Photoredox-catalyzed coupling of CO2 reduction and amines oxidation by Cu doped CdS quantum dots

Molecular Catalysis, Journal Year: 2024, Volume and Issue: 554, P. 113858 - 113858

Published: Jan. 20, 2024

Language: Английский

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Non‐Interacting Ni and Fe Dual‐Atom Pair Sites in N‐Doped Carbon Catalysts for Efficient Concentrating Solar‐Driven Photothermal CO₂ Reduction

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(50)

Published: Oct. 30, 2023

Solar-to-chemical energy conversion under weak solar irradiation is generally difficult to meet the heat demand of CO2 reduction. Herein, a new concentrated solar-driven photothermal system coupling dual-metal single-atom catalyst (DSAC) with adjacent Ni-N4 and Fe-N4 pair sites designed for boosting gas-solid reduction H2 O simulated irradiation, even ambient sunlight. As expected, (Ni, Fe)-N-C DSAC exhibits superior catalytic performance CO (86.16 μmol g-1 h-1 ), CH4 (135.35 ) CH3 OH (59.81 which are equivalent 1.70-fold, 1.27-fold 1.23-fold higher than those Fe-N-C catalyst, respectively. Based on theoretical simulations, Fermi level d-band center Fe atom efficiently regulated in non-interacting Ni dual-atom electronic interaction through electron orbital hybridization DSAC. Crucially, distance between atoms Ni-N-N-Fe configuration means that additional as active site contributes main *COOH *HCO3 dissociation optimize corresponding barriers reaction process, leading specific dual pathways (COOH HCO3 pathways) initial production.

Language: Английский

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MoS2 decorated CdS composite catalyst for photoredox-mediated C–N coupling of amines to imines and hydrogen production

Molecular Catalysis, Journal Year: 2024, Volume and Issue: 557, P. 113991 - 113991

Published: Feb. 29, 2024

Language: Английский

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Photoredox-promoted co-production of 3,4-dihydroisoquinoline and H2 over Pd-doped leaf-like CdS catalyst

Molecular Catalysis, Journal Year: 2024, Volume and Issue: 561, P. 114178 - 114178

Published: April 26, 2024

Language: Английский

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Interface Synergy of Exposed Oxygen Vacancy and Pd Lewis Acid Sites Enabling Superior Cooperative Photoredox Synthesis

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(47)

Published: Aug. 13, 2024

Abstract Photo‐driven cross‐coupling of o ‐arylenediamines and alcohols has emerged as an alternative for the synthesis bio‐active benzimidazoles. However, tackling key problem related to efficient adsorption activation both coupling partners over photocatalysts towards activity enhancement remains a challenge. Here, we demonstrate interface synergy strategy by exposed oxygen vacancies (V O ) Pd Lewis acid sites benzimidazole hydrogen (H 2 coproduction Pd‐loaded TiO nanospheres with highest photoredox compared previous works so far. The results show that introduction V optimizes energy band structure supplies coordinatively unsaturated adsorbing activating ethanol molecules, affording acetaldehyde active intermediates. acts site, enhancing alkaline amine molecules via acid‐base pair interactions driving condensation process. Furthermore, synergistically promote interfacial charge transfer separation. This work offers new insightful guidance rational design semiconductor‐based at molecular level high‐performance renewable fuels value‐added feedstocks.

Language: Английский

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Interfacial Synergy of Ni Single Atom/Clusters and MXene Enabling Semiconductor Quantum Dots Based Superior Photoredox Catalysis

ACS Catalysis, Journal Year: 2024, Volume and Issue: 15(1), P. 129 - 138

Published: Dec. 16, 2024

Semiconductor-based photocatalysis has evolved over the past decade into a prevalent approach for alcohol oxidation to afford corresponding carbonyl compounds or C–C/C–O coupled products. Nonetheless, photocatalytic oxidative lactonization of diols lactones still significantly lags behind, even though represent class ring moieties with excellent biological activities. In this work, we present high-performance visible-light-mediated and H2 Ti3C2Tx MXene-supported CdS quantum dots (QDs) Ni decoration (Ni/CdS/Ti3C2Tx). acts as two-dimensional platform immobilizing promote separation migration charge carriers, while concomitantly Cd2+ confinement effect retards hole-induced photocorrosion CdS. The unique modifications atomically dispersed species are either incorporated clusters in accelerate evolution, anchored single atom on efficient adsorption cyclization diols. optimized Ni/CdS/Ti3C2Tx exhibits remarkably enhanced activity lactone synthesis, which is 80.4 times higher than that blank CdS, along selectivity high durability. This work brings conceptual idea overcome well-known intrinsic drawback photoinduced decomposition semiconductor-based photocatalysts offers generic robust strategy utilizing cocatalyst active sites photoredox synthesis evolution.

Language: Английский

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Engineering semiconductor quantum dots for co-upcycling of CO₂ and biomass-derived alcohol

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(30), P. 19029 - 19038

Published: Jan. 1, 2024

A heterointerface engineering strategy of immobilizing core–shell CdSe/CdS quantum dots onto SiO 2 spheres was realized to efficiently integrate CO photoreduction with the oxidation furfuryl alcohol in one system.

Language: Английский

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Efficient Photoredox Co-Upcycling of CO₂ and Plastic Waste by Band-Gap-Engineered Zn_xCd_1–xS Catalyst

ACS Materials Letters, Journal Year: 2024, Volume and Issue: 7(1), P. 359 - 367

Published: Dec. 24, 2024

Solar-driven CO2 reduction combined with plastic waste valorization presents a versatile approach to simultaneously reset misaligned hydrocarbon resources and achieve carbon-neutral cycle. Herein, we demonstrate co-upcycling heterogeneous photoredox catalysis for efficient tunable syngas, integrated polyethylene terephthalate (PET) conversion accessing acetate, over the spherical band-gap-engineered ZnxCd1–xS catalyst. The key steering syngas H2/CO rate is modulate conduction band bottom potentials of photocatalysts by altering Zn/Cd ratio, which results in production wide range. Moreover, controlled variations molar ratio regulate electron–hole separation capability, thereby endowing Zn0.8Cd0.2S optimum acetate rates. underlying mechanistic origin such redox reaction involving CO2-assisted PET has been systematically investigated. This win-win cooperative offers tantalizing possibility into value-added feedstocks.

Language: Английский

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Photocatalytic biomass conversion for hydrogen and renewable carbon-based chemicals

Joule, Journal Year: 2024, Volume and Issue: 8(3), P. 604 - 621

Published: Jan. 22, 2024

Language: Английский

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Recent Advances in Diverse MXenes‐Based Structures for Photocatalytic CO₂ Reduction into Renewable Hydrocarbon Fuels

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(19)

Published: Jan. 17, 2024

Abstract Photocatalytic CO 2 reduction into renewable hydrocarbon fuels is a green solution to address emission and energy issues simultaneously. However, the fast recombination of photogenerated charge carriers sluggish surface reaction kinetics restrict efficiency photocatalytic reduction. The emergence 2D MXenes has potential in improving reduction, owing their high electrical conductivity, flexible structural properties, abundant active sites. Hence, this review will concisely summarize highlight recent advances MXenes‐based photocatalysts used First, synthesis properties briefly introduced. Second, mechanism photoreduction along with roles are summarized, including promoting adsorption , enhancing separation photo‐induced carriers, acting as robust support, photothermal effect. Third, different kinds such MXenes/metal oxides, MXenes/nitrides, MXenes/LDH, MXenes/perovskite, MXene‐derived for classified via type semiconductors. Finally, challenges perspectives also presented, exploring suitable machine learning, uncovering structure‐activity relationship by situ, time‐ space‐resolved characterization techniques, anti‐oxidization ability, scale‐up applications.

Language: Английский

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