Sequential organic ligand modifications to dedicatedly restructure grain boundary and surface of perovskites

Abstract

The durability of perovskite solar cells (PSCs) is substantially limited by defects and imperfect structures at grain boundaries (GBs) and grain surfaces (GSs) of perovskites, where common single-step ligand passivation struggles due to ligand heterogeneous distributions and distinct chemical environments. Herein, we demonstrate a two-step sequential dedicated-ligand (TSS-DL) strategy that selectively targets GBs and GSs through spatially resolved interactions of the dedicated ligands. We identified two classes of dedicated ligands, including Ligand X, notably 2,2-difluoroacetamide bromide (DFABr) for GBs to restructure them into stable 2D perovskites and suppress defects, and Ligand Y, featuring 4-aminopiperidinium dibromide (4APPBr2) for GSs to create a rigid 2D perovskite overlayer that shields 3D perovskites from external stresses. TSS-DL-treated PSCs retain >93% of their power conversion efficiency (PCE) after 3,000 hours of operation and >90% after 4,000 hours under high humidity (>85% RH). By sequentially restructuring GBs and GSs using dedicated ligands, the work provides an effective way to overcome the instability of 3D PSCs while maintaining high performance.

Metadata

Item Type:	Article
Authors/Creators:	Ahmad, S. https://orcid.org/0000-0001-9468-0067 Ali, W. Sun, J. Zhou, B. Jiang, Z. Meng, J. Wang, H. https://orcid.org/0000-0002-3443-8604 Wei, G. https://orcid.org/0000-0003-2209-2789 Choy, W.C.H. https://orcid.org/0000-0002-9535-4076
Copyright, Publisher and Additional Information:	© The Author(s) 2025. Open Access: This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License, which permits any non-commercial use, sharing, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if you modified the licensed material. You do not have permission under this licence to share adapted material derived from this article or parts of it. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by-nc-nd/4.0/.
Keywords:	Macromolecular and Materials Chemistry; Chemical Sciences; Physical Chemistry; Engineering; Materials Engineering; Affordable and Clean Energy
Dates:	Accepted: 7 November 2025 Published (online): 13 December 2025 Published: 13 December 2025
Institution:	The University of Sheffield
Academic Units:	The University of Sheffield > Faculty of Science (Sheffield) > School of Mathematical and Physical Sciences
Date Deposited:	08 Jan 2026 09:33
Last Modified:	08 Jan 2026 09:33
Status:	Published
Publisher:	Springer Science and Business Media LLC
Refereed:	Yes
Identification Number:	10.1038/s41467-025-66478-1
Related URLs:	PubMed URL
Sustainable Development Goals:
Open Archives Initiative ID (OAI ID):	oai:eprints.whiterose.ac.uk:236255

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Sequential organic ligand modifications to dedicatedly restructure grain boundary and surface of perovskites

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