From Single-Atom to Dual-Atom: A Universal Principle for the Rational Design of Heterogeneous Fenton-like Catalysts

Environmental Science & Technology, Год журнала: 2025, Номер unknown

Опубликована: Апрель 22, 2025

Developing efficient heterogeneous Fenton-like catalysts is the key point to accelerating removal of organic micropollutants in advanced oxidation process. However, a general principle guiding reasonable design highly has not been constructed up now. In this work, total 16 single-atom and 272 dual-atom transition metal/nitrogen/carbon (TM/N/C) for H2O2 dissociation were explored systematically based on high-throughput density functional theory machine learning. It was found that TM/N/C exhibited distinct volcano-type relationship between catalytic activity •OH adsorption energy. The favorable energies range -3.11 ∼ -2.20 eV. Three different descriptors, namely, energetic, electronic, structural found, which can correlate intrinsic properties their activity. Using energy, stability, activation energy as evaluation criteria, two CoCu/N/C CoRu/N/C screened out from candidates, higher than best catalyst due synergistic effect. This work could present conceptually novel understanding inspire structure-oriented viewpoint volcano relationship.

Язык: Английский

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A Revised High‐Throughput Screening Model on Oxygen Reduction Reaction Over Dual Atom Catalysts Based on the Axial Pre‐Adsorption and O₂ Adsorption

Advanced Energy Materials, Год журнала: 2024, Номер unknown

Опубликована: Окт. 16, 2024

Abstract Dual‐atom catalysts (DACs) often exhibit superior electrocatalytic activity, due to their versatile combinations and synergistic effects. However, the neglect of both dynamic axial adsorption active site upon working potential reactant as a rate‐determining step hinders establishment an accurate high‐throughput screening strategy. Here, oxygen reduction reaction (ORR) 42 kinds 3d–3d metal DACs by density functional theory (DFT) calculations are systematiclly investigated demonstrated that ORR kinetics can be limited O 2 * besides proton–electron transfer center may reconstructed pre‐adsorption intermediates under potential. Therefore, volcano plot is proposed using OH* activity descriptors. Then, method constructed 38 promising screened out from 267 containing 3d, 4d, or 5d metals. Importantly, previously unexplored MnCoN 6 DAC also experimentally synthesized, exhibits ultrahigh outperforming Pt/C, perfectly matching with theoretical prediction. In short, this work not only proposes plot‐based but provides proof‐of‐concept experimental verification prediction heuristically design electrocatalysts for other reactions.

Язык: Английский

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Wrinkled Graphene Nanoscroll-Fibers as a Support Platform to Encapsulate the CrFe-Codoped Cobalt Nanoparticles for Robust Zn–Air Batteries

Advanced Fiber Materials, Год журнала: 2025, Номер unknown

Опубликована: Апрель 1, 2025

Язык: Английский

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Single‐Atom Sb‐Doped RuSbO_x Bifunctional Catalysts for Ultra‐Stable PEM Water Electrolyzers

Small, Год журнала: 2025, Номер unknown

Опубликована: Апрель 17, 2025

Abstract Developing highly efficient and stable Pt/Ir‐free bifunctional catalysts is very urgent for lowering the catalyst cost of proton exchange membrane water electrolyzer (PEMWE). Herein, a single‐atom Sb‐doped RuSbO x developed ultra‐stable PEMWE. exhibits excellent stability with long‐term operation 150 h oxygen evolution reaction (OER) 300 hydrogen (HER) at 100 mA cm −2 in acidic media, respectively. Impressively, PEMWE as only needs 1.72 to reach 1.0 A , can maintain 200 . The situ Raman molecular probe methods reveal that Sb doping reconstruct interfacial structure on surface resulting an enriched supply free water, accelerating deprotonation process reducing local acidity surface, thereby improving OER activity stability. Density functional theory calculations further confirm above experimental results. In short, this work reveals outstanding structural stabilizer, Sb‐doping maximize Ru‐based acid, which provides useful strategy designing electrocatalysts

Язык: Английский

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Asymmetric Atomic Pt–B Dual-Site Catalyst for Efficient Photoreforming of Waste Polylactic Acid Plastics in Seawater

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Апрель 18, 2025

Waste plastic has imposed significant burdens on marine ecosystems. Converting into high-value products via photocatalysis is an emerging and promising approach, but its low activity product selectivity pose great challenges. Herein, we report a carbon nitride-anchored atomically dispersed Pt-B dual-site catalyst (Pt SA/BCN100) for the photoreforming of polylactic acid (PLA) chemicals H2 in seawater. Experiments DFT calculations reveal that significantly enhanced charge transfer occurs between Pt site B site, hole-rich can selectively trigger activation cleavage C-H C-C bonds PLA to form acetic (AA), while electron-rich drives reduction H protons H2. As result, SA/BCN100 exhibits high evolution rate 993 μmol gcatal-1 h-1 AA production 300 with over 98%. We also demonstrate direct g-scale real-world wastes concentrations microplastics natural Techno-economic analysis environmental assessment show this catalytic system reduce emissions potential commercial value.

Язык: Английский

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Potential‐Driven Dynamic Spring‐Effect of Pd─Cu Dual‐Atoms Empowered Stability and Activity for Electrocatalytic Reduction

Advanced Science, Год журнала: 2025, Номер unknown

Опубликована: Апрель 26, 2025

Abstract Atomic‐level catalysts are extensively applied in heterogeneous catalysis fields. However, it is a general but ineluctable issue that active metal atoms may migrate, aggregate, deactivate, or leach during reaction processes, suppressing their catalytic performances. Designing superior intrinsic‐structural stability of atomic‐level with high activity and revealing dynamic structure evolution vital for wide applications complex reactions harsh conditions. Herein, high‐stable Pd─Cu dual‐atom PdN 3 ─CuN coordination engineered via strong chelation Cu 2+ ‐ions electron pairs from palladium‐source, achieving the highest turnover frequency under lowest overpotential Cr(VI) electrocatalytic reduction detection strong‐acid electrolytes. In situ X‐ray absorption fine spectra reveal “spring‐effect” Cu─Pd Cu─N bonds reversibly stretched potential changes can be recovered at 0.6 V regeneration. The modulated electron‐orbit coupling effect prevents Cu‐atoms aggregating as metallic nanoparticles. dual‐atoms interact two O H 2 CrO 4 , forming stable bridge configurations transferring electrons to promote Cr─O bond dissociation, which prominently decreases energy barriers. This work provides feasible route boost robustness single‐atoms easily affected by conditions sustainable applications.

Язык: Английский

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Engineering Local Coordination and Electronic Structures of Dual-Atom Catalysts

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Май 1, 2025

Heterogeneous dual-atom catalysts (DACs), defined by atomically precise and isolated metal pairs on solid supports, have garnered significant interest in advancing catalytic processes technologies aimed at achieving sustainable energy chemical production. DACs present board opportunities for atomic-level structural property engineering to enhance performance, which can effectively address the limitations of single-atom catalysts, including restricted active sites, spatial constraints, typically positive charge nature supported single species. Despite rapid progress this field, intricate relationship between local atomic environments behavior dual-metal sites remains insufficiently understood. This review highlights recent major challenges field. We begin discussing modulation coordination electronic structures its impact performance. Through specific case studies, we demonstrate importance optimizing entire ensemble achieve efficient, selective, stable performance both model industrially relevant reactions. Additionally, also outline future research directions, emphasizing synthesis, characterization, practical applications, aiming fully unlock potential these advanced catalysts.

Язык: Английский

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High-Efficiency Electrochemical Ammonia Synthesis at Co-Catalytic Fe–Mo Dual-Atom Sites

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Май 5, 2025

To tackle the challenge in electrochemical nitrogen fixing and reduction aqueous electrolytes, conventional approach has been to suppress competitive hydrogen evolution reaction. Nonetheless, proton provision is a crucial step pathway produce ammonia, single active site faces daunting task striking balance between high fixation efficiency fast protonation kinetics. This work presents harmonic strategy featuring atomically dispersed dual Fe-Mo sites anchored an N-doped carbon (FeMoNC) substrate, where low-spin Fe center with enriched empty d orbitals aids activation, adjacent Mo accelerates kinetics of N-containing intermediates at via distal associative mechanism. Driven by this co-catalytic mechanism, FeMoNC catalyst achieves Faradaic 37.42%, marking significant improvement 7.8- 10.6-fold over or single-atom catalysts, respectively. Furthermore, excellent NH3 yield 54.40 μg h-1 mgcat.-1 realized flow cell enhancing mass transfer. study provides valuable insights into diatomic mechanisms for ammonia synthesis.

Язык: Английский

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Asymmetric Charge Distribution in Atomically Precise Metal Nanoclusters for Boosted CO2 Reduction Catalysis

ChemSusChem, Год журнала: 2024, Номер unknown

Опубликована: Окт. 30, 2024

Recently, atomically precise metal nanoclusters (NCs) have been widely applied in CO

Язык: Английский

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