Revealing the Active Sites in Atomically Dispersed Multi‐Metal–Nitrogen–Carbon Catalysts

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(29)

Published: Jan. 30, 2024

Abstract Atomically dispersed metal‐nitrogen‐carbon catalysts have been extensively explored for various sustainable energy‐related reactions. From a material perspective, these are likely to consist of combination single‐atom, dual‐atom and possibly even multi‐atom sites. However, pinpointing their true active sites has remained challenging task. In this study, model catalyst is introduced, Co/CoMn‐NC, featuring both Co single‐atom CoMn on nitrogen‐doped carbon substrate. By employing X‐ray adsorption spectroscopy density functional theory calculations, the atomic configuration Co/CoMn‐NC determined. Density calculations also used unequivocally identify Co‐atom within motif as predominate site toward oxygen reduction reaction (ORR), which further confirmed by in situ Raman spectroscopy. The cooperative interactions between can finely tune d‐band center ameliorate desorption behaviors intermediates, thereby facilitating ORR kinetic. Overall, study introduces systematic strategy elucidate structure superiority system provides new insights into atomically multi‐metal sites, showcasing that enhanced catalytic performance extends beyond unified diatomic or monatomic

Language: Английский

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Materials Containing Single‐, Di‐, Tri‐, and Multi‐Metal Atoms Bonded to C, N, S, P, B, and O Species as Advanced Catalysts for Energy, Sensor, and Biomedical Applications

Advanced Science, Journal Year: 2024, Volume and Issue: 11(33)

Published: July 1, 2024

Abstract Modifying the coordination or local environments of single‐, di‐, tri‐, and multi‐metal atom (SMA/DMA/TMA/MMA)‐based materials is one best strategies for increasing catalytic activities, selectivity, long‐term durability these materials. Advanced sheet supported by metal atom‐based have become a critical topic in fields renewable energy conversion systems, storage devices, sensors, biomedicine owing to maximum utilization efficiency, precisely located centers, specific electron configurations, unique reactivity, precise chemical tunability. Several offer excellent support are attractive applications energy, medical research, such as oxygen reduction, production, hydrogen generation, fuel selective detection, enzymatic reactions. The strong metal–metal metal–carbon with metal–heteroatom (i.e., N, S, P, B, O) bonds stabilize optimize electronic structures atoms due interfacial interactions, yielding activities. These provide models understanding fundamental problems multistep This review summarizes substrate structure‐activity relationship different active sites based on experimental theoretical data. Additionally, new synthesis procedures, physicochemical characterizations, biomedical discussed. Finally, remaining challenges developing efficient SMA/DMA/TMA/MMA‐based presented.

Language: Английский

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Interfacial interaction-induced shift of d-band center promotes photocatalytic antibiotics mineralization

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 352, P. 123998 - 123998

Published: April 21, 2024

Language: Английский

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Heteroatoms Modulate the Copper Single Atom Catalytic Host Materials for Promoting the Redox Reaction in Aqueous Zinc‐Selenium Batteries

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 18, 2024

Abstract Aqueous zinc‐selenium (Zn‐Se) batteries have garnered much attention due to their inherent safety and high specific capacity. Unfortunately, the problem of sluggish redox reaction represents a significant obstacle development aqueous Zn‐Se batteries. Here, nitrogen‐phosphorus asymmetrically coordinated copper single atom catalytic host material (CuN 3 P 1 @C) is synthesized for an battery. The CuN @C exhibits rich porous structure, high‐loading Cu atoms, unique asymmetric coordination environment, which significantly reduces energy barrier between Se Zn, enhancing electrochemical performance Consequently, Se/CuN cathode achieves capacity 756 mAh g −1 at 0.2 A cycling stability 4 000 cycles 5.0 (capacity decay 0.0044% per cycle). Meanwhile, conversion mechanism battery systematically explored via systematical characteristics density functional theory calculations. This work opens up novel approach boosting by modulating atom‐based materials heteroatoms.

Language: Английский

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Co‐Adjusting d‐Band Center of Fe to Accelerate Proton Coupling for Efficient Oxygen Electrocatalysis

Small, Journal Year: 2023, Volume and Issue: 20(20)

Published: Dec. 10, 2023

Abstract The problem in d‐band center modulation of transition metal‐based catalysts for the rate‐determining steps oxygen conversion is an obstacle to boost electrocatalytic activity by accelerating proton coupling. Herein, Co doping FeP adopted modify Fe. Optimized Fe sites accelerate coupling reduction reaction (ORR) on N‐doped wood‐derived carbon through promoting water dissociation. In situ generated optimize adsorption oxygen‐related intermediates evolution (OER) CoFeP NPs. Superior catalytic toward ORR (half‐wave potential 0.88 V) and OER (overpotential 300 mV at 10 mA cm −2 ) express unprecedented level carbon‐based metal‐phosphide catalysts. liquid zinc–air battery presents outstanding cycling stability 800 h (2400 cycles). This research offers a newfangled perception designing highly efficient bifunctional OER.

Language: Английский

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Structural engineering of metal oxyhydroxide for electrochemical energy conversion and storage

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 513, P. 215880 - 215880

Published: April 30, 2024

Language: Английский

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Single-Atom Ni Sites with Asymmetric Coordination Structures for Efficient Photocatalytic CO₂ Reduction

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 20, 2025

The exploration of single-atom catalysts (SACs) with unique coordination structures is vital importance for boosting photocatalytic CO2 reduction, yet it remains challenging. Herein, we develop a novel SAC asymmetric structure the Ni catalytic site, which can trap photogenerated electrons to realize highly efficient reduction in presence triethanolamine as an electron donor. Doping B heteroatom into N-doped carbon substrate would introduce B–N bond and meanwhile create defects, thus providing feasible strategy break symmetry Ni–N4 moiety finally producing unsaturated Ni–N3–B structure. It demonstrated that species improve trapping ability reduce formation energy barrier *COOH intermediate compared symmetric reduction. Such concept breaking SACs could provide promising approach constructing effective sites toward solar energy-driven conversion.

Language: Английский

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Ni/Fe2O3 Mott-Schottky heterointerface engineering and phosphate doping synergistically refining d-band center for efficient oxygen evolution reaction

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 479, P. 147723 - 147723

Published: Nov. 30, 2023

Language: Английский

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Fe based MOF encapsulating triethylenediamine cobalt complex to prepare a FeN3-CoN3 dual-atom catalyst for efficient ORR in Zn-air batteries

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 676, P. 871 - 883

Published: July 23, 2024

Language: Английский

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Manipulation of Electronic States of Pt Sites via d-Band Center Tuning for Enhanced Oxygen Reduction Reaction in Proton Exchange Membrane Fuel Cells

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(4), P. 2138 - 2147

Published: Jan. 18, 2024

Expediting the torpid kinetics of oxygen reduction reaction (ORR) at cathode with minimal amounts Pt under acidic conditions plays a significant role in development proton exchange membrane fuel cells (PEMFCs). Herein, novel Pt–N–C system consisting single atoms and nanoparticles anchored onto defective carbon nanofibers is proposed as highly active ORR catalyst (denoted Pt–N–C). Detailed characterizations together theoretical simulations illustrate that strong coupling effect between different sites can enrich electron density sites, modify d-band electronic environments, optimize intermediate adsorption energies, ultimately leading to significantly enhanced performance. Specifically, as-designed demonstrates exceptional properties high half-wave potential 0.84 V. Moreover, mass activity reaches 193.8 mA gPt–1 0.9 V versus RHE, which 8-fold greater than Pt/C, highlighting enormously improved electrochemical properties. More impressively, when integrated into electrode assembly an air-fed PEMFC, achieved higher maximum power (655.1 mW cm–2) compared Pt/C-based batteries (376.25 cm–2), hinting practical application PEMFCs.

Language: Английский

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