Dual defect regulation of BiOCl halogen layer enables photocatalytic O2 activation into singlet oxygen for refractory aromatic pollutant removal

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 345, P. 123689 - 123689

Published: Jan. 3, 2024

The generation of singlet oxygen (1O2) based on photocatalytic activation O2 is considered to have important application prospects in purifying refractory organic pollutants water. However, the uncertain dual pathway transformation activated severely limits 1O2. In this work, we show a robust BiOCl with defects (adjacent I-substitution defect and Cl vacancy) halogen layer for selective generate Combining experiments theoretical calculations, confirm that are beneficial optimizing band structures, improving carrier separation efficiency, promoting adsorption activation. More importantly, it confirmed can directionally convert into 1O2 by increasing thermodynamic conversion energy barrier non-1O2 pathways serving as necessary site functions oxidation reduction. Applying modified removal aromatic water, found has efficient stable degradation efficiency broad environmental adaptability. This work not only provides in-depth insights mechanism produce 1O2, but also lays foundation further development highly active photocatalysts remediation conversion.

Language: Английский

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Asymmetric Atomic Dual‐Sites for Photocatalytic CO₂ Reduction

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(38)

Published: July 23, 2024

Abstract Atomically dispersed active sites in a photocatalyst offer unique advantages such as locally tuned electronic structures, quantum size effects, and maximum utilization of atomic species. Among these, asymmetric dual‐sites are particular interest because their charge distribution generates local built‐in electric potential to enhance separation transfer. Moreover, the dual provide flexibility for tuning complex multielectron multireaction pathways, CO 2 reduction reactions. The coordination opens new possibilities engineering structure–activity–selectivity relationship. This comprehensive overview discusses efficient sustainable photocatalysis processes photocatalytic reduction, focusing on strategic active‐site design future challenges. It serves timely reference development conversion processes, specifically exploring here exemplified by into valuable chemicals.

Language: Английский

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Engineering low-coordination atoms on RhPt bimetallene for 12-electron ethanol electrooxidation

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(6), P. 2219 - 2227

Published: Jan. 1, 2024

The three-dimensional perforated RhPt bimetallene achieves a high exposure ratio of low-coordinated diatomic sites, demonstrating excellent activity and remarkable selectivity for 12-electron ethanol oxidation to CO 2 .

Language: Английский

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An oxygen-coordinated cobalt single-atom electrocatalyst boosting urea and urea peroxide production

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(5), P. 1950 - 1960

Published: Jan. 1, 2024

An oxygen-coordinated cobalt single-atom catalyst was successfully fabricated, exhibiting exceptional electrocatalytic activity toward urea and H 2 O production. Subsequently, the value-added peroxide efficiently synthesized.

Language: Английский

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Bifunctional Pt dual atoms for overall water splitting

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 355, P. 124214 - 124214

Published: May 18, 2024

Language: Английский

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Cascade Synthesis of Fe‐N2‐Fe Dual‐Atom Catalysts for Superior Oxygen Catalysis

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: July 3, 2024

Dual-atom catalysts (DACs) have been proposed to break the limitation of single-atom (SACs) in synergistic activation multiple molecules and intermediates, offering an additional degree freedom for catalytic regulation. However, it remains a challenge synthesize DACs with high uniformity, atomic accuracy, satisfactory loadings. Herein, we report facile cascade synthetic strategy DAC via precise electrostatic interaction control neighboring vacancy construction. We synthesized well-defined, uniformly dispersed dual Fe sites which were connected by two nitrogen bonds (denoted as Fe-N

Language: Английский

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Leveraging Dual‐Atom Catalysts for Electrocatalysis Revitalization: Exploring the Structure‐Performance Correlation

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(18)

Published: Feb. 27, 2024

Abstract In light of the profound shift toward renewable fuels, dual‐atom catalysts (DACs) are impressively prospected as auspicious for electrocatalysis revitalization, accomplishing environmental remediation and sustainable global energy security. Leveraging appealing attributes such inspiring synergistic effect, additional adjacent adsorption sites, ultrahigh atom utilization, DACs endowed with unprecedented stability, activity, selectivity in multifarious energy‐related applications. By virtue addressing time technological prominence to review this ground‐breaking atomic electrocatalyst, first encompasses a correlation elucidation between substrate, dual‐atoms, facile synthetic approaches intriguing modification strategies. Furthermore, state‐of‐the‐art characterization techniques specially employed spotlighted, alongside rigorously unveiling novel mechanistic insights’ milestone gained from both theoretical modeling experimental research multitudes environmentally benign electrocatalytic applications, including O 2 reduction, CO H evolution, N other fundamental reactions. As final note, presents brief conclusion highlighting current challenges outlining prospects frontier. Importantly, deciphers structure‐performance while excavating advancement DACs, thus is anticipated shed catalysis community on bolstering an intense evolution triggering sapient inspiration more robust next‐generation catalysts.

Language: Английский

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Site-designed dual-active-center catalysts for co-catalysis in advanced oxidation processes

npj Materials Sustainability, Journal Year: 2025, Volume and Issue: 3(1)

Published: Jan. 7, 2025

Abstract Advanced Oxidation Processes (AOPs) are promising for treating persistent pollutants, yet challenges arise due to the step-wise oxidants activation process, which traditional single-active-center catalysts struggle facilitate effectively. Recently, dual-active-center have emerged as a solution by enabling synergistic reactions. This review covers advances in these catalysts, their co-catalytic mechanisms, and applications electro-Fenton, photocatalytic, peroxymonosulfate-, pollutant-as-electron-donor based Fenton-like processes, along with active site design considerations future challenges.

Language: Английский

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Precisely designing asymmetrical selenium-based dual-atom sites for efficient oxygen reduction

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Jan. 7, 2025

Owing to their synergistic interactions, dual-atom catalysts (DACs) with well-defined active sites are attracting increasing attention. However, more experimental research and theoretical investigations needed further construct explicit understand the synergy that facilitates multistep catalytic reactions. Herein, we precisely design a series of asymmetric selenium-based comprise heteronuclear SeN2–MN2 (M = Fe, Mn, Co, Ni, Cu, Mo, etc.) for efficient oxygen reduction reaction (ORR). Spectroscopic characterisation calculations revealed selenium atoms can efficiently polarise charge distribution other metal through short-range regulation. In addition, compared Se or Fe single-atom sites, SeFe facilitate in conversion energy barrier from *O *OH via coadsorption intermediates. Among these designed catalysts, selenium-iron achieves superior alkaline ORR performance, half-wave potential 0.926 V vs. reversible hydrogen electrode. SeN2–FeN2-based Zn–air battery has high specific capacity (764.8 mAh g−1) maximum power density (287.2 mW cm−2). This work may provide good perspective designing DACs improve efficiency. Dual-atom precise gaining attention, but studies optimise construction synergy. Here authors report dual- atom reaction.

Language: Английский

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UV‐Induced Synthesis of Graphene Supported Iridium Catalyst with Multiple Active Sites for Overall Water Splitting

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(22)

Published: Feb. 7, 2024

Abstract Catalysts that can promote the hydrogen evolution reaction (HER) and oxygen (OER) are in demand for efficient water splitting. Here, a general practical UV‐induced synthesis of noble metal catalysts supported on reduced electrochemical graphene oxide (M‐rEGO, M = Ir, Pt or Pd) is proposed. The use EGO with low degree oxidation generation highly reducing isopropanol radical from added acetone crucial this one‐step, one‐pot synthesis. Using Ir as model material, vacancies rEGO allow interaction undercoordinated C forming multiple active species including single atoms (SAs), dual‐atom pairs (DAs) nanoparticles. This Ir‐rEGO catalyst exhibits overpotentials only 42.3 294 mV to reach 10 mA cm −2 0.5 м H 2 SO 4 HER 1 KOH OER, respectively, at an extremely loading (2.1 wt%). water‐splitting cells featuring outperform those using commercial Pt/C (20 wt%) RuO both acidic alkaline electrolytes. Density functional theory calculations confirm stabilization SAs DAs lattice well high activity OER.

Language: Английский

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