In Situ Copper Ions Redox Engineering Elevates Hole Transport for Efficient Perovskite Solar Cells
ABSTRACT Interfacial non‐radiative recombination and energy‐level mismatch remain critical bottlenecks for perovskite solar cells (PSCs). Here, we reported an in situ redox engineering strategy using a cobweb‐like quadrangular macrocyclic copper‐organic complex, Cu(II) meso‐tetra(4‐sulfonatophenyl) porphine [Cu(TSPPa) 2 ], to simultaneously achieve defect passivation and enhanced hole transport at the perovskite/hole transport layer interface. Benefiting from its lattice‐matching macrocyclic structure, Cu(TSPPa) 2 infiltrates grain boundaries and anchors undercoordinated Pb 2+ via sulfonate and N–H groups, while forming hydrogen bonds with organic cations. Notably, partial release of Cu 2+ triggers a reversible Cu 2+ /Cu + redox shuttle, which mitigates deep‐level Pb 0 /I 0 defects and generates p‐type CuI in situ, smoothing the interfacial energy barrier and boosting hole extraction. This multifunctional modification yields a champion power conversion efficiency of 26.32% with negligible hysteresis, along with significantly enhanced operational, thermal, and ambient stability. Our work demonstrates a paradigm of leveraging metal‐ion redox chemistry in metal–organic complexes for synergistic interfacial engineering in high‐performance PSCs.
Authors
- Guojia Fang (ORCID: https://orcid.org/0000-0002-3880-9943)
- Pingli Qin (ORCID: https://orcid.org/0000-0003-1824-2748)
- Haisheng Song (ORCID: https://orcid.org/0000-0002-7764-7975)
- Weijun Ke (ORCID: https://orcid.org/0000-0003-2600-5419)
- Liang Ma (ORCID: https://orcid.org/0000-0002-9636-118X)
- Jiyuan Gao (ORCID: https://orcid.org/0009-0006-4560-5208)
- Liangbin Xiong (ORCID: https://orcid.org/0000-0002-3147-7384)
- Zhongli Qin (ORCID: https://orcid.org/0000-0003-0413-3794)
- Wenwen Zheng (ORCID: https://orcid.org/0000-0002-8237-7498)
- Haibing Wang (ORCID: https://orcid.org/0009-0005-2549-9172)
- Qingbo Liu
- Bingxin Ding
- Jiangling Li
Institutions
- Wuhan University (CN)
- Hubei University of Science and Technology (CN)
- Wuhan Textile University (CN)
- Guangdong Polytechnic Normal University (CN)
- Wuhan National Laboratory for Optoelectronics (CN)
- Huazhong University of Science and Technology (CN)
- Wuhan Institute of Technology (CN)
Publication Details
- Journal
- Small
- Published
- 2026-10-29
- DOI
- https://doi.org/10.1002/smll.76265
- Primary Topic
- Perovskite Materials and Applications
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- Salt Science Research Foundation
- Hubei Provincial Department of Education
- National Natural Science Foundation of China
- Natural Science Foundation of Hubei Province
- Hubei University of Automotive Technology
- Wuhan National Laboratory for Optoelectronics
- Wuhan Institute of Technology
- Department of Education of Guangdong Province
- Science and Technology Department of Hubei Province
- CAS Key Laboratory of Quantum Information
- Division of Graduate Education