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Supramolecular Engineering for Formamidinium‐Based Layered 2D Perovskite Solar Cells: Structural Complexity and Dynamics Revealed by Solid‐State NMR Spectroscopy
Author(s) -
Milić Jovana V.,
Im JeongHyeok,
Kubicki Dominik J.,
Ummadisingu Amita,
Seo JiYoun,
Li Yang,
RuizPreciado Marco A.,
Dar M. Ibrahim,
Zakeeruddin Shaik M.,
Emsley Lyndon,
Grätzel Michael
Publication year - 2019
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.201900284
Subject(s) - formamidinium , perovskite (structure) , materials science , supramolecular chemistry , van der waals force , spectroscopy , chemical engineering , supramolecular assembly , nanotechnology , chemical physics , crystallography , organic chemistry , chemistry , molecule , crystal structure , physics , engineering , quantum mechanics
Perovskite solar cells are one of the most promising photovoltaic technologies, although their molecular level design and stability toward environmental factors remain a challenge. Layered 2D Ruddlesden–Popper perovskite phases feature an organic spacer bilayer that enhances their environmental stability. Here, the concept of supramolecular engineering of 2D perovskite materials is demonstrated in the case of formamidinium (FA) containing A 2 FA n −1 Pb n I 3 n +1 formulations by employing (adamantan‐1‐yl)methanammonium (A) spacers exhibiting propensity for strong Van der Waals interactions complemented by structural adaptability. The molecular design translates into desirable structural features and phases with different compositions and dimensionalities, identified uniquely at the atomic level by solid‐state NMR spectroscopy. For A 2 FA 2 Pb 3 I 10 , efficiencies exceeding 7% in mesoscopic device architectures without any additional treatment or use of antisolvents for ambient temperature film deposition are achieved. This performance improvement over the state‐of‐the‐art FA‐based 2D perovskites is accompanied by high operational stability under humid ambient conditions, which illustrates the utility of the approach in perovskite solar cells and sets the basis for advanced supramolecular design in the future.

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