CN110590816B - 一种一维铜碘基杂化半导体材料及其光电应用 - Google Patents
一种一维铜碘基杂化半导体材料及其光电应用 Download PDFInfo
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- IOJUPLGTWVMSFF-UHFFFAOYSA-N cyclobenzothiazole Natural products C1=CC=C2SC=NC2=C1 IOJUPLGTWVMSFF-UHFFFAOYSA-N 0.000 claims abstract description 46
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- 239000013110 organic ligand Substances 0.000 claims abstract description 6
- CMPNPRUFRJFQIB-UHFFFAOYSA-N [N].[Cu] Chemical compound [N].[Cu] CMPNPRUFRJFQIB-UHFFFAOYSA-N 0.000 claims abstract description 3
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- 238000001514 detection method Methods 0.000 claims description 2
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Abstract
本发明公开了一种一维铜碘基无机‑有机杂化钙钛矿半导体材料及其制备方法和应用。所述的杂化钙钛矿半导体分子结构式为CuI(Btz),式中的Btz是苯并噻唑,该材料表现为有机配体和无机组分通过配位键相连的杂化一维链结构。铜碘原子交替配位相连形成阶梯状中性一维链,苯并噻唑则通过铜氮配位键呈翼状分布在铜碘链的两侧。该材料可通过选择碘化亚铜,苯并噻唑等反应原料通过简便的溶剂热反应获得,材料无机和有机组分间电子传输效率高,光电转换性能优异,稳定性好,可用作光伏器件的制作。
Description
技术领域
本发明涉及杂化半导体材料领域,尤其涉及一种一维铜碘基杂化钙钛矿半导体材料CuI(Btz)与其光电应用,其中Btz为苯并噻唑。
背景技术
人口持续增长以及重工业迅速发展带来了能源短缺和环境污染等一系列问题。为了满足日益增长的能源需求,能源系统在未来必须具备实用低成本、高效可持续和环境污染小等特点。因此,发展可再生能源来获取清洁能源是当今世界面临的挑战,而太阳能作为一种取之不尽用之不竭的能源,其有效的利用技术成为研究热点,其中太阳能电池材料的研究备受关注。 近年来,有机金属卤化物钙钛矿材料由于具有载流子迁移率高、光吸收系数高等优点受到广泛的关注。而有机-无机杂化钙钛矿(HOIP)太阳能电池的出现迅速革新了整个光伏领域,转化效率由最初的3.8%提升到23.9%,而效率的快速提升得益于钙钛矿材料本身的光电特性。但是有机金属卤化物钙钛矿材料在加热、潮湿、光伏照等环境下不稳定成为目前急需解决的问题。
为了提升有机金属卤化物钙钛矿的稳定性,可以对有机金属卤化物钙钛矿材料结构成分进行优化,即采取离子替换或掺杂的方式。Gratzel课题组将Cs+引入FAPbI3中,提升了材料的热稳定性,也排除了MA吸湿性的不稳定影响,而使用溴元素部分替换碘元素不仅能够提升稳定性,同时能够在保持原有结构框架的基础上减少Pb-6s/I-5p的重叠,所得到的黑色Cs0.2FA0.8PbI2.84Br0.16相在外界环境中表现出良好的稳定性,并且器件转换效率也达到了18.02%。而研究发现三维钙钛矿材料环境稳定性较差,而较低结构维度的钙钛矿材料具有良好的稳定性,因此通过对有机金属卤化物钙钛矿材料结构维度的优化也能达到提高材料稳定性的目的。
此外,从晶体工程的角度,有机组分与无机组分间有两类作用力可用于构筑杂化材料:强作用力,如配位键和弱相互作用力,如氢键,库仑力等。与弱相互作用力相比,配位键构筑的杂化材料有利于有机和无机组分间的电子传输,更有利于构筑光电转换材料。
目前钙钛矿太阳能电池吸光剂材料以杂化铅基钙钛矿为主,易造成环境污染,所以非铅金属卤化物钙钛矿材料的研究受到广泛关注。本发明中以碘化亚铜作为反应物与有机配体相结合构成一维有机金属杂化钙钛矿半导体材料,属于非铅无污染有机金属钙钛矿材料;该材料在紫外及可见光区域具有较强的光吸收能力,并且展现出优异的光电转换性能,在光电探测及太阳能电池材料研究领域具有重要价值。
发明内容
本发明的目的在于提供一种一维铜碘基杂化钙钛矿半导体材料,该材料有机组分苯并噻唑通过配位键与无机铜碘链相连,既有利于两组分间的电子传输,又避免了苯并噻唑上的N原子形成亲水基团,克服现阶段已报道三维钙钛矿材料环境稳定性差以及杂化铅基半导体材料中铅的毒性问题;该合成方法条件简单,合成原料价格低廉、易获得且无毒无害,获得的材料具有良好的光电转换性能。
本发明的技术方案包括以下内容:
1. 一种一维铜碘基无机-有机杂化钙钛矿半导体材料CuI(Btz),式中的Btz表示苯并噻唑。该化合物为单斜晶系,结晶于P21/c空间群,单胞参数为a = 4.19(2) Å,b=12.32(2) Å,c=16.43(1) Å,α=90 º,β=90.14(2) º,γ=90 º。材料的晶体颜色为淡黄色,表现为有机配体和无机组分通过配位键相连的杂化一维链结构。具体结构特征为每个铜离子均与三个碘离子以及一个苯并噻唑中的氮原子配位形成(CuI3N)四面体单元,所有I原子均作为μ3桥连原子,形成铜碘交替的阶梯式结构,有机配体则通过铜氮配位键呈翼状分布在铜碘链的两侧。
2. 如项1所述的一维铜碘基无机-有机杂化钙钛矿半导体材料的制备方法,其特征在于:称取摩尔比为1:1:4的碘化亚铜、苯并噻唑和碘化钾,分散于体积比为3:3:1的异丙醇、乙腈和氢碘酸混合液,在溶剂热条件下可得淡黄色晶态产物,即为CuI(Btz)。
3. 如项1所述的铜碘基无机-有机杂化半导体材料的用途,其特征在于:该杂化物具有优异的光电转换性能,作为一种光电探测器的备选材料。
本发明的有益效果为产物的合成条件简单、易控且无污染;材料有机和无机组分间电子传输效率高,光电转换性能优异,稳定性好,可用作光伏器件的制作。
附图说明
图1为有机-无机杂化半导体CuI(Btz)的分子结构图,忽略氢原子。
图2为有机-无机杂化半导体CuI(Btz)分子中无机铜碘链的部分结构图。
图3为有机-无机杂化半导体CuI(Btz)分子在单胞内沿a轴的空间堆积图,忽略氢原子。
图4为有机-无机杂化半导体CuI(Btz)收集样品的粉末衍射花样,与单晶模拟衍射结果完全吻合。
图5为有机-无机杂化半导体CuI(Btz)的红外光谱图。
图6为有机-无机杂化半导体CuI(Btz)的热重分析图。
图7为有机-无机杂化半导体CuI(Btz)的电流-电压曲线,材料在偏压2伏特的on/off比值接近4。
图8为有机-无机杂化钙钛矿半导体CuI(Btz)在恒定偏压2伏特下测试的光暗电流循环曲线,说明材料具有良好的稳定性。
具体实施方式
(1)化合物CuI(Btz)的合成
将0.048 g CuI和0.166 g KI放入25 mL聚四氟乙烯内胆中,加入1 mL 氢碘酸、3mL异丙醇、3 mL乙腈和200 μL苯并噻唑,然后聚四氟乙烯内胆放入不锈钢反应釜中,旋紧后放在140 ℃烘箱的加热,并在此温度下恒温三天,然后冷却至室温,经过乙醇洗涤后得到淡黄色针状晶体,即为化合物CuI(Btz)。在上述的反应条件下得到的晶体的纯度、产率较高。
(2)光对于半导体性能的影响
将5 mg充分研磨的CuI(Btz)粉末和5粒ZrO2球放入1 mL玻璃瓶中,加入0.3 mL乙醇并在混匀器上混匀处理三十分钟,再将7 μL混合物分两次滴涂在叉指电极上成膜,40 ℃真空干燥四小时后在光源的照射下进行线性伏安扫描。
Claims (2)
1.一种具有光电转换性能的一维铜碘基杂化钙钛矿半导体材料,其特征在于:该杂化材料的结构式为CuI(Btz),式中的Btz表示苯并噻唑;所述的铜碘基杂化材料结晶于单斜晶系,P21/c空间群,单胞参数为a = 4.19(2) Å,b=12.32(2) Å,c=16.43(1) Å,α=90 º,β=90.14(2) º,γ=90 º,材料的晶体颜色为淡黄色,表现为有机配体和无机组分通过配位键相连的杂化一维链结构,具体结构特征为每个铜离子均与三个碘离子和一个苯并噻唑的氮原子配位形成CuI3N四面体单元,所有I原子均作为μ3桥连原子,形成铜碘交替的阶梯式一维链结构,有机配体则通过铜氮配位键呈翼状分布在铜碘链的两侧。
2.一种权利要求1所述的一维铜碘基杂化钙钛矿半导体材料的用途,其特征在于:该材料用作光伏器件和光探测器件的制作。
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