Accessing Metal‐Containing Species in Tin–Lead Perovskite Precursor Solutions via Molecular Strategies Guided by the Hard–Soft Acid–Base Principle

S Shuaifeng Hu X Xinru Sun (Key Laboratory for Special Functional Materials of Ministry of Education, School of Nanoscience and Materials Engineering Henan University Kaifeng 475004 P.R. China) W Wentao Liu (State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science) L Luca Gregori (Department of Chemistry, Biology and Biotechnology University of Perugia Via Elce di Sotto 8 Perugia 06123 Italy) P Pei Zhao (Institute for Molecular Science, 38, NishigoNaka, Myodaiji, Okazaki-shi, Aichi 444-8601, Japan) J Jorge Pascual (Instituto de Tecnología Química Universitat Politècnica València‐Consejo Superior de Investigaciones Científicas, Av. dels Tarongers València Spain) A André Dallmann (Humboldt Universität zu Berlin Institut für Chemie, AG NMR Germany) A Akash Dasgupta (Clarendon Laboratory, Department of Physics, University of Oxford, Parks Road, Oxford OX1 3PU, U.K.) F Fengjiu Yang (Helmholtz‐Zentrum Berlin für Materialien und Energie GmbH Hahn‐Meitner‐Platz 1 14109 Berlin Germany) G Guixiang Li (Institute of Chemical Sciences and Engineering) M Mahmoud Aldamasy (Helmholtz‐Zentrum Berlin für Materialien und Energie Berlin Germany) S Silver‐Hamill Turren‐Cruz (Instituto Universitario de Ciencia de los Materiales (ICMUV) Universitat de València Paterna Spain) M Marion A. Flatken (Helmholtz‐Zentrum Berlin für Materialien und Energie GmbH Hahn‐Meitner‐Platz 1 14109 Berlin Germany) S Sheng Fu Y Yasuko Iwasaki (Institute for Chemical Research, Kyoto University, Gokasho, Uji, Kyoto 611-0011, Japan) R Richard Murdey (Institute for Chemical Research, Kyoto University, Gokasho, Uji, Kyoto 611-0011, Japan) A Armin Hoell (Helmholtz‐Zentrum Berlin für Materialien und Energie Berlin Germany) S Susan Schorr (Helmholtz‐Zentrum Berlin für Materialien und Energie Berlin Germany) S Steve Albrecht (Helmholtz‐Zentrum Berlin für Materialien und Energie GmbH Hahn‐Meitner‐Platz 1 14109 Berlin Germany) S Shangfeng Yang A Antonio Abate (Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Hahn-Meitner-Platz 1, 14109 Berlin, Germany) A Atsushi Wakamiya (Institute for Chemical Research) F Filippo De Angelis (Department of Chemistry, Biology and Biotechnology and INSTM) M Meng Li H Henry J. Snaith

Abstract

AbstractThe properties of metal‐centred species in metal halide perovskite precursor solutions substantially influence the formation and evolution of colloidal particles, which in turn dictate the crystallisation process and the film quality. In this work, we assess the “hard” and “soft” Lewis acid characteristics of Sn2+ and Pb2+ cations as a strategy to modulate the chemical environment of these metal‐containing species in mixed‐metal tin–lead perovskite precursor solutions. We observe enhanced simultaneous access to both metal centres upon adding compounds with functional groups suggested by the hard–soft acid–base principle. Theoretical calculations suggest that the hard base carboxyl group preferentially interacts with Sn2+‐based species, while the softer base thiol group also targets Pb2+‐based species. By effectively accessing and manipulating possible classes of inorganic species and their colloidal particle properties in the precursor solutions, we achieve 1.26 eV perovskite polycrystalline films exhibiting enhanced structural and optoelectronic quality, giving the best quasi‐Fermi level splitting values of up to 0.95 eV. As a result, the solar cell devices demonstrate efficiency values of up to 23.3% with an extended operational lifetime, retaining 80% of their initial efficiency after over 280 and 180 h of maximum power point tracking under simulated AM1.5G illumination at 25 and 65 °C, respectively.

Article Details

Volume / Issue Vol. 64, Issue 41
Published October 06, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (25)

S

Shuaifeng Hu

X

Xinru Sun

Key Laboratory for Special Functional Materials of Ministry of Education, School of Nanoscience and Materials Engineering Henan University Kaifeng 475004 P.R. China

W

Wentao Liu

State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science

L

Luca Gregori

Department of Chemistry, Biology and Biotechnology University of Perugia Via Elce di Sotto 8 Perugia 06123 Italy

P

Pei Zhao

Institute for Molecular Science, 38, NishigoNaka, Myodaiji, Okazaki-shi, Aichi 444-8601, Japan

J

Jorge Pascual

Instituto de Tecnología Química Universitat Politècnica València‐Consejo Superior de Investigaciones Científicas, Av. dels Tarongers València Spain

A

André Dallmann

Humboldt Universität zu Berlin Institut für Chemie, AG NMR Germany

A

Akash Dasgupta

Clarendon Laboratory, Department of Physics, University of Oxford, Parks Road, Oxford OX1 3PU, U.K.

F

Fengjiu Yang

Helmholtz‐Zentrum Berlin für Materialien und Energie GmbH Hahn‐Meitner‐Platz 1 14109 Berlin Germany

G

Guixiang Li

Institute of Chemical Sciences and Engineering

M

Mahmoud Aldamasy

Helmholtz‐Zentrum Berlin für Materialien und Energie Berlin Germany

S

Silver‐Hamill Turren‐Cruz

Instituto Universitario de Ciencia de los Materiales (ICMUV) Universitat de València Paterna Spain

M

Marion A. Flatken

Helmholtz‐Zentrum Berlin für Materialien und Energie GmbH Hahn‐Meitner‐Platz 1 14109 Berlin Germany

S

Sheng Fu

Y

Yasuko Iwasaki

Institute for Chemical Research, Kyoto University, Gokasho, Uji, Kyoto 611-0011, Japan

R

Richard Murdey

Institute for Chemical Research, Kyoto University, Gokasho, Uji, Kyoto 611-0011, Japan

A

Armin Hoell

Helmholtz‐Zentrum Berlin für Materialien und Energie Berlin Germany

S

Susan Schorr

Helmholtz‐Zentrum Berlin für Materialien und Energie Berlin Germany

S

Steve Albrecht

Helmholtz‐Zentrum Berlin für Materialien und Energie GmbH Hahn‐Meitner‐Platz 1 14109 Berlin Germany

S

Shangfeng Yang

A

Antonio Abate

Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Hahn-Meitner-Platz 1, 14109 Berlin, Germany

A

Atsushi Wakamiya

Institute for Chemical Research

F

Filippo De Angelis

Department of Chemistry, Biology and Biotechnology and INSTM

M

Meng Li

H

Henry J. Snaith