Minimizing Interfacial Energy Loss and Volatilization of Formamidinium via Polymer‐Assisted D–A supramolecular Self‐Assembly Interface for Inverted Perovskite Solar Cells with 25.78% Efficiency

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: July 18, 2024

Abstract 2D perovskite passivation strategies effectively reduce defect‐assisted carrier nonradiative recombination losses on the surface. Nonetheless, severe energy are causing by thermalization, interfacial recombination, and conduction band offset still persist at heterojunction perovskite/PCBM interfaces, which limits further performance enhancement of inverted PSCs. Here, 5,10,15,20‐tetrakis(pentafluorophenyl)porphyrin (5FTPP) is introduced between 3D/2D PCBM. Compared to tetraphenylporphyrin without electron‐withdrawing fluoro‐substituents, 5FTPP can self‐assemble with PCBM interface into donor–acceptor (D–A) complex stronger supramolecular interaction lower transfer losses. This rapid from donor acceptor (PCBM) within femtosecond scale demonstrated enlarge hot extraction rates ranges, reducing thermalization Furthermore, incorporation polystyrene derivative (PD) reinforces D–A inhibiting self‐π–π stacking 5FTPP, while fine‐tuning suppressing via Schottky barrier, dipole, n‐doping. Notably, multidentate anchoring PD‐5FTPP FA + , Pb 2+ I − mitigates adverse effects volatilization during thermal stress. Ultimately, devices achieve a power conversion efficiency 25.78% (certified: 25.36%), maintaining over 90% initial after 1000 h continuous illumination maximum point (65 °C) under ISOS‐L‐2 protocol.

Language: Английский

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Rational Construction and Efficient Regulation of Stable and Long-Lived Charge-Separation State in Fullerene Materials

Accounts of Materials Research, Journal Year: 2024, Volume and Issue: 5(4), P. 426 - 437

Published: March 12, 2024

ConspectusPhotoinduced charge separation (CS) ensures efficient light-energy conversion. The stable and long-lived charge-separation state (CSs) is beneficial for suppressing recombination facilitating the of highly reduction-active electrons or oxidation-active holes to participate in subsequent photoreactions. Accordingly, construction states has been an important goal researchers. These results highlighted importance fullerene materials. Characterized by their well-defined structures exceptional electronic properties, fullerenes have emerged as prominent electron acceptors. energy levels excited-state transfer features can be modulated altering carbon cage (selecting diverse carbon-cage configurations), embedding clusters (metallofullerenes), modifying functional groups on (fullerene additive reactions). Importantly, low reorganization makes them promising materials constructing CSs. Therefore, researchers commonly employ acceptors design photoelectric investigate fundamental mechanisms. primary task construct CSs through system extend lifetime according appropriate regulations. However, critical challenges stem from inadequate comprehension CS patterns, unsuitable choices, lack simple strategies regulation. our research approach, which originates inherent principles CS, aims explore regulating derivatives.In this Account, we systematically summarize following three aspects (1) Construction thermodynamically We established a mathematical correlation between external HOMO levels, enabling rapid straightforward prediction stability Stable successfully constructed increasing donor, lowering LUMO acceptor, direction (2) Develop kinetic regulation lifetime. found that meta- ortho-substituted configuration determines localization, effectively slowing thus prolonging Additionally, findings indicate restricting molecular conformational changes Strategies regulation, including redox introduction steric hindrance, were subsequently designed. (3) Potential applications primarily elucidated photovoltaics photocatalysis (hydrogen production NAD+ regeneration). effective photogenerated carrier transport, are photovoltaic photocatalytic reactions. Finally, aiming prolonged lifetime, more universal strategies, broader state, propose some perspectives further applied fullerene-based

Language: Английский

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Bioinspired Self‐Assembly of Metalloporphyrins and Polyelectrolytes into Hierarchical Supramolecular Nanostructures for Enhanced Photocatalytic H₂ Production in Water

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(8)

Published: Jan. 3, 2024

Polypeptides, as natural polyelectrolytes, are assembled into tailored proteins to integrate chromophores and catalytic sites for photosynthesis. Mimicking nature create the water-soluble nanoassemblies from synthetic polyelectrolytes photocatalytic molecular species artificial photosynthesis is still rare. Here, we report enhancement of full-spectrum solar-light-driven H

Language: Английский

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Efficiently photocatalytic conversion of amine to imidine via perylene diimides supramolecules with oxygen vacancy

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 350, P. 123915 - 123915

Published: April 24, 2024

Language: Английский

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Recent Progress in Porphyrin/g-C3N4 Composite Photocatalysts for Solar Energy Utilization and Conversion

Molecules, Journal Year: 2023, Volume and Issue: 28(11), P. 4283 - 4283

Published: May 23, 2023

Transforming solar energy into chemical bonds is a promising and viable way to store energy. Porphyrins are natural light-capturing antennas, graphitic carbon nitride (g-C3N4) an effective, artificially synthesized organic semiconductor. Their excellent complementarity has led growing number of research papers on porphyrin/g-C3N4 hybrids for utilization. This review highlights the recent progress in composites, including: (1) porphyrin molecules/g-C3N4 composite photocatalysts connected via noncovalent or covalent interactions, (2) porphyrin-based nanomaterials/g-C3N4 photocatalysts, such as MOF/g-C3N4, COF/g-C3N4, assembly/g-C3N4 heterojunction nanostructures. Additionally, discusses versatile applications these including artificial photosynthesis hydrogen evolution, CO2 reduction, pollutant degradation. Lastly, critical summaries perspectives challenges future directions this field also provided.

Language: Английский

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Rational design of bimetallic sites in covalent organic frameworks for efficient photocatalytic oxidative coupling of amines

Journal of Colloid and Interface Science, Journal Year: 2023, Volume and Issue: 655, P. 611 - 621

Published: Nov. 7, 2023

Language: Английский

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Donor-acceptor type conjugated porous polymers based on benzotrithiophen and triazine derivatives: Effect of linkage unit on photocatalytic water splitting

International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 64, P. 109 - 119

Published: March 26, 2024

Language: Английский

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Fullerene Intercalation of MXene Toward Super‐Long‐Cycle Sodium Ion Storage

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(33)

Published: May 19, 2024

Abstract 2D layered MXene‐based materials are applied as cation‐intercalation electrode for sodium‐ion batteries (SIBs) due to their structures but suffer from spontaneous restacking during Na + insertion and deintercalation processes, resulting in sluggish reaction kinetics poor cycling stability. Herein, fullerene C 60 is intercalated covalently into the interlayer of Ti 3 2 T x MXene nanosheets by using a low‐temperature hydrothermal between water‐soluble derivative hydrophilic nanosheets, enlarged spacing 12.8 14.1 Å consequently retarded self‐restacking. Moreover, strong electron extraction ability facilitates transfer , enabling faster charge transport transportation. The as‐prepared @MXene hybrid novel anode SIBs, exhibiting outstanding electrochemical performance super‐long @MXene‐based SIB delivers specific capacity 226.8 mAh g −1 at 0.1 A after 300 cycles, which surpasses that obtained pristine anode, retains 94.5% 1 10 000 cycles. DFT simulations confirm ‐induced benefits migrations, responsible improved

Language: Английский

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Phenanthraquinone modified carbon quantum dots covalent-grafted onto Cu-MOF for photocatalytic CO2 reduction: Construction of dual-active sites and parallel charge channels based on the cooperation between photoexcitation and electron-entrap

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 349, P. 123857 - 123857

Published: April 24, 2024

Language: Английский

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Constructing Donor–Acceptor-Linked COFs Electrolytes to Regulate Electron Density and Accelerate the Li+ Migration in Quasi-Solid-State Battery

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 17(1)

Published: Sept. 26, 2024

Abstract Regulation the electronic density of solid-state electrolyte by donor–acceptor (D–A) system can achieve highly-selective Li + transportation and conduction in metal batteries. This study reports a high-performance thorough D–A-linked covalent organic frameworks (COFs) based on intramolecular charge transfer interactions. Unlike other reported COF-based electrolyte, developed concept with COFs not only achieves modulation to promote migration inhibit dendrite, but also offers crucial opportunity understand role The introduced strong electronegativity F-based ligand COF results (transference number 0.83), high ionic conductivity (6.7 × 10 –4 S cm −1 ), excellent cyclic ability (1000 h) symmetric cell high-capacity retention Li/LiFePO 4 (90.8% for 300 cycles at 5C) than substituted C- N-based ligands. is ascribed outstanding D–A interaction between donor porphyrin acceptor F atoms, which effectively expedites electron transferring from enhances kinetics. Consequently, we anticipate that this work creates insight into strategy accelerating batteries through system.

Language: Английский

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