Tuning Energy Transfer Pathways in Halide Perovskite–Dye Hybrids through Bandgap Engineering

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(5), P. 3352 - 3362

Published: Jan. 24, 2024

Lead halide perovskite nanocrystals, which offer rich photochemistry, have the potential to capture photons over a wide range of visible and infrared spectrum for photocatalytic, optoelectronic, photon conversion applications. Energy transfer from nanocrystal an acceptor dye in form triplet or singlet state offers additional opportunities tune properties semiconductor–dye hybrid extend excited-state lifetimes. We now successfully established key factors that dictate energy between excited CsPbI3 surface-bound rhodamine dyes using absorption emission spectroscopies. The pendant groups on influence surface binding turn kinetics, as well efficiency transfer. Of three investigated (rhodamine B, B isothiocyanate, rose Bengal), CsPbI3–rose Bengal with strongest showed highest (96%) rate constant 1 × 109 s–1. This is nearly 2 orders magnitude slower than observed pure-bromide CsPbBr3–rose (1.1 1011 s–1). Intriguingly, although single-halide CsPbBr3 nanocrystals selectively populate states Bengal, respectively, mixed perovskites were able generate mixture both states. By tuning bromide/iodide ratio thus bandgap CsPb(Br1–xIx)3 compositions, percentage singlets vs triplets delivered was systematically tuned 0 100%. perovskite-molecular hybrids discussed here provide new ways modulate semiconductor–molecular through functionalization donor engineering.

Language: Английский

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Recent advances in novel materials for photocatalytic carbon dioxide reduction

Carbon Neutralization, Journal Year: 2024, Volume and Issue: 3(1), P. 142 - 168

Published: Jan. 1, 2024

Abstract The conversion of CO 2 into chemical fuels, which can be stored and utilized through photocatalysis, represents an effective, environmentally friendly, sustainable means to address both environmental concerns energy shortages. , as a stable oxidation product, poses challenges for reduction light alone, necessitating the use catalysts. Thus, crucial aspect photocatalytic technology lies in development effective photocatalysts. Based on basic principle PCRR (photocatalytic reaction), review provides detailed introduction core issues process, including relationship between band gap catalyst performance, utilization photogenerated carriers, product selectivity, methods analysis. Then, recent research progresses various photocatalysts are reviewed form examples combined with above principles. Finally, this summarizes insights techniques enhancing activity while also offering future prospects field.

Language: Английский

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Key Materials and Fabrication Strategies for High-Performance Dye-Sensitized Solar Cells: Comprehensive Comparison and Perspective

ACS Energy Letters, Journal Year: 2025, Volume and Issue: unknown, P. 881 - 895

Published: Jan. 22, 2025

For more than three decades, dye-sensitized solar cells (DSSCs) have attracted numerous researchers as viable alternatives in photovoltaic technology. It offers several advantages, such using eco-friendly materials, inexpensive processing techniques, indoor potentials, and integrating photovoltaics into building applications. Nevertheless, DSSCs will require further development manufacturing methods materials to remain competitive with other thin-film technologies that offer high efficiency. is essential give an overview of the latest developments this area highlight primary elements required for realizing high-performance technologies, photoanode modification, dye formulation, electrolyte optimization. Recent advancements shown promising improvements copper-based electrolytes, new interface like preadsorbents or postadsorbents has also opened possibilities DSSCs. Here, we comprehensively compare discuss key device fabrication processes present future research perspectives.

Language: Английский

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Self-supported CsPbBr3/Ti3C2Tx MXene aerogels towards efficient photocatalytic CO2 reduction

Journal of Colloid and Interface Science, Journal Year: 2023, Volume and Issue: 643, P. 174 - 182

Published: April 7, 2023

Language: Английский

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Photocatalysis of Metallic Nanoparticles: Interband vs Intraband Induced Mechanisms

The Journal of Physical Chemistry C, Journal Year: 2023, Volume and Issue: 127(32), P. 15685 - 15698

Published: Aug. 4, 2023

Photocatalysis induced by localized surface plasmon resonance of metallic nanoparticles has been studied for more than a decade, but photocatalysis originating from direct interband excitations is still under-explored. The spectral overlap and the coupling these two optical regimes also complicate determination hot carriers' energy states eventually hinder accurate assignment their catalytic role in reactions. In this Featured Article, after reviewing previous studies, we suggest classifying photoexcitation via intra- transitions where physical carriers are well-defined. Intraband featured creating electrons above Fermi level suitable reductive pathways, whereas generating d-band holes below better oxidative pathways. Since contribution different regions excitations, wavelength dependence photocatalytic activities very helpful assigning which contribute to observed catalysis.

Language: Английский

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Environmental application of perovskite material for organic pollutant-enriched wastewater treatment

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 495, P. 215378 - 215378

Published: Aug. 10, 2023

Language: Английский

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Organolead Halide-Based Coordination Polymers: Intrinsic Stability and Photophysical Applications

Accounts of Chemical Research, Journal Year: 2023, Volume and Issue: 56(4), P. 452 - 461

Published: Jan. 31, 2023

ConspectusOrganolead halide-based photovoltaics are one of the state-of-the-art solar cell systems with efficiencies increasing to 25% over past decade, ascribed their high light-absorption coefficient, broad wavelength coverage, tunable band structure, and excellent carrier mobility. Indeed, these optical characteristics highly demanding in photocatalysis photoluminescence (PL), which also involve energy utilization charge transport. However, vast majority organolead halides ionically bonded structures susceptible degradation upon high-polarity protic molecules (e.g., water (vapor) alcohol), often inevitable many photochemical applications. Encapsulation is a commonly used stabilization approach by coating protective layers, avoiding direct contact between polar molecules. this may partially hinder light penetration inner hybrid halide materials, introduce new interface problems that important luminescent sensing. Therefore, developing intrinsically stable organometal hybrids major target for applications optoelectronic applications.In Account, recent research progress on synthesis coordination polymers variety photoactive described. Herein, we propose general strategy advance intrinsic stability crystalline materials using coordinating anionic organic linkers, occupy photophysical features analogous those perovskites. Unlike organoammonium cations as structures, structure-directing agents organocarboxylates) render well-defined metal-carboxylate motifs extended architectures spanning from low-dimensional (0D, 1D) high-dimensional cationic inorganic Pb-X-Pb (X = F-/Cl-/Br-/I-) sublattices. This family can endure chemically reactive environments wide range pH aqueous boiling condition, have been systematically investigated experimental studies theoretical calculations. Many chloride/bromide-based show air-stable, broadband self-trapped emission large Stokes shift color rendition, exhibiting absolute quantum yields 35-72%. Among them, porous frameworks blocks recognized rare class metal-organic (MOFs) constructed lead secondary building units (SBUs). They not only substantially higher light-harvesting carrier-transport properties than conventional metal oxide-based MOFs, but allow isoreticular modification regulate PL guest More importantly, combining characteristics, layered iodide polymer shows overall photocatalytic splitting without use any sacrificial agent under simulated sunlight illumination. Given choice structurally diverse organocarboxylate hope Account provides deep insights importance chemistry discovery expand

Language: Английский

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Design Principle of a Water-Dispersed Photocatalytic Perovskite through Ligand Deconstruction

ACS Energy Letters, Journal Year: 2023, Volume and Issue: 8(5), P. 2159 - 2168

Published: April 12, 2023

Strategically designed surface modifiers that produce stable perovskite nanocrystals (NCs) and allow efficient charge extraction in polar solvents are critical for photocatalysis. We a multifunctional bolaamphiphilic ligand (NKE-12) with multidentate ionic groups at both ends, which significantly increases the colloidal stability of CsPbBr3 NCs an aqueous medium without affecting their structural integrity catalytic attributes. Ligand deconstruction via K E fragmented ligands revealed synergistic actions cationic anionic functionalities passivation, phase separation, water localization away from NKE-12-modified NCs. Multidimensional nuclear magnetic resonance experiments contact angle measurements further suggested interactions improved hydrophilicity terminal account stability. Photogenerated hole-transfer dynamics CsPbBr3/NKE-12 to probe molecule 6,7-dihydroxycoumarin was studied using transient absorption spectroscopy. Overall, this study paves way design principles engineering develop water-stable photocatalysts.

Language: Английский

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Recent Advances and Opportunities in Low‐Dimensional Layered Perovskites for Emergent Applications beyond Photovoltaics

Advanced Materials Technologies, Journal Year: 2023, Volume and Issue: 8(17)

Published: June 21, 2023

Abstract Layered metal halide perovskites have attracted enormous research attention over the last few years, befitting their unique optical and electronic properties. Low‐dimensional layered demonstrate great potential for various optoelectronic sensing applications beyond photovoltaics. Herein, recent progress opportunities in 2D quasi‐2D light‐emitting diodes (LEDs), lasers, memristors, neuromorphic/synaptic applications, UV–vis photodetection, X‐ray detection, scintillators, photocatalytic are reviewed. First, crystal structure, characteristics, fundamental properties of discussed. Recent efforts developments perovskite with excellent luminescence Unique perovskites, such as negligible leakage current due to restricted carrier transport, high stability, hydrophobicity, make them viable memristor devices. After discussing neuromorphic devices using outstanding performance photodetection including polarization‐sensitive is recently proved a superior candidate detection stability. Further, scintillation ionizing radiation Finally, some very achievements present future outlook, exciting this burgeoning field highlighted.

Language: Английский

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Atomically Contacted Cs₃Bi₂Br₉ QDs@UiO‐66 Composite for Photocatalytic CO₂ Reduction

Small, Journal Year: 2024, Volume and Issue: 20(34)

Published: April 9, 2024

Abstract Metal halide perovskite quantum dots (QDs) are widely studied in the field of photocatalytic CO 2 due to their strong light absorption and long carrier migration length. However, it can not exhibit high catalytic performance because radiative recombination lack effective sites. organic frameworks (MOFs) encapsulated QDs only solve aforementioned problems, but also maintain own unique characteristics with ultra‐high specific surfaces area abundant metal In this work, lead‐free bismuth‐based into Zr‐based MOF (UiO‐66), which combines advantages power conversion efficiency surface porosity UiO‐66. addition, benefiting from close contact between Cs 3 Bi Br 9 UiO‐66 enables photogenerated electrons be rapidly transferred MOF. As a result, @UiO‐66 composite exhibits higher yield for reduction than that prepared large‐sized

Language: Английский

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