Steering Electron–Hole Migration Pathways Using Oxygen Vacancies in Tungsten Oxides to Enhance Their Photocatalytic Oxygen Evolution Performance

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(15), P. 8236 - 8242

Published: Jan. 25, 2021

Abstract The overall water splitting efficiency is mainly restricted by the slow kinetics of oxygen evolution. Therefore, it essential to develop active evolution catalysts. In this context, we designed and synthesized a tungsten oxide catalyst with vacancies for photocatalytic evolution, which exhibited higher rate 683 μmol h −1 g than that pure WO 3 (159 ). Subsequent studies through transient absorption spectroscopy found can produce electron trapping states inhibit direct recombination photogenerated carriers. Additionally, Pt cocatalyst promote trap participate in reaction improve performance further. This work uses femtosecond explain mechanism inorganic materials provides new insights into design high‐efficiency water‐splitting

Language: Английский

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Copper‐Based Plasmonic Catalysis: Recent Advances and Future Perspectives

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(32)

Published: May 29, 2021

With the capability of inducing intense electromagnetic field, energetic charge carriers, and photothermal effect, plasmonic metals provide a unique opportunity for efficient light utilization chemical transformation. Earth-abundant low-cost Cu possesses tunable localized surface plasmon resonance from ultraviolet-visible to near infrared region. Moreover, essentially exhibits remarkable catalytic performance toward various reactions owing its intriguing physical properties. Coupling with light-harvesting ability function, serves as promising platform light-driven reaction. Herein, recent advancements Cu-based photocatalysis are systematically summarized, including designing synthetic strategies catalysts, performance, mechanistic understanding over catalysts. What's more, approaches enhancement efficiency construction active centers on catalysts highlighted discussed in detail, such morphology size control, regulation electronic structure, defect strain engineering, etc. Remaining challenges future perspectives further development catalysis also proposed.

Language: Английский

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Recognition in the Domain of Molecular Chirality: From Noncovalent Interactions to Separation of Enantiomers

Chemical Reviews, Journal Year: 2022, Volume and Issue: 122(16), P. 13235 - 13400

Published: Aug. 2, 2022

It is not a coincidence that both chirality and noncovalent interactions are ubiquitous in nature synthetic molecular systems. Noncovalent interactivity between chiral molecules underlies enantioselective recognition as fundamental phenomenon regulating life human activities. Thus, represent the narrative thread of fascinating story which goes across several disciplines medical, chemical, physical, biological, other natural sciences. This review has been conceived with awareness modern attitude toward its consequences needs to be founded on multidisciplinary approaches disclose basis essential phenomena domain With primary aim discussing this topic an integrated way, comprehensive pool rational systematic information provided, concerns fundamentals chirality, description interactions, their implications processes occurring different contexts. A specific focus devoted enantioselection chromatography electromigration techniques because unique feature "multistep" processes. second motivation for writing make clear statement about state art, tools we have at our disposal, what still missing fully understand mechanisms underlying recognition.

Language: Английский

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Coherent Two-Dimensional and Broadband Electronic Spectroscopies

Chemical Reviews, Journal Year: 2022, Volume and Issue: 122(3), P. 4257 - 4321

Published: Jan. 17, 2022

Over the past few decades, coherent broadband spectroscopy has been widely used to improve our understanding of ultrafast processes (e.g., photoinduced electron transfer, proton and proton-coupled transfer reactions) at femtosecond resolution. The advances in laser technology along with development nonlinear multidimensional enabled further insights into energy carrier relaxation complex biological material systems. New discoveries interpretations have led improved design principles for optimizing photophysical properties various artificial In this review, we first provide a detailed theoretical framework both two-dimensional electronic (2DES). We then discuss selection experimental approaches considerations 2DES best practices data processing analysis. Finally, review several examples where were employed reveal mechanisms photoinitiated molecular, biological, end brief perspective on future techniques themselves their potential answer an even greater range scientific questions.

Language: Английский

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Simultaneous benzyl alcohol oxidation and H2 generation over MOF/CdS S-scheme photocatalysts and mechanism study

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Journal Year: 2023, Volume and Issue: 51, P. 204 - 215

Published: Aug. 1, 2023

Language: Английский

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Ultrafast hot electron dynamics in plasmonic nanostructures: experiments, modelling, design

Nanophotonics, Journal Year: 2023, Volume and Issue: 12(1), P. 1 - 28

Published: Jan. 1, 2023

Metallic nanostructures exhibit localized surface plasmons (LSPs), which offer unprecedented opportunities for advanced photonic materials and devices. Following resonant photoexcitation, LSPs quickly dephase, giving rise to a distribution of energetic 'hot' electrons in the metal. These out-of-equilibrium carriers undergo ultrafast internal relaxation processes, nowadays pivotal variety applications, from photodetection sensing driving photochemical reactions all-optical modulation light. Despite intense research activity, exploitation hot real-world nanophotonic devices remains extremely challenging. This is due complexity inherent carrier phenomena at nanoscale, involving short-lived electronic states over very broad range energies, interaction with thermal phononic baths. issues call comprehensive understanding electron dynamics plasmonic nanostructures. paper aims review our contribution field: starting fundamental physics nanostructures, we first describe experimental techniques used probe electrons; then introduce numerical model nanoscale present examples experiments modelling are combined, aim designing novel optical functionalities enabled by hot-electron dynamics.

Language: Английский

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Optical Phenomena in Molecule-Based Magnetic Materials

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(9), P. 5930 - 6050

Published: April 30, 2024

Since the last century, we have witnessed development of molecular magnetism which deals with magnetic materials based on species, i.e., organic radicals and metal complexes. Among them, broadest attention was devoted to molecule-based ferro-/ferrimagnets, spin transition materials, including those exploring electron transfer, nanomagnets, such as single-molecule magnets (SMMs), qubits, stimuli-responsive materials. Their physical properties open application horizons in sensors, data storage, spintronics, quantum computation. It found that various optical phenomena, thermochromism, photoswitching characteristics, luminescence, nonlinear chiroptical effects, well responsivity external stimuli, can be implemented into Moreover, fruitful interactions these effects provide new cross-effects multifunctionality, enriching applications optical, electronic, devices. This Review aims show scope phenomena generated recent advances areas high-temperature photomagnetism, thermometry utilizing SMMs, addressability magneto-chiral dichroism, opto-magneto-electric multifunctionality. These findings are discussed context types accessible for classes

Language: Английский

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In Situ UV–Vis–NIR Absorption Spectroscopy and Catalysis

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(5), P. 2352 - 2418

Published: Feb. 26, 2024

This review highlights

Language: Английский

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Manipulating the Dynamics of Dark Excited States in Organic Materials for Phototheranostics

Accounts of Chemical Research, Journal Year: 2020, Volume and Issue: 54(3), P. 697 - 706

Published: Dec. 10, 2020

Manipulating the dynamics of dark excited states (DESs), such as higher singlet or triplet with no small radiative decay, are both fundamental and practical interests, an important application being photoactivated diagnosis therapy (phototheranostics), which include photoacoustic (PA) imaging, photodynamic (PDT), photothermal (PTT). However, current understanding DESs in organic structures is rather limited, thus making any rational manipulation DES materials very challenging.A decays primarily by radiationless transition through two pathways: (i) singlet-to-triplet intersystem crossing (ISC) (ii) internal conversion (IC) relaxation. The deactivation a via ISC can generate cytotoxic reactive oxygen species (ROS) for PDT, while IC could convert photons into heat PA imaging PTT. In this Account, we highlight our research on developing structure-property relationships relation to phototheranostic applications. We describe femtosecond transient absorption (fs-TA) spectroscopy obtaining valuable insights dynamics. Afterward, present work nonrigid molecules that revealed greatly enhanced geometry twisting, leads innovative pathway develop exhibiting external stimuli-responsive reversible switching ISC. introduce concept smart PDT where highly efficient imparted twisting acidic environment specific tumors localized leaving surrounding healthy tissues at different pH unaffected. This insightful lead development more advanced photosensitizers PDT. Two other emergent concepts from presented here (1) significantly producing strong local heating combining two-photon state cumulative multiphoton absorption, increasing strength signal nonlinear (2) shown example molecule, BODIPY, nanoscale charge-transfer mediated aggregate nanoparticles resulting exceptionally high efficiency 61% Some vivo results studies using BODIPY presented, providing elegant dynamics.This Account concludes summary discussion future perspectives. hope will deepen molecular control materials, hopefully enticing broad range scientists within disciplinary areas.

Language: Английский

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Free Charge Carriers in Homo-Sorted π-Stacks of Donor–Acceptor Conjugates

Chemical Reviews, Journal Year: 2021, Volume and Issue: 121(13), P. 8234 - 8284

Published: June 16, 2021

Inspired by the high photoconversion efficiency observed in natural light-harvesting systems, hierarchical organization of molecular building blocks has gained impetus past few decades. Particularly, arrangement and packing active layer organic solar cells (OSCs) have garnered significant attention due to decisive role nature donor/acceptor (D/A) heterojunctions charge carrier generation ultimately power conversion efficiency. This review focuses on recent developments emergent optoelectronic properties exhibited self-sorted donor-on-donor/acceptor-on-acceptor covalently linked D–A highlighting ultrafast excited state dynamics transfer transport. Segregated donors acceptors promotes delocalization photoinduced charges among stacks, engendering an enhanced separation lifetime percolation pathways with ambipolar conductivity yield. Covalently linking ensure a sufficient interface interchromophoric electronic coupling as required for faster while providing better control over their supramolecular assemblies. The design strategies attain conjugate assemblies optimal efficiency, scope application compared state-of-the-art OSCs, current challenges, future opportunities are discussed review. An integrated overview rational approaches derived from comprehension underlying processes can pave way toward superior devices bring new possibilities avenue functional architectures.

Language: Английский

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