En Route to Recyclable Semi-Heterogeneous Photocatalysis with Photoinert CeCl₃

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(10), P. 7664 - 7673

Published: May 2, 2024

Our study proposes an approach to semiheterogeneous photocatalysis, focusing on recyclability challenges. We developed a method employing visible light with photoinert anhydrous CeCl3, rendering it into reusable photocatalyst. Despite being and insoluble in organic solvents, CeCl3 formed transient charge transfer complex acetonitrile, denoted as - NXS (NBS or NCS), due the strong oxophilicity of trivalent cerium toward oxygen. This facilitated visible-light absorption, leading photoexcitation Ce(III) complexes conversion centers potent reductants, donating electrons NXS. As proof concept, we demonstrated reactions where NXS, upon accepting electrons, generated halide radicals, allowing synthesis gem-dihaloketones under sunlight from terminal aromatic alkynes via C–X cross-coupling reactions. Significantly, exhibited without notable decomposition, by its regeneration isolation through simple filtration postreaction, underscoring potential for prolonged use.

Language: Английский

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Exploring structures of Pd clusters on hydrogenated ceria surface using High-Dimensional neural network potential

Applied Surface Science, Journal Year: 2025, Volume and Issue: unknown, P. 162780 - 162780

Published: Feb. 1, 2025

Language: Английский

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Gallium-Promoted Strong Metal–Support Interaction over a Supported Cu/ZnO Catalyst for Methanol Steam Reforming

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(12), P. 9511 - 9520

Published: June 10, 2024

The strong metal–support interaction (SMSI), which involves the encapsulation of metal nanoparticles with support material to form an overlayer, affects interfacial structure and electronic characteristics supported metal, profoundly influencing its catalytic properties. However, developing facile approaches capable a achieving controllable, permeable, stable particularly under mild conditions, remains challenge. Here, we report that formation process ZnOx overlayer on Cu can be accelerated by addition promoter, aiming at strengthening SMSI effect. It is found introduction Ga promotes migration species onto surface metallic Cu0 after hydrogen reduction 300 °C atmospheric pressure. Such reconstruction forms more abundant Cu–ZnOx sites increases intrinsic activity 4.6-fold, as compared Cu/ZnO negligible SMSI, toward methanol steam reforming reaction. This investigation provides approach for rational design optimization catalysts deepens understanding concept SMSI.

Language: Английский

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Interface engineering of Ni and CeO2 catalysts for ethane dry reforming

International Journal of Hydrogen Energy, Journal Year: 2025, Volume and Issue: 103, P. 501 - 512

Published: Jan. 21, 2025

Language: Английский

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Atom-to-nm Scale Engineering of PtCo Alloy Catalysts over Supported Co Nanoparticles for Advanced Toluene Hydrogenation Efficiency in Hydrogen Storage Applications

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 3191 - 3202

Published: Feb. 7, 2025

Hydrogen storage and transportation are pivotal for a hydrogen- carbon-neutral society, yet current approaches face considerable limitations in efficiency cost, which typically related to catalyst design. Alloying trace amount of Pt on supported Co nanoparticles has emerged as an innovative design that leads substantial reduction the precious metal used catalytic hydrogenation toluene (TOL) methylcyclohexane (MCH), is important aspect hydrogen transportation. However, because difficulty controlling surface structure PtCo alloy catalysts, maximizes synergistic interaction between sites not been identified. In this study, we explore structure–function relationship TOL over catalysts by designing three distinct structures: single-atom alloys, nanoislands nanoparticles, support, i.e., monoclinic-phase ZrO2 (m-ZrO2). designs, m-ZrO2 was employed support control nanoparticle diameter 5–7 nm, maximizing fraction plane required efficient fixation/hydrogenation enhancing synergy with site-derived functionality. The highest turnover frequency (TOF) had following magnitude relationship: > m-ZrO2. Remarkably, enhanced utilization up 51-fold resulting record activity literature. Based kinetic experiments coupled in-depth structural analyses using series well-defined it clarified high attributed (1) optimal competitive adsorption H2 created single atoms-containing ensemble (2) large such sites. Stability tests microscopy confirmed catalysis remained stable at least 24 h, indicating also play crucial role preventing aggregation. Our findings underscore importance atom-to-nm scale achieving ultrafast even extremely low usage, offering approach saving

Language: Английский

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Oxygen Vacancies Promote Formaldehyde Base-Free Reforming into Hydrogen over Cu Doping-Induced Cu–Cu_xZn_1–xO Heterointerfaces

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 12, 2025

Element doping is a viable strategy to regulate the metal–support interface for enhancing catalytic performance of supported metal catalysts. Herein, Cu/ZnO:Cu-TH catalysts are prepared by immobilizing Cu nanoparticles (NPs) on ZnO nanorods featuring an adjustable oxygen vacancy, in which partial atoms at Cu–ZnO incorporated into lattice form CuxZn1–xO species. Such atom induces creation distinctive Cu–CuxZn1–xO sites and optimizes electron transfer from NPs, thereby achieving intermediate activation ultimately endowing catalyst with superior reforming alkali-free formaldehyde (HCHO) hydrogen low temperatures. The serve as pivotal centers HCHO reforming, where selectively engage cleavage C–H bonds O–H H2O, respectively. Meanwhile, presence vacancies bolsters adsorption further improving activity. Cu/ZnO:Cu-450H catalyst, distinguished abundant high concentration vacancies, demonstrates optimal activity TOF values 16.9 72.4 h–1 under anaerobic aerobic conditions, respectively, 8.9 29.0 times higher than those Cu/ZnO-450N lacks doped vacancies.

Language: Английский

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Size-dependent strong metal-support interaction modulation of Pt/CoFe2O4 catalysts

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Journal Year: 2025, Volume and Issue: 69, P. 292 - 302

Published: Feb. 1, 2025

Language: Английский

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Reconstructed rich oxygen defects and Ag0 on Pr6O11 surface through interface-defect engineering for enhanced electrochemical carbon dioxide reduction

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: unknown, P. 137368 - 137368

Published: March 1, 2025

Language: Английский

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Toward a molecular-scale picture of water electrolysis: mechanistic insights, fundamental kinetics and electrocatalyst dynamic evolution

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 536, P. 216651 - 216651

Published: April 6, 2025

Language: Английский

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Microenvironment‐Engineered Multilayered Electrode Design for Sustainable Seawater Oxidation

Small, Journal Year: 2025, Volume and Issue: unknown

Published: April 27, 2025

Abstract The reliance on high‐purity water for hydrogen production increases the strain freshwater resources. Direct seawater electrolysis is a promising alternative but impeded by complex challenges such as chloride‐induced corrosion and electrode surface fouling. Herein, microenvironment‐engineered, multilayered design sustainable presented, utilizing strategic integration of carbonate (CO₃ 2 ⁻) Lewis base sites anchored Cobalt layered double hydroxides (Co LDH) embedded within NiBO x nanostructure supported Ni(OH)₂/NF microarray. Incorporating boron into Ni‐OOH matrix forms protective metaborate film, preventing metal dissolution non‐conductive oxide formation, thereby enhancing current collector resistance in saline conditions. CO₃ ⁻ covalently functionalized Co‐active sites, establishes dynamic interaction that continuously splits molecules while sequestering H⁺ ions, generating localized acidic microenvironment. This acidification enhances OER kinetics protects against chloride attack precipitate addressing key stability efficiency barriers direct electrolysis. advanced anode achieves an industrially viable density 1.0 A cm⁻ at 1.65 V under standard conditions, marking significant step toward scalable, desalination‐free directly from seawater.

Language: Английский

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