Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2022-09-05 , DOI: 10.1016/j.cej.2022.138962 Yuxuan Yang , Tao Zhao , Ming-Hua Li , Xiaoxue Wu , Mingyue Han , Shih-Chi Yang , Qiaoling Xu , Lede Xian , Xiang Chi , Ning-Jiu Zhao , Hong Cui , Sihan Li , Jin-Song Hu , Bao Zhang , Yan Jiang
Positively charged cationic defects are the main source of defects in metal-halide perovskite solar cells. They determine the quasi-Fermi level of electrons under illumination and contribute to non-radiative recombination loss, causing an open-circuit voltage deficit. In addition, they act as ion migration pathways for halide hopping, thus deteriorating long-term stability. Herein, a nitrogen-donor crown ether as a positive defect passivator is developed, which demonstrates a soft Lewis base nature, a large donor number and a higher formation constant with positively charged cationic defects. Density functional theory calculation indicates that the electron-donating nitrogen atom dramatically increases the electron density of oxygen atoms, leading to a strong affinity with positively charged cationic defects (Pb2+ and Cs+). The electron trap density in perovskite is significantly reduced by 27 %, resulting in an increased build-in potential. By adding a small amount of nitrogen-donor crown ether to the precursor solution, the perovskite solar cells achieve an efficiency of 24.07 % with an open-circuit voltage of 1.174 V and a fill factor of 82.15 %. Moreover, the unencapsulated perovskite solar cells show a T80 lifetime of 510 h under continuous operation (1 sun equivalent illumination, maximum power point tracking condition, dry N2 atmosphere), and enhanced moisture and heat stability.
中文翻译:
用氮供体冠醚钝化钙钛矿中带正电的阳离子缺陷,实现高效的钙钛矿太阳能电池
带正电的阳离子缺陷是金属卤化物钙钛矿太阳能电池缺陷的主要来源。它们确定光照下电子的准费米能级,并导致非辐射复合损失,从而导致开路电压不足。此外,它们充当卤化物跳跃的离子迁移途径,从而降低长期稳定性。在此,开发了一种作为正缺陷钝化剂的氮给体冠醚,它表现出柔软的路易斯碱性质、大的给体数和较高的形成常数以及带正电荷的阳离子缺陷。密度泛函理论计算表明,给电子氮原子显着增加了氧原子的电子密度,导致与带正电的阳离子缺陷(Pb 2+和 Cs + )。钙钛矿中的电子陷阱密度显着降低了 27%,从而增加了内置电位。通过在前驱体溶液中添加少量的氮供体冠醚,钙钛矿太阳能电池的效率为 24.07%,开路电压为 1.174 V,填充因子为 82.15%。此外,未封装的钙钛矿太阳能电池在连续运行(1 太阳等效光照、最大功率点跟踪条件、干燥的 N 2气氛)下的T 80寿命为 510 小时,并且具有增强的湿热稳定性。