Quantum Dot-Sensitized Triplet–Triplet Annihilation Photon Upconversion for Solar Energy Conversion and beyond

Accounts of Materials Research, Journal Year: 2024, Volume and Issue: 5(2), P. 136 - 145

Published: Feb. 7, 2024

ConspectusThe Nobel Prize in Chemistry 2023 was awarded to Moungi G. Bawendi, Louis E. Brus, and Aleksey Ekimov for the discovery synthesis of quantum dots (QDs). Since QDs 1980s, endeavors have been put improve synthetic strategies with controllable sizes, crystal structures, surfaces. With development about half a century, used multiple optoelectronic applications, which are based on conversion between one photon exciton. In this case, photons energies lower than bandgap cannot be absorbed by semiconductors. For example, solar cells or photocatalysts transparent sub-bandgap near-infrared (NIR) light spectrum, rendering transmission loss.Photon upconversion (PUC), combination low-energy high-energy one, plays critical role reshaping spectrum mitigating energy loss. Among different achieve PUC, QD sensitized triplet–triplet annihilation PUC exhibits high response irradiation, makes it an ideal strategy conversion.Here, we introduce QD-sensitized emphasize how is applied conversion. This Account starts introduction acting as active materials directly convert electricity chemical bonds due strong absorptivity, flexible tunable surface chemistry, capability accommodating transferring electrons/holes. Then move can upconvert NIR under one-sun condition. We discuss deconvolution total QY into efficiencies triplet transfer from sensitizers organic emitters, annihilation, singlet emission emitters. Next, summarize progress PUC-enhanced photovoltaics photochemical reactions. photovoltaics, two examples that beyond 1100 nm, possible couple Si-based cells. reactions, discussion separated visible-to-ultraviolet ultraviolet light-triggered reactions NIR-to-visible visible last section, point out challenges future directions field. low solid-state reabsorption must overcome photovoltaic application, more types PUC-assisted explored. also propose other potential applications such biological imaging phototherapy. hope will help readers understand systems promote application efficient beyond.

Language: Английский

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Hole Polaron‐Mediated Suppression of Electron–Hole Recombination Triggers Efficient Photocatalytic Nitrogen Fixation

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

Published: Aug. 30, 2024

In the pursuit of successful photocatalytic transformations, challenges persist due to limitations in charge carrier utilization and transfer efficiency, which stemming from rapid recombination. Overcoming these necessitates exploration novel mechanisms that enhance effective separation photogenerated electron-hole pairs. Herein, deviating conventional approach enhancing migration separate charges extend their lifetime, proposal is directly prevent recombination electrons holes by forming hole polarons. Specifically, disordered pores are introduced on surface KTaO

Language: Английский

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人工光合固氮

Chinese Science Bulletin (Chinese Version), Journal Year: 2025, Volume and Issue: 70(7), P. 835 - 849

Published: Feb. 18, 2025

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A Supramolecular Artificial Light-Harvesting System with Excitation Energy and Electron Transfer

ACS Materials Letters, Journal Year: 2023, Volume and Issue: 6(1), P. 290 - 297

Published: Dec. 19, 2023

We present a supramolecular artificial light-harvesting system that combines excitation energy and electron transfer to drive chemical reactions. Different from the traditional system, this tailored assembly realizes construction of fully functionalized including light capture, transfer, solar-to-chemical conversion. A tetraphenylethylene derivative (D) was chosen as antenna chromophores coassembled with an iodide BODIPY (A) produce quadruple hydrogen-bonded assembly. D photoirradiated excited singlet state, subsequently undergoing (EET) high efficiency (ΦEET = 95.3%). Then, captured nearby generate radical ions D+• A–•, leading charge-separation This used important compound, hydrogen peroxide. In addition, it applied kill tumor cells by oxidizing NADH generating cytotoxic reactive oxygen species.

Language: Английский

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A temperature-responsive artificial light-harvesting system in water with tunable white-light emission

Journal of Materials Chemistry A, Journal Year: 2023, Volume and Issue: 11(34), P. 18419 - 18425

Published: Jan. 1, 2023

A tadpole-type amphiphilic monomer containing cyanostilbene and oligo(ethylene glycol) chains has been designed synthesized, which can be used to construct a thermo-responsive light-harvesting system in water with tunable white-light emission.

Language: Английский

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Functional Regulation of Covalent Organic Frameworks for Photocatalytic Water Splitting

ACS Materials Letters, Journal Year: 2024, Volume and Issue: 6(6), P. 2276 - 2294

Published: May 10, 2024

Solar-driven water splitting into hydrogen and oxygen fuels represents a promising way for clean energy production to achieve carbon-neutral future. The efficiency of photocatalytic strongly relies on the development high-performance catalysts. Noteworthily, covalent organic frameworks (COFs) offer distinctive platform designing photo-to-chemical conversion, benefiting from their tailorable structure, ultrahigh porosity, robust framework, sufficient light absorption, rich active sites. Herein we highlight systematic overview recent research progress using COFs half-reactions overall splitting. With an aim shed understanding structural design COF photocatalysts splitting, various functional strategies are discussed. Finally, major challenges future perspectives proposed with hope achieving ongoing this emerging field.

Language: Английский

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Host‐Guest Approach to Promoting Photocatalysis Based on Consecutive Photo‐Induced Electron‐Transfer Processes via Efficient Förster Resonance Energy Transfer

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(37)

Published: May 29, 2024

Abstract Supramolecular artificial light‐harvesting system with highly efficient host–guest energy transfer pathway provides an ideal platform for optimizing the photochemistry process. The consecutive photo‐induced electron (conPET) process overcomes limitation of visible‐light photocatalysis, but is often compromised by mismatching between absorption ground state dye and its radical, weakening efficiency photoredox reaction. By encapsulating a conPET photocatalyst rhodamine 6G into metal‐organic cage, supramolecular approach was undertaken to tackle intrinsic difficulty matching light photoexcitation radical. Förster resonance from photoexcited cage forced encapsulation facilitates single‐wavelength light‐driven activation aryl halides stabilizing accelerating production accumulation radical intermediate. tunable flexible nature complex renders cage‐based strategy promising development photocatalysts toward better utilization solar energy.

Language: Английский

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Visible-Light-Mediated Ruthenium-Catalyzed para-Selective Alkylation of Unprotected Anilines

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(11), P. 7310 - 7321

Published: May 15, 2023

Anilines are important moieties in organic chemistry, pharmaceuticals, and materials science. Although para-selective functionalization of anilides tertiary anilines is well established, unprotected have posed a challenge. Herein, we report visible-light-mediated Ru(II)-catalyzed para-alkylation anilines. The distinct Ru(II)–aniline complex enabled the reaction to proceed with extremely high efficiency (2 h) under mild conditions. good functional group tolerance allowed late-stage even aggregation-induced emission luminogen labeling natural products drugs. A mechanistic investigation suggests that crucial for both triggering controlling para-selectivity.

Language: Английский

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Photocatalytic hydrogen evolution and simultaneously converting high-concentration of thiols into disulfides with excellent yield under visible-light

Journal of Materials Chemistry A, Journal Year: 2023, Volume and Issue: 11(6), P. 2726 - 2736

Published: Jan. 1, 2023

CdS/P25/Ni 2 P were prepared for photocatalytic hydrogen-evolution and simultaneously converting high-concentration of thiols into disulfides with excellent yield under visible-light. A possible mechanism was proposed based on experiment data.

Language: Английский

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Concurrent Ammonia Synthesis and Alcohol Oxidation Boosted by Glutathione‐Capped Quantum Dots under Visible Light

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(24)

Published: March 19, 2024

Abstract Mother nature accomplishes efficient ammonia synthesis via cascade N 2 oxidation by lightning strikes followed with enzyme‐catalyzed nitrogen oxyanion (NO x − , = 2,3) reduction. The protein environment of enzymatic centers for NO ‐to‐NH 4 + process greatly inspires the design glutathione‐capped (GSH) quantum dots (QDs) under visible light (440 nm) in tandem plasma‐enabled oxidation. Mechanistic studies reveal that GSH induces positive shift surface charge to strengthen interaction between and QDs. Upon irradiation QDs, balanced rapid hole electron transfer furnish GS·radicals 2e /2H alcohol H·for 8e /10H 3 reduction simultaneously. For first time, mmol‐scale is realized apparent yields 5.45% ± 0.64%, gram‐scale value‐added acetophenone NH Cl proceeds 1:4 stoichiometry stability, demonstrating promising multielectron multiproton efficiency sustainability nature‐inspired artificial photocatalysts.

Language: Английский

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