高性能反式钙钛矿太阳能电池的制备及界面优化研究

有机-无机杂化钙钛矿材料因其具有较长的载流子扩散距离、较高的电荷迁移率、以及可溶液加工的特点，使其在光电器件领域获得飞速发展。然而，钙钛矿太阳能电池目前的效率与理论极限效率相比仍存在着较大的差距，同时器件的不稳定性和昂贵的制备成本也限制了钙钛矿电池的进一步产业化。其中，钙钛矿薄膜的结晶形貌和传输层界面对载流子的产生、提取和传输具有决定性意义，会对钙钛矿器件的效率和稳定性产生重要影响。由于钙钛矿薄膜晶界处和外表面以及传输层界面都存在着各种深能级和浅能级缺陷，这些缺陷会导致电荷产生较大的非辐射复合，从而对钙钛矿电池的性能及稳定性造成很大影响。鉴于此，本论文以反式钙钛矿电池为研究对象，基于多种体系掺杂和界面钝化手段，研究了界面内部改性机制并加以应用，从而使得电池的效率和稳定性得到明显提升，并有助于降低电池的制备成本。主要研究内容及结果如下：

为了提升空穴传输层材料聚（3,4-乙烯二氧噻吩）聚苯乙烯磺酸钠（PEDOT: PSS）的光电特性，促进PEDOT: PSS/钙钛矿界面的电荷传输和提取能力，将多功能离子液体1-乙基-3-甲基咪唑氯化物（EMIC）掺杂到PEDOT: PSS前驱体溶液中。基于EMIC掺杂的PEDOT: PSS薄膜展现出了更高的电导率、更低的能级以及更光滑的表面，促进了空穴在钙钛矿/PEDOT: PSS界面的提取和传输效能。此外，使用S-乙酰硫代胆碱氯化物两性离子化合物作为钙钛矿表面钝化层以代替昂贵的 PCBM，对钙钛矿表面的正、负电荷缺陷进行了有效地钝化。经过S-乙酰硫代胆碱氯化物钝化的钙钛矿薄膜显示出更长的载流子寿命以及更低的电荷缺陷密度。最终，研制出的小面积钙钛矿电池的光电转化效率达到20.06%，而1cm2电池的光电转化效率也可达到18.77%，且无明显的迟滞效应。同时，器件的湿度和热稳定性也有较大的改善：电池器件在空气环境中（60% 湿度）放置35天后仍保持85%的初始效率，在80°C下保存24小时后仍保持87%的初始效率。

为了改善理想带隙（1.3-1.4 eV）铅锡钙钛矿薄膜的结构和光电特性，在前期获得的高质量EMIC-PEDOT:PSS空穴传输层和S-乙酰硫代胆碱氯化物钝化剂的基础上，利用溴化胍（GABr）对理想带隙铅锡钙钛矿（~1.35 eV）薄膜进行了掺杂修饰。GABr可与铅锡钙钛矿形成局部二维结构，促进了铅锡钙钛矿晶格的稳定。同时，基于GABr掺杂的铅锡钙钛矿薄膜展现出更高的结晶质量、更少的缺陷密度和更长的载流子寿命。利用GABr掺杂制备的器件，其光电转换效率为20.63%，经第三方机构认证的效率为19.8%，器件的开路电压（Voc）达到了1.02 V，这也是目前基于理想带隙铅锡钙钛矿电池实现的最小Voc损失（0.33 V）。GABr掺杂的器件还具有更好的湿度稳定性和热稳定性。

在GABr掺杂的理想带隙铅锡钙钛矿薄膜和器件的基础上，采用近红外体异质结（BHJ）对铅锡混合钙钛矿薄膜进行表面处理，得到一种集成式太阳能电池器件。近红外体异质结是由近红外聚合物DTBTI和PCBM构成，它与铅锡混合钙钛矿之间具有良好的能级排列和较强的相互作用，有利于两者之间的电荷转移。近红外体异质结不仅增加了钙钛矿薄膜对近红外光的响应，同时也降低了薄膜缺陷，提升了载流子的传输效率，进一步提升了器件的短路电流和开路电压。最终，该集成式器件实现了24.27%的光电转换效率，以及1.07 V的开路电压。经第三方机构认证效率为23.4%，这是目前集成式单结钙钛矿器件和铅锡混合钙钛矿电池的世界最高效率。该器件在耐热、耐湿和持续工作稳定性方面得到明显提升。

为了进一步简化钙钛矿器件结构并减少器件的制备成本，将氯硫脲合铜（Cu(Tu)Cl）和氨基硫脲（TSC）掺杂到钙钛矿前驱体溶液中，得到一种无空穴传输层（HTL）的高效简式钙钛矿器件。Cu(Tu)Cl和TSC的掺杂可以同时减少钙钛矿表面和内部缺陷，降低界面能级屏障。基于Cu(Tu)Cl和TSC掺杂的钙钛矿薄膜显示出更好的结晶质量，更长的载流子寿命，以及更低的电荷缺陷密度。最终，这种简式器件实现了22%的光电转换效率，这是目前报道的无空穴传输层钙钛矿电池的最高效率之一。此外，基于宽带隙钙钛矿Cs0.05MA0.15FA0.8Pb(I0.75Br0.25)3（1.65 eV）无HTL器件的效率达到19.7%，并具有 1.2 V开路电压，这是目前报道的无空穴传输层宽带隙钙钛矿电池的最高效率。经Cu(Tu)Cl和TSC掺杂的器件也具有更好的湿度稳定性、热稳定性以及长期运行稳定性。

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