Graphitic Carbon Nitride (g-C₃N₄)-Based Photocatalysts for Artificial Photosynthesis and Environmental Remediation: Are We a Step Closer To Achieving Sustainability?

Chemical Reviews, Journal Year: 2016, Volume and Issue: 116(12), P. 7159 - 7329

Published: May 20, 2016

As a fascinating conjugated polymer, graphitic carbon nitride (g-C3N4) has become new research hotspot and drawn broad interdisciplinary attention as metal-free visible-light-responsive photocatalyst in the arena of solar energy conversion environmental remediation. This is due to its appealing electronic band structure, high physicochemical stability, "earth-abundant" nature. critical review summarizes panorama latest progress related design construction pristine g-C3N4 g-C3N4-based nanocomposites, including (1) nanoarchitecture bare g-C3N4, such hard soft templating approaches, supramolecular preorganization assembly, exfoliation, template-free synthesis routes, (2) functionalization at an atomic level (elemental doping) molecular (copolymerization), (3) modification with well-matched levels another semiconductor or metal cocatalyst form heterojunction nanostructures. The characteristics each classification system will be critically reviewed, namely metal-g-C3N4, semiconductor-g-C3N4, isotype g-C3N4/g-C3N4, carbon-g-C3N4, conducting polymer-g-C3N4, sensitizer-g-C3N4, multicomponent heterojunctions. structures, properties, optical absorption, interfacial charge transfer heterostructured nanohybrids also theoretically discussed based on first-principles density functional theory (DFT) calculations provide insightful outlooks carrier dynamics. Apart from that, advancement versatile photoredox applications toward artificial photosynthesis (water splitting photofixation CO2), decontamination, bacteria disinfection presented detail. Last but not least, this comprehensive conclude summary some invigorating perspectives challenges future directions forefront platform. It anticipated that can stimulate doorway facilitate next generation photocatalysts ameliorated performances by harnessing outstanding structural, electronic, properties for development sustainable without detriment.

Language: Английский

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Meso-Substituted Porphyrins for Dye-Sensitized Solar Cells

Chemical Reviews, Journal Year: 2014, Volume and Issue: 114(24), P. 12330 - 12396

Published: Dec. 12, 2014

ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTMeso-Substituted Porphyrins for Dye-Sensitized Solar CellsMaxence Urbani†‡, Michael Grätzel§, Mohammad Khaja Nazeeruddin*§, and Tomás Torres*†‡View Author Information† Departamento de Química Orgánica, Universidad Autónoma Madrid, Cantoblanco, 28049 Spain‡ Instituto Madrileño Estudios Avanzados (IMDEA)−Nanociencia, c/Faraday,9, Spain§ Laboratory of Photonics Interfaces, Institute Chemical Science Engineering, Swiss Federal Technology, Station 6, CH 1015 Lausanne, Switzerland*E-mail: [email protected]*E-mail: protected]Cite this: Chem. Rev. 2014, 114, 24, 12330–12396Publication Date (Web):December 12, 2014Publication History Received7 April 2014Published online12 December inissue 24 2014https://pubs.acs.org/doi/10.1021/cr5001964https://doi.org/10.1021/cr5001964review-articleACS PublicationsCopyright © 2014 American SocietyRequest reuse permissionsArticle Views11755Altmetric-Citations844LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum full text article downloads since November 2008 (both PDF HTML) across all institutions individuals. These metrics regularly updated to reflect usage leading up last few days.Citations number other articles citing this article, calculated by Crossref daily. Find more information about citation counts.The Altmetric Attention Score is a quantitative measure attention that research has received online. Clicking on donut icon will load page at altmetric.com with additional details score social media presence given article. how calculated. Share Add toView InAdd Full Text ReferenceAdd Description ExportRISCitationCitation abstractCitation referencesMore Options onFacebookTwitterWechatLinked InRedditEmail Other access optionsGet e-Alertsclose SUBJECTS:Dyes pigments,Oxides,Photovoltaics,Power conversion efficiency,Pyrroles Get e-Alerts

Language: Английский

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The PYXAID Program for Non-Adiabatic Molecular Dynamics in Condensed Matter Systems

Journal of Chemical Theory and Computation, Journal Year: 2013, Volume and Issue: 9(11), P. 4959 - 4972

Published: Oct. 14, 2013

This work introduces the PYXAID program, developed for non-adiabatic molecular dynamics simulations in condensed matter systems. By applying classical path approximation to fewest switches surface hopping approach, we have an efficient computational tool that can be applied study photoinduced at ab initio level systems composed of hundreds atoms and involving thousands electronic states. The technique is used detail ultrafast relaxation hot electrons crystalline pentacene. simulated occurs on a 500 fs time scale, excellent agreement with experiment, driven by lattice vibrations 200–250 cm–1 frequency range. program organized as Python extension module easily combined other Python-driven modules, enhancing user-friendliness flexibility software. source code additional information are available Web address http://gdriv.es/pyxaid. released under GNU General Public License.

Language: Английский

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Recent Advances and Perspectives on Nonadiabatic Mixed Quantum–Classical Dynamics

Chemical Reviews, Journal Year: 2018, Volume and Issue: 118(15), P. 7026 - 7068

Published: May 16, 2018

Nonadiabatic mixed quantum–classical (NA-MQC) dynamics methods form a class of computational theoretical approaches in quantum chemistry tailored to investigate the time evolution nonadiabatic phenomena molecules and supramolecular assemblies. NA-MQC is characterized by partition molecular system into two subsystems: one be treated mechanically (usually but not restricted electrons) another dealt with classically (nuclei). The subsystems are connected through couplings terms enforce self-consistency. A local approximation underlies classical subsystem, implying that direct can simulated, without needing precomputed potential energy surfaces. split allows reducing costs, enabling treatment realistic systems diverse fields. Starting from three most well-established methods—mean-field Ehrenfest, trajectory surface hopping, multiple spawning—this review focuses on programs developed last 10 years. It stresses relations between their domains application. electronic structure commonly used together reviewed as well. accuracy precision simulations critically discussed, general guidelines choose an adequate method for each application delivered.

Language: Английский

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2D phosphorene as a water splitting photocatalyst: fundamentals to applications

Energy & Environmental Science, Journal Year: 2016, Volume and Issue: 9(3), P. 709 - 728

Published: Jan. 1, 2016

In this review, we focus on analysing the fundamental electronic, optical and chemical properties of 2D phosphorene to assess its suitability as a metal-free water splitting photocatalyst.

Language: Английский

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Progress in Developing Metal Oxide Nanomaterials for Photoelectrochemical Water Splitting

Advanced Energy Materials, Journal Year: 2017, Volume and Issue: 7(19)

Published: June 12, 2017

Abstract Photoelectrochemical (PEC) water splitting represents an environmentally friendly and sustainable method to obtain hydrogen fuel. Semiconductor materials as the central components in PEC cells have decisive influences on device's solar‐to‐hydrogen conversion efficiency. Among semiconductors, metal oxides received a lot of attention due their outstanding (photo)‐electrochemical stability, low cost, favorable band edge positions wide distribution bandgaps. In past decades, significant processes been made developing oxide nanomaterials for splitting. this review, recent progress using photoelectrodes co‐catalysts is summarized. Their performance, limitations potentials are also discussed. Last, key challenges opportunities development implementation

Language: Английский

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Advanced Capabilities of the PYXAID Program: Integration Schemes, Decoherence Effects, Multiexcitonic States, and Field-Matter Interaction

Journal of Chemical Theory and Computation, Journal Year: 2014, Volume and Issue: 10(2), P. 789 - 804

Published: Jan. 10, 2014

In our previous work [J. Chem. Theory Comput. 2013, 9, 4959], we introduced the PYXAID program, developed for purpose of performing nonadiabatic molecular dynamics simulations in large-scale condensed matter systems. The methodological aspects and basic capabilities program have been extensively discussed. present work, perform a thorough investigation advanced namely, integration techniques time-dependent Schrodinger equation (TD-SE), decoherence corrections via decoherence-induced surface hopping, use multiexciton basis configurations, direct simulation photoexcitation explicit light–matter interaction. We demonstrate importance mentioned features by studying electronic variety particular, that solving TD-SE may lead to significant speedup calculations provide more stable solutions. show is necessary accurate description slow relaxation processes such as electron–hole recombination solid C60. By using configurations direct, nonperturbative treatment field–matter interactions, found nontrivial optimality conditions multiple exciton generation small silicon cluster.

Language: Английский

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Recent advances and perspectives for solar-driven water splitting using particulate photocatalysts

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(9), P. 3561 - 3608

Published: Jan. 1, 2022

Recent advances in particulate photocatalytic water splitting are reviewed and the pioneering works scalable H 2 evolution via OWS presented.

Language: Английский

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Coherent ultrafast charge transfer in an organic photovoltaic blend

Science, Journal Year: 2014, Volume and Issue: 344(6187), P. 1001 - 1005

Published: May 29, 2014

Blends of conjugated polymers and fullerene derivatives are prototype systems for organic photovoltaic devices. The primary charge-generation mechanism involves a light-induced ultrafast electron transfer from the light-absorbing electron-donating polymer to acceptor. Here, we elucidate initial quantum dynamics this process. Experimentally, observed coherent vibrational motion moiety after impulsive optical excitation donor. Comparison with first-principle theoretical simulations evidences between donor acceptor oscillations transferred charge 25-femtosecond period matching that modes. Our results show vibronic coupling electronic nuclear degrees freedom is key importance in triggering delocalization noncovalently bound reference system.

Language: Английский

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Thermally Activated Delayed Fluorescence (TADF) Path toward Efficient Electroluminescence in Purely Organic Materials: Molecular Level Insight

Accounts of Chemical Research, Journal Year: 2018, Volume and Issue: 51(9), P. 2215 - 2224

Published: Aug. 24, 2018

ConspectusSince the seminal work of Tang and Vanslyke in 1987 on small-molecule emitters that Friend co-workers 1990 conjugated-polymer emitters, organic light-emitting diodes (OLEDs) have attracted much attention from academia as well industry, OLED market is estimated to reach $30 billion mark by end 2018. In these first-generation basis simple spin statistics, electrical excitation resulted formation ∼25% singlet excitons ∼75% triplet excitons. Radiative decay ground state leads a prompt fluorescence emission, while only lead weak phosphorescence due very small spin–orbit couplings present purely molecules. The consequence ca. 75% energy loss, which triggered wide-ranging efforts try harvest many possible. 1998, Thompson, Forrest, their reported second-generation based coordination complexes with heavy transition metals (e.g., iridium or platinum). Here, stimulate efficient fast strong enabled heavy-metal atoms. Internal quantum efficiencies (IQE) up 100% been reported, means for every electron injected into device, photon emitted. While are those mainly exploited current applications, there impetus both cost environmental standpoints find new ways exploiting addition can offer greater flexibility fine-tune electronic optical properties synthetic chemistry toolbox.In 2012, Adachi introduced promising strategy, thermally activated delayed (TADF), molecular materials. These materials now represent third generation emitters. Impressive photophysical device performances internal also reaching nearly 100%.Our objectives this Account threefold: (i) lay out comprehensive description, at level, fundamental processes behind TADF emitters; (ii) discuss some challenges facing design such need balance efficiency thermal activation manifold radiative state; (iii) highlight briefly recent molecular-design strategies pave way classes

Language: Английский

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