下,将一根直径100微米的聚丙烯(PP)单丝包覆在其表面。得到CNT@镍@PP电极。
(5)称取配制0.3mol/l双氧水,0.15mol/l高氯酸,0.1mol/l氯化钠混合水溶液,3种溶液的混合体积比1:1:1,配制成燃料电解液。
(6)将所述的(CNT)@Fe3[Co(CN)6]2和CNT@镍@PP电极加捻在一起,装进硅胶管中注入电解液,从而制备成柔性的线型的双氧水燃料电池。
实施例3
(1)称取FeSO4·7H2O和K3[Co(CN)6]试剂分别配制成0.20mol/L和0.15mol/L的20ml水溶液,将FeSO4·7H2O水溶液缓慢加入到K3[Co(CN)6]水溶液中在240转/分钟的磁力搅拌下得到悬浮液,过滤留下沉淀,将沉淀用用去离子水离心洗涤3-5次后,在常温下烘干8h得到催化剂Fe3[Co(CN)6]2。
(2)将碳纳米管膜从碳纳米管森林上拉出来,长度为15cm,宽度为4cm,叠上15层数后,卷成圆柱状,将步骤(1)中所述的催化剂与乙醇溶液配成一定5mg/mL的溶液,然后量取1ml所述的催化剂溶液均匀的滴涂到圆柱状的碳膜上,然后在100转/分钟的电机的辅助下,加捻1.5min,加捻成均匀的(CNT)@Fe3[Co(CN)6]2阴极电极纱线。
(3)将碳纳米管膜铺在玻璃片上,长度为15cm,宽度为4cm,叠上10层,然后将纳米镍粉超声分散在DMF溶液中,制备成20mg/ml的分散液,然后称取2ml所述分散液均匀滴涂到纳米碳膜上,在100转/分钟电机的加捻下,加捻1min制成CNT@镍颗粒阳极电极纱线。
(4)等CNT@镍颗粒纱线自然烘干后,在两个转数为50转/分钟的同步电机辅助下,将一根直径100微米的聚丙烯(PP)单丝包覆在其表面。得到CNT@镍@PP电极。
(5)称取配制0.3mol/l双氧水,0.15mol/l高氯酸,0.1mol/l氯化钠混合水溶液,3种溶液的混合体积比1:1:1,配制成燃料电解液。
(6)将所述的(CNT)@Fe3[Co(CN)6]2和CNT@镍@PP电极加捻在一起,装进硅胶管中注入电解液,从而制备成柔性的线型的双氧水燃料电池。
3个实施例的差异在于,不同的宽度和不同的层数保证了负载的分布不一样,负载的质量比不一样,实施例1为最佳实施例。
根据图1,2可知,我们负载的催化剂都均匀的包覆在碳纳米管纱线上,图3是我们制备的燃料电池的示意图,从图上可以看出我们的器件的结构部分,图4是我们实际制作出来的线型燃料电池的器件图,图5是最终得到的器件的性能图,由图5可知,我们的线型燃料电池可以提供一个稳定的0.89V电压,功率密度可达6.2mW cm-2。
Claims (7)
1.一种柔性的无隔膜的线型燃料电池的制备方法,其特征在于,具体步骤如下:
(1)称取FeSO4·7H2O和K3[Co(CN)6]试剂分别配制成水溶液,混合后在磁力搅拌下得到悬浮液,过滤留下沉淀,用去离子水洗涤沉淀,真空低温烘干得到催化剂Fe3[Co(CN)6]2;
(2)将碳纳米管膜从碳纳米管森林上拉出来,叠上不同的层数后,卷成圆柱状,将步骤(1)中所述的催化剂Fe3[Co(CN)6]2与乙醇溶液配成一定浓度的溶液,然后将所述的催化剂溶液均匀的滴涂到圆柱状的碳膜上,然后在电机的辅助下,加捻成均匀的(CNT)@Fe3[Co(CN)6]2阴极电极纱线;
(3)将所述的碳纳米管膜铺在玻璃片上,然后将纳米镍粉超声分散在DMF溶液中,然后将所得分散液均匀滴涂到纳米碳膜上,在电机的辅助下,加捻制成CNT@镍颗粒阳极电极纱线;
(4)等CNT@镍颗粒阳极电极纱线自然烘干后,在两个同步电机辅助下,在CNT@镍颗粒阳极电极纱线表面包覆一层聚丙烯(PP)单丝,得到CNT@镍@PP电极;
(5)称取双氧水溶液,高氯酸溶液,氯化钠盐,配制成燃料电解液;
(6)将所述的(CNT)@Fe3[Co(CN)6]2阴极电极纱线和CNT@镍@PP电极加捻在一起,装进硅胶管中注入电解液,从而制备成柔性的线型的双氧水燃料电池。
2.如权利要求1所述的一种柔性的无隔膜的线型燃料电池的制备方法,其特征在于,步骤(1)中FeSO4·7H2O和K3[Co(CN)6]水溶液的浓度分别为0.2mol/l和0.15mol/l;所述的混合体积比1:1,所述的磁力搅拌转速为240转/分钟;所述的真空低温烘干的时间为6-10小时,所述的真空低温烘干的温度为40℃。
3.如权利要求1所述的一种柔性的无隔膜的线型燃料电池的制备方法,其特征在于,步骤(2)中所述的碳纳米管膜的长度为15cm,宽度为2.5cm,层数为10层;所述的催化剂的浓度为5mg/ml,所述的滴加的催化剂溶液的量为1ml;所述的电机加捻的转速为100转/分钟,所述的加捻时间为1min。
4.如权利要求1所述的一种柔性的无隔膜的线型燃料电池的制备方法,其特征在于,步骤(3)中所述的碳纳米管膜的长度为15cm,宽度为2.5cm,层数为10层;所述的分散液中,纳米镍粉的浓度为20mg/ml,所滴加的量为2ml;所述的电机加捻的转速为100转/分钟,所述的加捻时间为1min。
5.如权利要求1所述的一种柔性的无隔膜的线型燃料电池的制备方法,其特征在于,步骤(4)中所述的两个同步电机的转数为50转/分钟,所述的PP单丝的直径为100微米。
6.如权利要求1所述的一种柔性的无隔膜的线型燃料电池的制备方法,其特征在于,步骤(5)中所述的双氧水的浓度为0.03mol/l,所述的高氯酸溶液的浓度0.15mol/l,所述的氯化钠溶液为0.1mol/l,所述的3种溶液的混合体积比1:1:1。
7.如权利要求1所述的一种柔性的无隔膜的线型燃料电池的制备方法,其特征在于,步骤(6)中所述的硅胶管的内径为0.1mm,长度为10-20cm。
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