Synergistic Molecular Modulation via Coordination and Hydrogen Bonding for Efficient Perovskite and Tandem Solar Cells
Abstract
ABSTRACT Molecular additives offer a powerful route to control crystallization kinetics and homogenize component distribution in perovskite semiconductors. However, additives that integrate Pb‐related coordination and hydrogen‐bonding functionalities within a single molecular framework to jointly regulate crystallization evolution and defect chemistry remain largely underexplored. Herein, we introduce 4,4’‐(phenylphosphoryl)dibenzoic acid (PPDBA) as a multifunctional molecular modulator that combines P═O and ─COOH groups within a single framework. Compared with P═O‐only reference molecule triphenylphosphine oxide (TPPO), PPDBA expands the interaction scope by coupling Pb‐related coordination involving P═O/─COOH functionalities with additional ─COOH‐assisted hydrogen bonding toward organic cations. These cooperative interactions facilitate intermediate‐phase evolution modulation, crystallization retardation, and the formation of uniform perovskite films with reduced residual PbI 2 . In addition, PPDBA preferentially enriches near the perovskite surface, where it contributes to defect passivation and improved carrier extraction. Consequently, PPDBA‐treated 1.55 eV PSCs achieve a power conversion efficiency of 26.31% with exceptional stability. The universality of the strategy is further demonstrated by high efficiencies of 23.50% and 19.13% PCEs for 1.68 and 1.84 eV wide‐bandgap PSCs, respectively. Beyond single‐junctions, PPDBA enables high‐performance tandems, delivering 33.05% (certified 32.65%) in perovskite/silicon and 26.11% in perovskite/organic architectures. This work provides a molecular design blueprint for high‐performance, durable perovskite‐based photovoltaics.
Article Details
Authors (26)
Tao Zhang
Zehang Liu
Science and Education Integration College of Energy and Carbon Neutralization College of Materials Science and Engineering State Key Laboratory of Green Chemical Synthesis and Conversion Zhejiang University of Technology Hangzhou China
Yonggui Sun
Hoffmann Institute of Advanced Materials Shenzhen Polytechnic University Shenzhen Guangdong P. R. China
Taomiao Wang
Hoffmann Institute of Advanced Materials Shenzhen Polytechnic University Shenzhen China
Qiannan Li
Xiaowei Li
College of Chemistry, Institute of Nuclear Science and Technology, Key Laboratory of Radiation Physics and Technology of Ministry of Education
Ruijie Li
Xiaokang Sun
Hoffmann Institute of Advanced Materials Shenzhen Polytechnic University Shenzhen 518055 P.R. China
Fei Wang
Xinquan Wang
The Ministry of Education Key Laboratory of Protein Science
Yu Bao
Ruoyu Li
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry
Yuzhou Wu
Yaxuan Yang
Pengcheng Wang
Institute of Functional Nano & Soft Materials & Collaborative Innovation Center of Suzhou Nano Science and Technology (NANO−CIC)
Xianfang Zhou
State Key Laboratory of Advanced Glass Materials Wuhan 430070 China
Shicheng Pan
State Key Laboratory of Green Chemical Synthesis and Conversion Science and Education Integration College of Energy and Carbon Neutralization College of Materials Science and Engineering Zhejiang Provincial Key Laboratory of Clean Energy Conversion and Utilization Zhejiang University of Technology Hangzhou China
Xiuyuan Chen
Department of Chemistry, College of Arts and Sciences
Dawei Duan
Hoffmann Institute of Advanced Materials Shenzhen Polytechnic University Shenzhen China
Guo Yang
Jing Li
Zijia Li
Wen‐Hua Zhang
Southwest United Graduate School, National Center for International Joint Research of Photoelectric Energy Materials and Application, School of Materials and Energy Yunnan University Kunming China
Qingquan He
Science and Education Integration College of Energy and Carbon Neutralization College of Materials Science and Engineering State Key Laboratory of Green Chemical Synthesis and Conversion Zhejiang University of Technology Hangzhou China
Hanlin Hu
Jun Pan