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

Abstract The 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 Sn 2+ and Pb 2+ 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 Sn 2+ ‐based species, while the softer base thiol group also targets Pb 2+ ‐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.

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Publication Details

Journal
Angewandte Chemie
Published
2025-08-19
DOI
https://doi.org/10.1002/ange.202514010
Citations
3
Primary Topic
Perovskite Materials and Applications
Type
article
Field-Weighted Citation Impact
2.19

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article

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

Armin Hoell, Shuaifeng Hu, Atsushi Wakamiya, Silver‐Hamill Turren‐Cruz et al.
3 citations
Angewandte Chemie
Perovskite Materials and Applications
2.19
article

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

Armin Hoell, Shuaifeng Hu, Atsushi Wakamiya, Silver‐Hamill Turren‐Cruz, Antonio Abate, Mahmoud H. Aldamasy, Filippo De Angelis, Susan Schorr, Guixiang Li, Jorge Pascual, Yasuko Iwasaki, Steve Albrecht, Fengjiu Yang, Akash Dasgupta, Luca Gregori, Pei Zhao, Henry James Snaith, Marion A. Flatken, André Dallmann, Richard Murdey, Wentao Liu, Meng Li, Sheng Fu, Xinru Sun, Shangfeng Yang
article en
3 citations

Abstract

Abstract The 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 Sn 2+ and Pb 2+ 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 Sn 2+ ‐based species, while the softer base thiol group also targets Pb 2+ ‐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.

Angewandte ChemieVol. 137(41)
University of Science and Technology of China (CN), Anhui University (CN), Henan University (CN), Kyoto University (JP), University of Perugia (IT), Helmholtz-Zentrum Berlin für Materialien und Energie (DE), Parc Científic de la Universitat de València (ES), Humboldt-Universität zu Berlin (DE), University of Oxford (GB), Kyoto Bunkyo University (JP), Polymat (ES), Institute for Molecular Science (JP), East China Normal University (CN), University of Naples Federico II (IT), Southeast University (CN), Sungkyunkwan University (KR)
University of Oxford, National Natural Science Foundation of China, New Energy and Industrial Technology Development Organization, Ministry of Environment, China Scholarship Council, Ministerio de Ciencia e Innovación, Natural Science Foundation of Henan Province, Engineering and Physical Sciences Research Council, Japan Society for the Promotion of Science, JST-Mirai Program
Openalex Percentile: Top 11%
Perovskite Materials and Applications
2.19
DOIOpen Access PDFOpenAlex
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