Photocatalytic toluene oxidation with nickel-mediated cascaded active units over Ni/Bi2WO6 monolayers

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: May 31, 2024

Abstract Adsorption and activation of C–H bonds by photocatalysts are crucial for the efficient conversion to produce high-value chemicals. Nevertheless, delivery surface-active oxygen species bond oxygenation inevitably needs overcome obstacles due separated active centers, which suppresses catalytic efficiency. Herein, Ni dopants introduced into a monolayer Bi 2 WO 6 create cascaded units consisting unsaturated W atoms Bi/O frustrated Lewis pairs. Experimental characterizations density functional theory calculations reveal that these special sites can establish an controllable oxidation process. The activated on readily transferred oxygenation. catalyst with mass fraction 1.8% exhibits excellent toluene rates high selectivity towards benzaldehyde. This study presents fascinating strategy through design units.

Language: Английский

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Optimizing low-temperature CO2 methanation through frustrated Lewis pairs on Ni/CeO2 catalysts

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 484, P. 149471 - 149471

Published: Feb. 17, 2024

Language: Английский

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Research progress of bimetallic catalysts for CO2 hydrogenation to methane

International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 58, P. 872 - 891

Published: Jan. 30, 2024

Language: Английский

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Design of catalysts for selective CO2 hydrogenation

Nature Synthesis, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 27, 2025

Language: Английский

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Improvement in the activity of Ru/ZrO2 for CO2 methanation by the enhanced hydrophilicity of zirconia

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 360, P. 124549 - 124549

Published: Aug. 28, 2024

Language: Английский

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CeO₂‐Based Frustrated Lewis Pairs via Defective Engineering: Formation Theory, Site Characterization, and Small Molecule Activation

Small, Journal Year: 2024, Volume and Issue: 20(26)

Published: Jan. 18, 2024

Abstract Activation of small molecules is considered to be a central concern in the theoretical investigation environment‐ and energy‐related catalytic conversions. Sub‐nanostructured frustrated Lewis pairs (FLPs) have been an emerging research hotspot recent years due their advantages molecule activation. Although progress applications FLPs increasingly reported, fundamental theories related structural formation, site regulation, mechanism not yet fully developed. Given this, it attempted demonstrate underlying theory corresponding regulation methods, its activation on using CeO 2 as representative metal oxide. Specifically, this paper presents three principles for constructing surfaces, feasible engineering methods sites are presented. Furthermore, cases where typical (e.g., hydrogen, carbon dioxide, methane oxygen, etc.) activated over analyzed. Meanwhile, future challenges development FLPs‐centered The insights presented may contribute FLPs, which can potentially provide inspiration broader catalysis involving

Language: Английский

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High-dispersed CeOx species on mesopores silica to accelerate Ni-catalysed CO2 methanation at low temperatures

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 479, P. 147453 - 147453

Published: Nov. 16, 2023

Language: Английский

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Overturning CO₂ Hydrogenation Selectivity by Tailoring the Local Electron Density of Ru/CeO₂ Catalysts

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(16), P. 12214 - 12224

Published: Aug. 1, 2024

Flexible tuning of the CO2 hydrogenation selectivity through properly designed catalysts to obtain desired high-added-value products is a promising strategy for addressing environmental and energy issues but also huge challenge. Herein, over commonly used Ru/CeO2 methanation was facilely overturned from ∼99% CH4 100% CO by tailoring local electron density Ru electronic interaction induced acceptors (Bi, In, Sn, etc.). Systematically, in situ spectroscopic characterizations DFT calculations reveal that owing electron-withdrawing role acceptor, sites lose more charges than unmodified catalyst, which weakens binding strength carbonyl further induces imbalance reaction barrier formate intermediates. Thus, original parallel processes involving generation (carbonyl route route) are transformed into preferential desorption CO, finally acquiring opposite selectivity. Importantly, such an general overturning product can be extended other Ni catalysts. This discovery may offer way develop with controllable

Language: Английский

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Comprehensive Density Functional and Kinetic Monte Carlo Study of CO₂ Hydrogenation on a Well-Defined Ni/CeO₂ Model Catalyst: Role of Eley–Rideal Reactions

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(4), P. 2284 - 2299

Published: Jan. 30, 2024

A detailed multiscale study of the mechanism CO2 hydrogenation on a well-defined Ni/CeO2 model catalyst is reported that couples periodic density functional theory (DFT) calculations with kinetic Monte Carlo (kMC) simulations. The includes an analysis role Eley-Rideal elementary steps for water formation step, which are usually neglected overall picture mechanism, catalytic activity, and selectivity. DFT chosen consisting Ni4 cluster supported CeO2 (111) show large enough adsorption energies along low energy barriers suggest this to be good option high selective methanation. kMC simulations results synergic effect between two 3-fold hollow sites some reactions dominant in one site, while other prefer another, nearly equivalent site. This even more evident explicitly including steps. reveal CO formed via dissociative pathway reverse water-gas shift reaction, methane → HCO CH CH2 CH3 CH4 mechanism. Overall, our importance point small Ni clusters surface as potential catalysts methanation under mild conditions, very active toward at higher temperatures.

Language: Английский

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Heterolytic H₂ Activation in Heterogeneous Hydrogenation/Hydroprocessing Catalysis

ChemCatChem, Journal Year: 2024, Volume and Issue: 16(8)

Published: Jan. 5, 2024

Abstract In heterogeneous catalysis, heterolytic H 2 activation for (selective) hydrogenation and hydroprocessing reactions involves the dissociation of adsorbed molecules into proton (H δ+ ) hydride δ− on catalyst surface. This approach offers several advantages, including high selectivity polar bond (s), a low energy barrier dissociation, capacity reaction‐favorable adsorption, reduced poisoning. requires construction frustrated Lewis pairs surface, satisfying specific criteria, such as having an abundant quantity with steric hindrance maintaining certain distance 3–5 Å between pairs. review highlights intrinsic properties based state‐of‐the‐art reports. The main components necessary this include supports strong basic sites and/or oxygen vacancies, metals single atom. For purpose, designed catalytic materials aim to strengthen acidity basicity, improve polarization pairs, enrich maximize interfacial area metal species base, enhance metal–support interaction. Therefore, catalysts retaining characteristics will be significantly effective in various reactions.

Language: Английский

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