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Fluorinated spacer cations in quasi-2D (Q-2D) perovskites have recently been demonstrated to improve the Q-2D perovskite solar cell (PSC) performance. However, the underlying mechanism of fluorination of organic cations on the improvement is still unclear. Here, using fluorinated benzylammonium (named F-BZA) as a spacer cation in Q-2D Ruddlesden-Popper (RP) perovskites, we deeply investigate the effect of fluorination of organic cations on perovskite crystallization and intermolecular interactions for improving the charge transport and device performance. It is found that fluorination of spacer cations can slow down the crystallization rate of perovskites, resulting in vertically aligned large grains. Moreover, the interaction between the adjacent spacer cations is further enhanced, constructing a new faster charge-transport channel with a lifetime of 77 ps. Accordingly, the carrier mobility is improved by an order of magnitude and a power conversion efficiency (PCE) of 16.82% is achieved in much more stable F-BZA-based Q-2D RP PSCs, 35% higher than that of BZA-based devices (12.39%). Our results elucidate the mechanism and its importance of fluorinating spacer cations for high-performance Q-2D PSC development.
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http://dx.doi.org/10.1021/acsami.1c21715 | DOI Listing |
Small Methods
September 2025
Institute of Applied Mechanics, National Taiwan University, No. 1, Section 4, Roosevelt Road, Taipei, 106216, Taiwan.
2D lead-halide perovskites have garnered considerable attention owing to their superior environmental stability and tunable optoelectronic properties, which can be precisely controlled through varying quantum well (QW) width (denoted by the integer n). However, the commonly observed phenomenon of mixed QW width distributions poses a major obstacle to achieving optimal device performance, necessitating an in-depth understanding of how QW width distributions depend on chemical composition and thermodynamic stability. In this work, a robust machine learning (ML)-based energy model is developed, rigorously benchmarked against first-principles calculations, enabling extensive molecular-level simulations of 2D perovskites with butylammonium (BA) and phenethylammonium (PEA) spacer cations.
View Article and Find Full Text PDFJ Phys Chem B
September 2025
Hubei Key Laboratory of Drug Synthesis and Optimization, Jingchu University of Technology, Jingmen, Hubei 448000, China.
Phosphoric acid (PA) retention is essential for the efficient and stable operation of PA-doped proton exchange membranes (PEMs) in fuel cells. The strength of the interactions between polymer functional groups and PA is a key determinant of PA retention. In this work, we systematically investigate the interactions between zwitterionic sulfobetaines (SBs) with varying carbon spacer lengths (CSLs) and PA under both anhydrous and hydrated conditions using density functional theory calculations and molecular dynamics (MD) simulations.
View Article and Find Full Text PDFPharmaceutics
August 2025
Department of Applied Chemistry, Tokyo Metropolitan University, Hachioji, Tokyo 192-0397, Japan.
To design the pDNA delivery carrier for delivery into skeletal muscle, a total of twelve terminal-alkylated PEGs (Cx-I-PEGy) with four alkyl groups of different carbon numbers (Cx: x = 4, 8, 12, 16) modified via an imine spacer at the ends of three methoxy PEGs of different molecular weights (PEGy: y = 500, 2k, 5k) have been synthesized. Among them, four Cx-I-PEG5k formed an imine-mediated complex formation with pDNA, as assessed by agarose gel electrophoresis, defined as an iminium mono-ion complex (I-MIC) without multivalent electrostatic interaction by minimizing potential toxic cations. Most resulting I-MICs maintained the flexible structure of pDNA and promoted the binding to pDNA.
View Article and Find Full Text PDFLangmuir
August 2025
Branch of Petersburg Nuclear Physics Institute Named By B.P. Konstantinov of National Research Centre "Kurchatov Institute", Institute of Macromolecular Compounds, Bolshoi Prospect V.O. 31, St. Petersburg 199004, Russia.
Antibiotic resistance has been widely recognized as a global threat to public health, calling for alternative antimicrobial agents. Here, we focused on acyl-lysine, a biomimetic polymer with proven antimicrobial activity. Using atomic-scale computer simulations, we show that the binding of acyl-lysine to model bacterial membranes is a two-step process.
View Article and Find Full Text PDFSmall
August 2025
Key Laboratory for Intelligent Nano Materials and Devices of Ministry of Education, State Key Laboratory of Mechanics and Control for Aerospace Structures, and Institute for Frontier Science, Nanjing University of Aeronautics and Astronautics, Nanjing, 210016, China.
2D perovskites as interfacial modifiers have demonstrated potential for improving the stability of perovskite solar cells (PSCs); however, 2D structures based on flexible long-chain cations often lead to a high degree of octahedral distortions and larger interlayer spacing. These factors hinder efficient charge extraction between the perovskite and charge transport layers and affect the stability of 2D/3D devices. Here, imidazolyl spacers with rigid ring structures are employed as interfacial modifiers.
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