CN111009589A - 氮化铜薄膜太阳能电池及其制备方法 - Google Patents
氮化铜薄膜太阳能电池及其制备方法 Download PDFInfo
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- CN111009589A CN111009589A CN201911106109.2A CN201911106109A CN111009589A CN 111009589 A CN111009589 A CN 111009589A CN 201911106109 A CN201911106109 A CN 201911106109A CN 111009589 A CN111009589 A CN 111009589A
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- 239000010949 copper Substances 0.000 title claims abstract description 87
- 229910052802 copper Inorganic materials 0.000 title claims abstract description 86
- -1 Copper nitride Chemical class 0.000 title claims abstract description 76
- 239000010409 thin film Substances 0.000 title claims abstract description 31
- 238000002360 preparation method Methods 0.000 title abstract description 14
- 239000010408 film Substances 0.000 claims abstract description 80
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims abstract description 59
- 229910052757 nitrogen Inorganic materials 0.000 claims abstract description 30
- 239000011521 glass Substances 0.000 claims abstract description 29
- 229910052709 silver Inorganic materials 0.000 claims abstract description 10
- 239000004332 silver Substances 0.000 claims abstract description 10
- 238000000034 method Methods 0.000 claims abstract description 6
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 54
- 238000004544 sputter deposition Methods 0.000 claims description 45
- 229910052786 argon Inorganic materials 0.000 claims description 27
- 239000000758 substrate Substances 0.000 claims description 23
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 12
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 9
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims description 8
- BUGBHKTXTAQXES-UHFFFAOYSA-N Selenium Chemical compound [Se] BUGBHKTXTAQXES-UHFFFAOYSA-N 0.000 claims description 7
- 239000011248 coating agent Substances 0.000 claims description 7
- 238000000576 coating method Methods 0.000 claims description 7
- 239000011777 magnesium Substances 0.000 claims description 7
- 229910052749 magnesium Inorganic materials 0.000 claims description 7
- 229910052711 selenium Inorganic materials 0.000 claims description 7
- 239000011669 selenium Substances 0.000 claims description 7
- 238000001704 evaporation Methods 0.000 claims description 3
- 239000007789 gas Substances 0.000 claims description 3
- 238000007738 vacuum evaporation Methods 0.000 claims description 3
- 238000000861 blow drying Methods 0.000 claims description 2
- 238000004140 cleaning Methods 0.000 claims description 2
- 238000004519 manufacturing process Methods 0.000 claims description 2
- 238000001755 magnetron sputter deposition Methods 0.000 abstract description 3
- 238000001228 spectrum Methods 0.000 abstract description 3
- 239000012495 reaction gas Substances 0.000 abstract description 2
- 239000000463 material Substances 0.000 description 6
- 238000004458 analytical method Methods 0.000 description 4
- 230000031700 light absorption Effects 0.000 description 4
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 2
- 230000005355 Hall effect Effects 0.000 description 2
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 238000004833 X-ray photoelectron spectroscopy Methods 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 125000004433 nitrogen atom Chemical group N* 0.000 description 2
- 230000003287 optical effect Effects 0.000 description 2
- 239000004065 semiconductor Substances 0.000 description 2
- 238000003860 storage Methods 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- 238000004506 ultrasonic cleaning Methods 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- MARUHZGHZWCEQU-UHFFFAOYSA-N 5-phenyl-2h-tetrazole Chemical compound C1=CC=CC=C1C1=NNN=N1 MARUHZGHZWCEQU-UHFFFAOYSA-N 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 1
- KTSFMFGEAAANTF-UHFFFAOYSA-N [Cu].[Se].[Se].[In] Chemical compound [Cu].[Se].[Se].[In] KTSFMFGEAAANTF-UHFFFAOYSA-N 0.000 description 1
- 238000004847 absorption spectroscopy Methods 0.000 description 1
- 229910021417 amorphous silicon Inorganic materials 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 238000007664 blowing Methods 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 229910021419 crystalline silicon Inorganic materials 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 238000000151 deposition Methods 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- 230000005525 hole transport Effects 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- AMGQUBHHOARCQH-UHFFFAOYSA-N indium;oxotin Chemical compound [In].[Sn]=O AMGQUBHHOARCQH-UHFFFAOYSA-N 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 1
- 231100000252 nontoxic Toxicity 0.000 description 1
- 230000003000 nontoxic effect Effects 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 125000003748 selenium group Chemical group *[Se]* 0.000 description 1
- 239000013077 target material Substances 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- 238000002834 transmittance Methods 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
- 239000011701 zinc Substances 0.000 description 1
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Abstract
本发明公开了一种氮化铜薄膜太阳能电池及其制备方法,电池自下而上包括如下结构:ITO玻璃\镁掺杂氮化铜薄膜\组分渐变氮化铜薄膜\硒掺杂氮化铜薄膜\ITO薄膜\银电极,其中组分渐变氮化铜薄膜中,氮的含量自下而上逐渐变大。本发明的氮化铜薄膜利用反应磁控溅射方法制备,通过调节反应气体(氮气)的流量,获得禁带宽度逐渐变化的氮化铜薄膜,拓宽了薄膜对太阳光吸收的光谱范围。
Description
技术领域
本发明属于薄膜太阳能电池技术领域,具体涉及一种氮化铜薄膜太阳能电池及其制备方法。
背景技术
尽管目前晶体硅太阳能电池占据了光伏市场的90%以上的份额,但是薄膜太阳能电池在建筑幕墙玻璃、汽车玻璃等方面应用具有明显的优势。目前薄膜太阳能电池主要有非晶硅薄膜电池、铜铟镓硒薄膜电池、碲化镉薄膜电池、钙钛矿薄膜电池等。但是目前这些薄膜电池在成本、环保、元素储量、稳定性等方面存在一定的局限性,因此,绿色环保、储量丰富、成本低廉的新型薄膜太阳能电池逐渐成为人们关注的热点,也是未来薄膜太阳能电池发展的主流方向。新型太阳能电池材料的一般要满足以下要求:(1)光吸收系数高;(2)带隙宽度为1.1~1.8eV;(3)对环境友好、地球上储量丰富、成本低;(4)制备工艺简单,能大规模、大面积生产;(4)长期稳定性号,没有明显的衰减。
近年来,无毒、廉价、储量丰富的氮化铜(Cu3N)新型光伏材料受到人们的青睐,对其光电特性已经展开了广泛的研究,但是作为薄膜太阳能电池还未见报道。氮化铜是由氮原子和铜原子以离子键与共价键共同存在的形式相结合的,具有较高的光学吸收系数,通过改变氮原子和铜原子比例来调节禁带宽度(1.2~1.8eV),非常适合作为薄膜太阳能电池材料。同时,氮化铜为简单二元化合物,可以在低温和简单工艺条件下实现高质量、大面积的薄膜生长。利用钛、锰、铁、钴、镍、锌等过渡金属掺杂,氮化铜的光电特性可以发生很大的改变,为氮化铜应用于光电器件打下来基础。
发明内容
本发明的目的是提供一种禁带宽度渐变的氮化铜薄膜太阳能电池及其制备方法。
为实现第一个发明目的,所采用的技术方案是这样的:
氮化铜薄膜太阳能电池,其特征在于:自下而上包括如下结构:ITO玻璃\镁掺杂氮化铜薄膜\组分渐变氮化铜薄膜\硒掺杂氮化铜薄膜\ITO薄膜\银电极,其中组分渐变氮化铜薄膜中,氮的含量自下而上逐渐变大。
所述的组分渐变氮化铜薄膜的厚度为500nm,分为10层,每层50nm,氮的含量自下而上逐渐变大。
为实现第二个发明目的,所采用的技术方案是这样的:
氮化铜薄膜太阳能电池的制备方法,其特征在于:包括以下步骤:
1)ITO玻璃衬底清洗吹干后放入溅射腔室内,玻璃基片的温度为80~110℃,通入氮气,氮气与氩气的流量比为1:1,氩气流速控制为10sccm,溅射腔压强为0.8Pa;铜靶的溅射功率固定为250W,镁靶的溅射功率为10~15W;至薄膜厚度为30~50nm;
2)待玻璃基片的温度降低到50~60℃以后,开始生长组分渐变氮化铜薄膜;溅射腔压强恒定为0.8Pa,铜靶的溅射功率维持在60W;氩气流速恒定为10sccm,氮气与氩气的流量比开始为1,每沉积50nm薄膜后改变一次氮气与氩气流量比,从1.2、1.5、1.9、2.5、3.3、4.2、5.2、6.3依次变化到7.5,以获得组分渐变的氮化铜薄膜;
3)玻璃基片温度上升至150~180℃,然后开始生长硒掺杂氮化铜薄膜;氮气与氩气的流量比为1:1,氩气流速控制为10sccm,溅射腔压强为0.8Pa;铜靶的溅射功率固定为250W,硒靶的溅射功率为10~15W,至薄膜厚度为20~30nm;
4)硒掺杂氮化铜薄膜生长结束以后,生长ITO薄膜;玻璃基片的温度为200℃,溅射工作气体为氩气,流量为30sccm,溅射腔压强为0.8Pa;ITO靶的溅射功率为80W,ITO薄膜的生长厚度为80nm;
5)ITO生长结束后,从溅射腔取出样品,在表面放置掩膜板,利用真空蒸镀仪蒸镀500nm的叉指状银电极。
本发明的氮化铜薄膜利用反应磁控溅射方法制备,通过调节反应气体(氮气)的流量,获得禁带宽度逐渐变化的氮化铜薄膜,拓宽了薄膜对太阳光吸收的光谱范围。与单一禁带宽度的氮化铜薄膜电池相比,禁带宽度渐变的氮化铜薄膜电池减少了由于入射光子能量比光吸收层材料禁带宽度大而引起的晶格热损失,因此可以大幅提高电池的效率。禁带宽度渐变的氮化铜薄膜电池结构示意图如图1所示,电池的光吸收层为掺杂的组分渐变的氮化铜为光吸收层,从上至下薄膜中氮的组分逐渐减少,即薄膜的禁带宽度逐渐减少。硒掺杂氮化铜为空穴传输层,镁掺杂氮化铜为电子传输层。
附图说明
以下结合附图和本发明的实施方式来作进一步详细说明
图1为禁带宽度渐变的氮化铜薄膜电池结构示意图;
图2为禁带宽度渐变的氮化铜薄膜电池的电流-电压特性图。
具体实施方式
本实施例的氮化铜薄膜太阳能电池,自下而上包括如下结构:ITO玻璃1、镁掺杂氮化铜薄膜2、组分渐变氮化铜薄膜3、硒掺杂氮化铜薄膜4、ITO薄膜5、银电极6,其中组分渐变氮化铜薄膜3中,氮的含量沿→自下而上逐渐变大。所述的组分渐变氮化铜薄膜3的厚度为500nm,分为10层,每层50nm,氮的含量自下而上逐渐变大。太阳光从银电极6上方照射。
制备时:
1)主要原材料及设备
铜、硒、镁、ITO(氧化铟锡)等靶材:纯度99.99%,直径60mm,厚度5mm。
ITO导电玻璃:面积~25×25mm2,方块电阻~15Ω/□,光透过率≥90%。
氮气、氩气:纯度99.999%
双靶共溅射磁控溅射仪:极限真空优于5×10-5Pa,镀膜均匀性优于±2%。
2)镁掺杂氮化铜薄膜制备
首先将ITO玻璃衬底放入丙酮溶液中超声清洗5min,然后放入乙醇溶液中超声清洗5min,再用去离子水反复冲洗,重复上述步骤3次,最后用氮气吹干后放入溅射腔室内。
溅射腔室的本底真空达到极限真空度以后,通入氩气,首先对玻璃基片进行反溅射去除基片表面吸附的水汽和氧气等,然后对靶材表面进行预溅射以去除表面的残留的杂质。
玻璃基片的温度为80~110℃,通入氮气,氮气与氩气的流量比为1:1,氩气流速控制为10sccm,溅射腔压强为0.8Pa。铜靶的溅射功率固定为250W,镁掺杂浓度通过改变镁靶的溅射功率来调节,镁靶的溅射功率为10~15W。薄膜厚度利用膜厚监控仪监测,典型的薄膜厚度为30~50nm。通过X射线衍射图谱分析,镁原子已掺入氮化铜晶格中。利用X射线光电子谱分析,镁在氮化铜的掺杂浓度为0.35~0.45%。通过霍尔效应测量,镁掺杂的氮化铜薄膜呈n型半导体特性,载流子浓度为1017~1018cm-3。
3)组分渐变氮化铜薄膜制备
镁掺杂氮化铜薄膜生长结束以后,待玻璃基片的温度降低到50~60℃以后,开始生长组分渐变氮化铜薄膜。通过改变氮气与氩气的流量比来调节氮化铜薄膜中氮的组分,从而达到调控电池的光吸收层—氮化铜薄膜的禁带宽度,实现拓宽电池的光谱吸收范围。组分渐变氮化铜薄膜的总厚度设定为500nm,共分为10层,开始生长时氮化铜薄膜中氮的组分最小,然后依次增大。溅射腔压强恒定为0.8Pa,铜靶的溅射功率维持在60W。氩气流速恒定为10sccm,氮气与氩气的流量比开始为1,每沉积50nm薄膜(厚度由膜厚监控仪监测)后改变一次氮气与氩气流量比,从1.2、1.5、1.9、2.5、3.3、4.2、5.2、6.3依次变化到7.5,以获得禁带宽度逐渐增加的氮化铜薄膜。利用光吸收谱测量,薄膜的禁带宽度从1.32eV增加到1.84eV。
4)硒掺杂氮化铜薄膜制备
组分渐变的氮化铜薄膜生长结束以后,玻璃基片温度上升至150~180℃,然后开始生长硒掺杂氮化铜薄膜。氮气与氩气的流量比为1:1,氩气流速控制为10sccm,溅射腔压强为0.8Pa。铜靶的溅射功率固定为250W,硒掺杂浓度通过改变硒靶的溅射功率来调节,硒靶的溅射功率为10~15W。薄膜厚度利用膜厚监控仪监测,典型的薄膜厚度为20~30nm。通过X射线衍射图谱分析,硒原子已掺入氮化铜晶格中。利用X射线光电子谱分析,硒的掺杂浓度为0.62%~0.68%。通过霍尔效应测量,硒掺杂的氮化铜薄膜呈p型半导体电学特性,载流子浓度为1017~1018cm-3。
5)ITO薄膜制备
硒掺杂氮化铜薄膜生长结束以后,依次生长ITO薄膜和银电极。玻璃基片的温度为200℃,溅射工作气体为氩气,流量为30sccm,溅射腔压强为0.8Pa。ITO靶的溅射功率为80W,ITO薄膜的生长厚度为80nm。
6)银电极制备
ITO生长结束后,从溅射腔取出样品,在表面放置掩膜板,利用真空蒸镀仪蒸镀500nm厚的叉指状银电极。至此,组分渐变氮化铜薄膜太阳能电池的制备工序全部结束。
7)电池性能测试
标准测试条件(AM1.5,100mW/cm2,25℃)下,电池的电流-电压特性如图2所示,电池的开路电压(VOC)为1.16V,短路电流(ISC)为5.24mA/cm2,填充因子(FF)为0.62,光电转换效率为3.78%。在光照下持续超过200小时之后,没有发现电池存在光衰减。
Claims (3)
1.氮化铜薄膜太阳能电池,其特征在于:自下而上包括如下结构:ITO玻璃\镁掺杂氮化铜薄膜\组分渐变氮化铜薄膜\硒掺杂氮化铜薄膜\ITO薄膜\银电极,其中组分渐变氮化铜薄膜中,氮的含量自下而上逐渐变大。
2.如权利要求1所述的氮化铜薄膜太阳能电池,其特征在于:所述的组分渐变氮化铜薄膜的厚度为500nm,分为10层,每层50nm,氮的含量自下而上逐渐变大。
3.权利要求1所述的氮化铜薄膜太阳能电池的制备方法,其特征在于:包括以下步骤:
1)ITO玻璃衬底清洗吹干后放入溅射腔室内,玻璃基片的温度为80~110℃,通入氮气,氮气与氩气的流量比为1:1,氩气流速控制为10sccm,溅射腔压强为0.8Pa;铜靶的溅射功率固定为250W,镁靶的溅射功率为10~15W;至薄膜厚度为30~50nm;
2)待玻璃基片的温度降低到50~60℃以后,开始生长组分渐变氮化铜薄膜;溅射腔压强恒定为0.8Pa,铜靶的溅射功率维持在60W;氩气流速恒定为10sccm,氮气与氩气的流量比开始为1,每沉积50nm薄膜后改变一次氮气与氩气流量比,从1.2、1.5、1.9、2.5、3.3、4.2、5.2、6.3依次变化到7.5,以获得组分渐变的氮化铜薄膜;
3)玻璃基片温度上升至150~180℃,然后开始生长硒掺杂氮化铜薄膜;氮气与氩气的流量比为1:1,氩气流速控制为10sccm,溅射腔压强为0.8Pa;铜靶的溅射功率固定为250W,硒靶的溅射功率为10~15W,至薄膜厚度为20~30nm;
4)硒掺杂氮化铜薄膜生长结束以后,生长ITO薄膜;玻璃基片的温度为200℃,溅射工作气体为氩气,流量为30sccm,溅射腔压强为0.8Pa;ITO靶的溅射功率为80W,ITO薄膜的生长厚度为80nm;
5)ITO生长结束后,从溅射腔取出样品,在表面放置掩膜板,利用真空蒸镀仪蒸镀500nm的叉指状银电极。
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