Tropospheric Aqueous-Phase Chemistry: Kinetics, Mechanisms, and Its Coupling to a Changing Gas Phase

Chemical Reviews, Journal Year: 2015, Volume and Issue: 115(10), P. 4259 - 4334

Published: May 7, 2015

ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTTropospheric Aqueous-Phase Chemistry: Kinetics, Mechanisms, and Its Coupling to a Changing Gas PhaseHartmut Herrmann*, Thomas Schaefer, Andreas Tilgner, Sarah A. Styler, Christian Weller, Monique Teich, Tobias OttoView Author Information Atmospheric Chemistry Department (ACD), Leibniz Institute for Tropospheric Research (TROPOS), Permoserstraße 15, 04318 Leipzig, Germany*Phone: ++49341 2717 7024. Fax: ++ 49341 99 E-mail: [email protected]Cite this: Chem. Rev. 2015, 115, 10, 4259–4334Publication Date (Web):May 7, 2015Publication History Received15 August 2014Published online7 May 2015Published inissue 27 2015https://doi.org/10.1021/cr500447kCopyright © 2015 American Chemical Society. This publication is licensed under these Terms of Use. Request reuse permissions Open Access the license indicated. Learn MoreArticle Views16652Altmetric-Citations385LEARN ABOUT THESE METRICSArticle Views are COUNTER-compliant sum full text article downloads since November 2008 (both PDF HTML) across all institutions individuals. These metrics regularly updated 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 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 InReddit (7 MB) Get e-AlertscloseSUBJECTS:Aerosols,Anions,Kinetic parameters,Organic reactions,pH e-Alerts

Language: Английский

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Environment-Friendly Carbon Quantum Dots/ZnFe₂O₄ Photocatalysts: Characterization, Biocompatibility, and Mechanisms for NO Removal

Environmental Science & Technology, Journal Year: 2017, Volume and Issue: 51(5), P. 2924 - 2933

Published: Feb. 1, 2017

A highly efficient and environmentally-friendly oxidation process is always desirable for air purification. This study reported a novel carbon quantum dots (CQDs)/ZnFe2O4 composite photocatalyst the first time through facile hydrothermal process. The CQDs/ZnFe2O4 (15 vol %) demonstrates stronger transient photocurrent response, approximately 8 times higher than that of ZnFe2O4, indicating superior transfer efficiency photogenerated electrons separation electron–hole pairs. Compared with pristine ZnFe2O4 nanoparticles, displayed enhanced photocatalytic activities on gaseous NOx removal high selectivity nitrate formation under visible light (λ > 420 nm) irradiation. Electron spin resonance analysis series radical-trapping experiments showed reactive species contributing to NO elimination were ·O2– ·OH radicals. possible mechanisms proposed regarding how CQDs improve performance ZnFe2O4. are believed act as an electron reservoir transporter well powerful energy-transfer component during photocatalysis processes over samples. Furthermore, toxicity assessment authenticated good biocompatibility low cytotoxity CQDs/ZnFe2O4. results this indicate promising

Language: Английский

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Oxygen Vacancies Promoted the Selective Photocatalytic Removal of NO with Blue TiO₂ via Simultaneous Molecular Oxygen Activation and Photogenerated Hole Annihilation

Environmental Science & Technology, Journal Year: 2019, Volume and Issue: 53(11), P. 6444 - 6453

Published: May 3, 2019

Semiconductor photocatalytic technology has great potential for the removal of dilute gaseous NO in indoor and outdoor atmospheres but suffers from unsatisfactory NO-removal selectivity due to undesirable NO2 byproduct generation. In this study, we demonstrate that 99% oxidation toward nitrate can be achieved over blue TiO2 bearing oxygen vacancies (OVs) under visible-light irradiation. First-principles density functional theory calculation experimental results suggested OVs with localized electrons could facilitate molecular activation through single-electron pathways generate ·O2– simultaneously promote photogenerated hole annihilation. The generated directly converted nitrate, while annihilation inhibited side-reaction between holes avoid toxic formation, resulting highly selective NO. This study reveals dual functions defective photocatalysts also provides fundamental guidance purification technology.

Language: Английский

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Fabrication of Bi2O2CO3/g-C3N4 heterojunctions for efficiently photocatalytic NO in air removal: In-situ self-sacrificial synthesis, characterizations and mechanistic study

Applied Catalysis B Environment and Energy, Journal Year: 2016, Volume and Issue: 199, P. 123 - 133

Published: June 12, 2016

Language: Английский

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Unexpectedly high indoor hydroxyl radical concentrations associated with nitrous acid

Proceedings of the National Academy of Sciences, Journal Year: 2013, Volume and Issue: 110(33), P. 13294 - 13299

Published: July 29, 2013

The hydroxyl (OH) radical is the most important oxidant in atmosphere since it controls its self-oxidizing capacity. main sources of OH radicals are photolysis ozone and nitrous acid (HONO). Due to attenuation solar radiation indoor environment, possibility formation through photolytic pathways indoors has been ignored up now. In air, ozonolysis alkenes suggested as an alternative route formation. Models indirect measurements performed now according this hypothesis suggest concentrations on order 10 4 –10 5 molecules per cubic centimeter. Here, we present direct significant amounts 1.8⋅10 6 centimeter during experimental campaign carried out a school classroom Marseille. This concentration same magnitude outdoor levels urban scenario. We also show that HONO source under certain conditions (i.e., irradiation inside room). Additionally, were found follow linear dependence with product J(HONO)⋅[HONO]. was supported by using simple quasiphotostationary state model budget. These findings force change our understanding air quality because reactivity linked would involve secondary species chemical reactions potentially more hazardous than primary pollutants air.

Language: Английский

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Recent advances on cobalt metal organic frameworks (MOFs) for photocatalytic CO2 reduction to renewable energy and fuels: A review on current progress and future directions

Energy Conversion and Management, Journal Year: 2022, Volume and Issue: 253, P. 115180 - 115180

Published: Jan. 5, 2022

Language: Английский

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Hydroxyl Radical‐Mediated Efficient Photoelectrocatalytic NO Oxidation with Simultaneous Nitrate Storage Using A Flow Photoanode Reactor

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(28)

Published: May 16, 2023

The selective conversion of dilute NO pollutant into low-toxic product and simultaneous storage metabolic nitrogen for crop plants remains a great challenge from the perspective waste management sustainable chemistry. This study demonstrates that this bottleneck can be well tackled by refining reactive oxygen species (ROS) on Ni-modified NH2 -UiO-66(Zr) (Ni@NU) using nickel foam (NF) as three-dimensional (3D) substrate through flow photoanode reactor via gas-phase photoelectrocatalysis. By rationally ROS to ⋅OH, Ni@NU/NF rapidly eliminate 82 % without releasing remarkable NO2 under low bias voltage (0.3 V) visible light irradiation. abundant mesoporous pores are conducive diffusion formed nitrate, which enables progressive nitrate with selectivity over 99 long-term use. Through calculation, 90 could recovered species, indicating state-of-the-art strategy capture, enrich recycle N source atmosphere. offers new treatment exploitation, may possess potential development highly efficient air purification systems industrial indoor NOx control.

Language: Английский

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Targeted NO Oxidation and Synchronous NO₂ Inhibition via Oriented ¹O₂ Formation Based on Lewis Acid Site Adjustment

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(34), P. 12890 - 12900

Published: Aug. 17, 2023

An appealing strategy for ensuring environmental benefits of the photocatalytic NO oxidation reaction is to convert into NO3- instead NO2, yet selectivity products remains challenging. Here, such a scenario could be realized by tailoring exposure Lewis acid sites on surface ZrO2, aiming precisely regulate ROS evolution process selective NO3-. As evidenced highly combined experimental characterizations and density functional theory (DFT) simulations, serving as electron acceptors induce itinerant redistribution, charge-carrier transfer, further •O2-, which promotes oriented formation 1O2. result, monoclinic ZrO2 with more exhibited an outstanding conversion efficiency (56.33%) extremely low NO2 (5.04%). The ROS-based promotion mechanism performance have been revealed basis ESR analysis, ROS-quenching experiments, in situ DRIFTS. This work provide critical view toward advance unique

Language: Английский

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Visible-Light-Active Plasmonic Ag–SrTiO₃ Nanocomposites for the Degradation of NO in Air with High Selectivity

ACS Applied Materials & Interfaces, Journal Year: 2016, Volume and Issue: 8(6), P. 4165 - 4174

Published: Jan. 22, 2016

Harnessing inexhaustible solar energy for photocatalytic disposal of nitrogen oxides is great significance nowadays. In this study, Ag-SrTiO3 nanocomposites (Ag-STO) were synthesized via one-pot solvothermal method the first time. The deposition Ag nanoparticles incurs a broad plasmonic resonance absorption in visible light range, resulting enhanced driven activity on NO removal comparison with pristine SrTiO3. loading amount has significant influence properties Ag-STO, which further affects efficiency. It was shown that 0.5% onto SrTiO3 (in mass ratio) could remove 30% single reaction path under irradiation, twice higher than achieved Most importantly, generation harmful intermediate (NO2) largely inhibited over and Ag-STO nanocomposites, can be ascribed to basic surface property strontium sites. As identified by electron spin (ESR) spectra,·O2(-) ·OH radicals are major reactive species oxidation. Essentially speaking, abundance oxygen produced responsible improved activity. This work provides facile controllable route fabricate nanocomposite photocatalyst featuring high selectivity abatement.

Language: Английский

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Photosensitized Production of Atmospherically Reactive Organic Compounds at the Air/Aqueous Interface

Journal of the American Chemical Society, Journal Year: 2015, Volume and Issue: 137(26), P. 8348 - 8351

Published: June 12, 2015

We report on experiments that probe photosensitized chemistry at the air/water interface, a region does not just connect two phases but displays its own specific chemistry. Here, we follow reactions of octanol, proxy for environmentally relevant soluble surfactants, initiated by an attack triplet-state carbonyl compounds, which are themselves concentrated interface presence this surfactant. Gas-phase products determined using PTR-ToF-MS, and those remaining in organic layer ATR-FTIR spectroscopy HPLC-HRMS. observe production carboxylic acids as well unsaturated branched-chain oxygenated products, compounds act aerosol precursors had been thought to be produced solely biological activity. A mechanism is consistent with observations detailed here, energetics several key calculated quantum chemical methods. The results suggest concentrating nature leads being favorable venue radical yielding complex functionalized could initiate further secondary new particle formation atmospheric environment.

Language: Английский

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