物理化学学报2026，Vol.42Issue(3)：135-148,14.DOI:10.1016/j.actphy.2025.100194
π-共轭扩展二萘并咔唑膦酸作为反式钙钛矿太阳能电池的空穴选择层
π-Conjugation-extended dinaphthocarbazole phosphonic acid as a hole-selective layer for inverted perovskite solar cells
摘要
Abstract
In the rapidly evolving field of photovoltaic technology,self-assembled monolayers(SAMs)have become essential hole-selective layers(HSLs)for inverted perovskite solar cells(PSCs).SAMs not only determine interfacial hole extraction but also significantly influence the film quality of the atop perovskite layers,consequently affecting the efficiency and stability of perovskite solar cells.Among various SAMs,carbazole-based SAMs,exemplified by 4PACZ,have emerged as prominent due to their electron-rich characteristics,making them some of the most prevalent HSLs in modern inverted PSCs.Nevertheless,4PACZ exhibits significant limitations:one major issue is its limited molecular dipole,which leads to insufficient energy level alignment between the treated substrate and the perovskite,causing substantial interfacial energy loss.Another critical challenge is the flat structure of the carbazole unit,which often promotes molecular stacking,resulting in incomplete substrate coverage and non-uniform film formation,thereby compromising both device performance and stability.In this study,we designed a novel SAM based on a polycyclic aromatic hydrocarbon derivative,(4-(8H-dinaphtho[2,3-c:2',3'-g]carbazol-8-yl)butyl)phosphonic acid(4PADNC),with the aim of optimizing hole transport in inverted PSCs.This SAM incorporates the structurally extended dinaphtho[2,3-c:2',3'-g]carbazole(DNC)as the functional terminal group,replacing the single carbazole unit in the traditional material 4PACZ.The key structural difference is that the DNC group provides a significantly expanded π-conjugated skeleton and enhanced electron-rich characteristics.These features not only greatly enhance hole extraction and transport at the interface but also induce a significant increase in the molecular dipole moment,which is crucial for effectively adjusting the work function of ITO,ensuring proper alignment with the perovskite layer.Additionally,there is an intramolecular dihedral angle of approximately 34.62° in the DNC unit at the core of 4PADNC.This non-planar configuration contrasts sharply with the planar carbazole structure.The larger dihedral angle effectively suppresses excessive π-π stacking between molecules,which not only aids in forming a denser and more ordered molecular layer on the ITO surface but also provides a more favorable and defect-free substrate for the growth of the upper perovskite.With these upgrades,the inverted PSCs based on 4PADNC achieved a PCE as high as 24.32%,compared to 22.89%for the control devices based on 4PACZ.Furthermore,the 4PADNC-based devices also exhibited superior thermal stability and operational stability.关键词
钙钛矿太阳能电池/空穴选择层/自组装单层/二萘并咔唑/π共轭Key words
Perovskite solar cells/Hole-selective layer/Self-assembled monolayer/Dinaphtho carbazole/π-conjugation分类
化学化工引用本文复制引用
张善涛,刘生忠,杨上峰,侯天骜,王艳东,方志敏,吴宇,王灝霖,陈涛,陈爽,张文华..π-共轭扩展二萘并咔唑膦酸作为反式钙钛矿太阳能电池的空穴选择层[J].物理化学学报,2026,42(3):135-148,14.基金项目
国家自然科学基金(51925206,52461160328,52350710208,62174103) （51925206,52461160328,52350710208,62174103）
中国科学院战略性先导科技专项(XDB0450301,XDB1140000) （XDB0450301,XDB1140000）
中央高校基本科研业务费专项资金(20720220009,WK2490000002,GK202103106) （20720220009,WK2490000002,GK202103106）
知识创新工程项目(Y261261606) （Y261261606）
111计划(B21005,B1404),陕西省重点研发计划(2022LL-JB-08)资助项目 （B21005,B1404）
