Diammonium Molecular Configuration‐Induced Regulation of Crystal Orientation and Carrier Dynamics for Highly Efficient and Stable 2D/3D Perovskite Solar Cells

Abstract

The effects from the molecular configuration of diammonium spacer cations on 2D/3D perovskite properties are still unclear.H ere,w ei nvestigated systematically the mechanism of molecular configuration-induced regulation of crystallization kinetic and carrier dynamics by employing various diammonium molecules to construct Dion-Jacobson (DJ)-type 2D/3D perovskites to further facilitating the photovoltaic performance.T he minimum average Pb-I-Pb angle leads to the smallest octahedral tilting of [PbX 6 ] 4À lattice in optimal diammonium molecule-incorporated DJ-type 2D/3D perovskite,w hich enables suitable binding energy and hydrogen-bonding between spacer cations and inorganic [PbX 6 ] 4À cages,t hus contributing to the formation of high-quality perovskite film with vertical crystal orientation, mitigatory lattice distortion and efficient carrier transportation. As aconsequence,adramatically improved device efficiency of 22.68 % is achieved with excellent moisture stability.

From Structural Design to Functional Construction: Amine Molecules in High‐Performance Formamidinium‐Based Perovskite Solar Cells

“…At the same time, the moisture stability and light stability were greatly enhanced. Furthermore, some functional groups, such as −SH, [64] =S, [65] P=O, and −COOH, etc., [66–68] have also confirmed the significant effect in terms of crystallization modulation and defect passivation. For example, benefiting from its electron‐donating −SH functional group, (3‐mercaptopropyl)trimethoxysilane (MPTS) could combine with perovskite through a Lewis acid/base interaction, which effectively prevented the formation of shallow defects at GBs [64] .…”

“…At the same time, the moisture stability and light stability were greatly enhanced. Furthermore, some functional groups, such as À SH, [64] =S, [65] P=O, and À COOH, etc., [66][67][68] have also confirmed the (110) slab and on a defect-containing structure. Reproduced with permission.…”

Modulating preferred crystal orientation for efficient and stable perovskite solar cells—From progress to perspectives

“…As a result, the HTL-free printable mesoscopic PSCs delivered a PCE of 16.35%, and the unencapsulated cell retained 98% of the original PCE after aging 2500 h in air with humidity of 50 ± 5%. Zhong et al 97 systematically studied the working mechanism of molecular structure-induced regulation of crystallization kinetics and carrier dynamics via employing three diammonium spacer cations to construct Dion-Jacobson (D-J)-type 2D/3D hybrid perovskites, which include octane-1,8-diamine (ODA), triethylenetetramine (TETA), and 2,2 0 -(ethylenedioxy)bis (ethylamine) (EDOEA). The Pb-I distance and Pb-I-Pb angle are significantly affected by the hydrogen-bonding force between the diammonium cations and [PbX 6 ] 4À cage.…”

“…(G) Schematic illustration of the formation of 2D/3D perovskite with EDOEA. Reproduced with permission 97 . Copyright 2021, Wiley‐VCH.…”

Facet Engineering for Stable, Efficient Perovskite Solar Cells

“…Other materials, such as 2,2′-(ethylenedioxy)bis(ethylamine) and ethanolamine were also reported to achieve the preferred oriented thin films. 23 Although some ligands have been successfully used to tune the orientation of the perovskite crystals, the facets on the thin film are still unable to be identified due to the rough morphology. If well-defined facets on the thin film can be achieved, it is anticipated that more potential ligands will be explored.…”