Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Май 25, 2022

Methane (CH4) oxidation to high value chemicals under mild conditions through photocatalysis is a sustainable and appealing pathway, nevertheless confronting the critical issues regarding both conversion selectivity. Herein, visible irradiation (420 nm), synergy of palladium (Pd) atom cocatalyst oxygen vacancies (OVs) on In2O3 nanorods enables superior photocatalytic CH4 activation by O2. The optimized catalyst reaches ca. 100 μmol h-1 C1 oxygenates, with selectivity primary products (CH3OH CH3OOH) up 82.5%. Mechanism investigation elucidates that such induced dedicated function Pd single atoms boosting hole electron transfer, respectively. O2 proven be only source for CH3OH production, while H2O acts as promoter efficient ·OH production facilitates product desorption indicated DFT modeling. This work thus provides new understandings simultaneous regulation activity cocatalysts vacancies.

Язык: Английский

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Cocatalyst decorated ZnIn2S4 composites for cooperative alcohol conversion and H2 evolution

Applied Catalysis B Environment and Energy, Год журнала: 2021, Номер 298, С. 120541 - 120541

Опубликована: Июль 19, 2021

Язык: Английский

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Binary Au–Cu Reaction Sites Decorated ZnO for Selective Methane Oxidation to C1 Oxygenates with Nearly 100% Selectivity at Room Temperature

Journal of the American Chemical Society, Год журнала: 2021, Номер 144(2), С. 740 - 750

Опубликована: Дек. 20, 2021

Direct and efficient oxidation of methane to methanol the related liquid oxygenates provides a promising pathway for sustainable chemical industry, while still remaining an ongoing challenge owing dilemma between activation overoxidation. Here, ZnO with highly dispersed dual Au Cu species as cocatalysts enables selective photocatalytic conversion one-carbon (C1) using O2 oxidant operated at ambient temperature. The optimized AuCu-ZnO photocatalyst achieves up 11225 μmol·g-1·h-1 primary products (CH3OH CH3OOH) HCHO nearly 100% selectivity, resulting in 14.1% apparent quantum yield 365 nm, much higher than previous best photocatalysts reported oxygenates. In situ EPR XPS disclose that serve photoinduced electron mediators promote •OOH, simultaneously is hole acceptor enhance H2O •OH, thus synergistically promoting charge separation transformation. This work highlights significances co-modification suitable on simultaneous regulation activity selectivity.

Язык: Английский

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POM-incorporated ZnIn2S4 Z-scheme dual-functional photocatalysts for cooperative benzyl alcohol oxidation and H2 evolution in aqueous solution

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 306, С. 121087 - 121087

Опубликована: Янв. 7, 2022

Язык: Английский

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Carbon nitride based materials: more than just a support for single-atom catalysis

Chemical Society Reviews, Год журнала: 2023, Номер 52(15), С. 4878 - 4932

Опубликована: Янв. 1, 2023

Recently, the missing link between homogeneous and heterogeneous catalysis has been found it was named single-atom (SAC). However, SAC field still faces important challenges, one of which is controlling bonding/coordination single atoms support in order to compensate for increase surface energy when particle size reduced due atomic dispersion. Excellent candidates meet this requirement are carbon nitride (CN)-based materials. Metal can be firmly trapped nitrogen-rich coordination sites CN materials, makes them a unique class hosts preparing catalysts (SACs). As most promising two-dimensional supports stabilize isolated metal atoms, materials have increasingly employed SACs. Herein, we will cover recent advances single-atoms supported by In review, characterization techniques challenges faced topic discussed, commonly synthetic methods delineated different Finally, catalytic performance SACs based on nitrides reviewed with special focus their photocatalytic applications. particular, prove as non-innocent support. The relationship two-way, where change electronic properties support, while features matrix tune activity reactions. highlight frontiers field, including analytical method development, truly controlled methods, allowing fine control loading multi-element synthesis, how understanding two-way exchange behind push next level.

Язык: Английский

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Atomic‐Layered Cu₅ Nanoclusters on FeS₂ with Dual Catalytic Sites for Efficient and Selective H₂O₂ Activation

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(21)

Опубликована: Март 3, 2022

Regulating the distribution of reactive oxygen species generated from H2 O2 activation is prerequisite to ensuring efficient and safe use in chemistry life science fields. Herein, we demonstrate that constructing a dual Cu-Fe site through self-assembly single-atomic-layered Cu5 nanoclusters onto FeS2 surface achieves selective with high efficiency. Unlike its unitary Cu or Fe counterpart, sites residing at perimeter zone /FeS2 interface facilitate adsorption barrierless decomposition into ⋅OH via forming bridging Cu-O-O-Fe complex. The robust situ formation governed by this atomic-layered catalyst enables effective oxidation several refractory toxic pollutants across broad pH range, including alachlor, sulfadimidine, p-nitrobenzoic acid, p-chlorophenol, p-chloronitrobenzene. This work highlights concept building catalytic manipulating on molecular level towards environmental control beyond.

Язык: Английский

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Recent advances in Metal-Organic Frameworks-based materials for photocatalytic selective oxidation

Coordination Chemistry Reviews, Год журнала: 2021, Номер 450, С. 214240 - 214240

Опубликована: Окт. 13, 2021

Язык: Английский

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Photoreforming of Waste Polymers for Sustainable Hydrogen Fuel and Chemicals Feedstock: Waste to Energy

Chemical Reviews, Год журнала: 2023, Номер 123(8), С. 4443 - 4509

Опубликована: Апрель 17, 2023

Energy from renewable resources is central to environmental sustainability. Among the renewables, sunlight-driven fuel synthesis a sustainable and economical approach produce vectors such as hydrogen through water splitting. The photocatalytic splitting limited by oxidation half-reaction, which kinetically energetically demanding entails designer photocatalysts. Such challenges can be addressed employing alternative half-reactions. Photoreforming drive breakdown of waste plastics biomass into valuable organic products for production H2. We provide an overview photoreforming its underlying mechanisms that convert polymers H2 fuels fine chemicals. This paramount importance two complementary perspectives: (i) green energy harvesting (ii) sustainability decomposing valuables. Competitive results generation without hazards are being generated. process, mechanisms, critical assessment field scarce. address points focusing on concept up-to-date knowledge with key milestones achieved, uncovering concepts in photoreforming, (iii) design photocatalysts pathways use different polymer wastes substrates.

Язык: Английский

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A review on photo-, electro- and photoelectro- catalytic strategies for selective oxidation of alcohols

Journal of Energy Chemistry, Год журнала: 2022, Номер 77, С. 80 - 118

Опубликована: Ноя. 1, 2022

Язык: Английский

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Selective Enhancement of Photo‐Piezocatalytic Performance in BaTiO₃ Via heterovalent Ion Doping

Advanced Functional Materials, Год журнала: 2022, Номер 32(52)

Опубликована: Окт. 17, 2022

Abstract This study proposes a strategy based on heterovalent ion doping that gives rise to synergistic piezo‐phototronic effect with significantly improved catalytic activity and leads selective enhancement for specific pollutants. Owing the enhanced light absorption, hydrogen evolution rates are as high 3704 3178 µmolg −1 h in 0.01Li‐doped BaTiO 3 0.02La‐doped nanosheets, respectively, under simultaneous irradiation by ultrasound light, factor of 4.6 3.9 times higher than pure . The performance also far exceeds single piezocatalysis, photocatalysis, or sum two Li/La‐doped nanosheets due effects piezoelectric field promoting photo‐induced separation electron‐hole pairs. Further, carefully selecting donor acceptor doping, significant catalyst pollutants is obtained controlling band structure. Compared , possesses anionic dyes such Methyl blue Malachite Green, reaching 0.067 1.379 min while exhibits better cationic Rhodamine B Orange, degradation up 0.274 0.029 respectively. offers path design efficient piezocatalysts applications.

Язык: Английский

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