Molecular Design‐Driven Interface Engineering Enabling Simultaneous Defect Passivation and Enhanced Hole Extraction in Perovskite Solar Cells

W Wei Jia R Riming Sun (State Key Laboratory of Solidification Processing Center for Nano Energy Materials School of Materials Science and Engineering Northwestern Polytechnical University (NPU) Xi'an 710072 China) J Jingyuan Qiao (State Key Laboratory of Flexible Electronics (SoFE) Shaanxi Institute of Flexible Electronics (SIFE) Institute of Flexible Electronics (IFE) Northwestern Polytechnical University (NPU) Xi'an 710072 China) G Guangchao Shi (State Key Laboratory of Flexible Electronics (SoFE) Shaanxi Institute of Flexible Electronics (SIFE) Institute of Flexible Electronics (IFE) Northwestern Polytechnical University (NPU) Xi'an 710072 China) Q Qiangqiang Zhao Z Ziyan Gong (State Key Laboratory of Solidification Processing Center for Nano Energy Materials School of Materials Science and Engineering Northwestern Polytechnical University (NPU) Xi'an 710072 China) S Siming Zheng (Frontiers Science Center for Flexible Electronics (FSCFE), Shaanxi Institute of Flexible Electronics (SIFE) & Institute of Flexible Electronics (IFE), Northwestern Polytechnical University (NPU), 127 West Youyi Road, Xi’an 710072, China) R Ruida Xu (State Key Laboratory of Flexible Electronics (SoFE) Shaanxi Institute of Flexible Electronics (SIFE) Institute of Flexible Electronics (IFE) Northwestern Polytechnical University (NPU) Xi'an 710072 China) J Jingzhi Shang (State Key Laboratory of Flexible Electronics (SoFE) Shaanxi Institute of Flexible Electronics (SIFE) Institute of Flexible Electronics (IFE) Northwestern Polytechnical University (NPU) Xi'an 710072 China) L Lin Song K Kai Wang W Wei Huang R Ruihao Chen Y Yiyun Fang (Frontiers Science Center for Flexible Electronics (FSCFE), Shaanxi Institute of Flexible Electronics (SIFE) & Institute of Flexible Electronics (IFE), Northwestern Polytechnical University (NPU), 127 West Youyi Road, Xi’an 710072, China) H Hongqiang Wang Z Zi‐Qiang Rong (State Key Laboratory of Flexible Electronics (SoFE) Shaanxi Institute of Flexible Electronics (SIFE) Institute of Flexible Electronics (IFE) Northwestern Polytechnical University (NPU) Xi'an 710072 China)

Abstract

Abstract Interface engineering has emerged as an effective strategy to address interface defects and energy level misalignment between the perovskite and hole transport layer (HTL). Herein, three novel multifunctional hole interface molecules with distinct substituents were designed to passivate defects at the perovskite/HTL interface. These molecules integrate hole‐transporting groups with passivating units, enabling effective defect passivation, improved energy level alignment, and facilitating efficient carrier extraction. Among the three hole transport interface molecules (HTIMs), the 3‐(3,6‐bis(4‐(bis(4‐(methylthio)phenyl)amino)phenyl)‐9H‐carbazol‐9‐yl)hexan‐1‐amine hydroiodide (MeS‐TPA‐Cbz‐HAI), comprising ‐MeS and HAI units, exhibited superior interface passivation capability and greater chemical compatibility with 2,2′,7,7′‐Tetrakis (N,N‐di‐p‐methoxyphenylamine)‐9,9′‐spirobifluorene (Spiro‐OMeTAD), leading to a reduction in defect density and enhanced hole transport. Consequently, the device based on MeS‐TPA‐Cbz‐HAI achieved a notable power conversion efficiency (PCE) of 25.83%. Moreover, the unencapsulated device maintained 94% of its initial efficiency after 1000 hours of continuous operation under ambient conditions (30%–65% relative humidity), demonstrating remarkable long‐term stability. This design strategy for hole interface molecules presents a promising avenue for achieving both high efficiency and operational stability in perovskite solar cells.

Article Details

Volume / Issue Vol. 64, Issue 51
Published December 15, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (16)

W

Wei Jia

R

Riming Sun

State Key Laboratory of Solidification Processing Center for Nano Energy Materials School of Materials Science and Engineering Northwestern Polytechnical University (NPU) Xi'an 710072 China

J

Jingyuan Qiao

State Key Laboratory of Flexible Electronics (SoFE) Shaanxi Institute of Flexible Electronics (SIFE) Institute of Flexible Electronics (IFE) Northwestern Polytechnical University (NPU) Xi'an 710072 China

G

Guangchao Shi

State Key Laboratory of Flexible Electronics (SoFE) Shaanxi Institute of Flexible Electronics (SIFE) Institute of Flexible Electronics (IFE) Northwestern Polytechnical University (NPU) Xi'an 710072 China

Q

Qiangqiang Zhao

Z

Ziyan Gong

State Key Laboratory of Solidification Processing Center for Nano Energy Materials School of Materials Science and Engineering Northwestern Polytechnical University (NPU) Xi'an 710072 China

S

Siming Zheng

Frontiers Science Center for Flexible Electronics (FSCFE), Shaanxi Institute of Flexible Electronics (SIFE) & Institute of Flexible Electronics (IFE), Northwestern Polytechnical University (NPU), 127 West Youyi Road, Xi’an 710072, China

R

Ruida Xu

State Key Laboratory of Flexible Electronics (SoFE) Shaanxi Institute of Flexible Electronics (SIFE) Institute of Flexible Electronics (IFE) Northwestern Polytechnical University (NPU) Xi'an 710072 China

J

Jingzhi Shang

State Key Laboratory of Flexible Electronics (SoFE) Shaanxi Institute of Flexible Electronics (SIFE) Institute of Flexible Electronics (IFE) Northwestern Polytechnical University (NPU) Xi'an 710072 China

L

Lin Song

K

Kai Wang

W

Wei Huang

R

Ruihao Chen

Y

Yiyun Fang

Frontiers Science Center for Flexible Electronics (FSCFE), Shaanxi Institute of Flexible Electronics (SIFE) & Institute of Flexible Electronics (IFE), Northwestern Polytechnical University (NPU), 127 West Youyi Road, Xi’an 710072, China

H

Hongqiang Wang

Z

Zi‐Qiang Rong

State Key Laboratory of Flexible Electronics (SoFE) Shaanxi Institute of Flexible Electronics (SIFE) Institute of Flexible Electronics (IFE) Northwestern Polytechnical University (NPU) Xi'an 710072 China