Vacancy Engineering in the First Coordination Shell of Single‐Atom Catalysts for Enhanced Hydrogen and Oxygen Evolution Reactions

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

Published: March 10, 2025

Abstract Modulating the coordination environment of active centers has been proven to be an effective strategy for tuning activity and selectivity single‐atom catalysts (SACs). However, most current research primarily focuses on altering non‐metallic elements coordinating with single metal atom. In this study, a novel approach is presented by introducing various vacancies into first shell doped boron–carbon–nitride (BCN) catalysts, systematically evaluating their hydrogen evolution (HER) oxygen (OER) reactions performances. Results indicate that introduction vacancy defects enhances stability M‐B X C Y N Z structures. Furthermore, adjusting atoms around sites modulates charge distribution, influencing binding propensity intermediates adsorption promoting synergistic effects between nonmetal, thereby catalytic activity. Specifically, among 147 ‐vacancy structures, 17 excellent HER performance have identified. Notably, C‐vacancy modulated Ni‐BC 2 exhibits OER overpotential only 0.36V, suggesting N‐C1 may serve as efficient multifunctional electrocatalyst water‐splitting reactions. This work employs engineering precisely modulate not screening out HER/OER electrocatalysts but also providing guidance development potential BCN‐based electrocatalysts.

Language: Английский

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Engineering Multi‐Site Platinum Ensembles Synergistically Boosts Catalysis

Advanced Science, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 18, 2025

Abstract Engineering stable and efficient noble metal ensembles with multi‐type active sites while understanding the role of each site at atomic level remains a significant challenge in heterogeneous catalysis. Herein, sub‐nanometric Pt ensemble catalyst diverse array is constructed via dual‐confinement strategy, which exhibits superior activity durability minimal loading (0.13 wt.%). Simultaneously, roles different scale are determined through situ characterization methods density functional theory (DFT) calculations. Specifically, top predominantly serve as pivotal centers for O═O bond activation, whereas Pt−O−Si interfacial primarily govern activation H─OH C─H bonds. The reactive oxygen species (O 2 − , O 2− −OH) generated from H synergistically enhance formaldehyde (HCHO) oxidation shorten reaction pathway. This study sheds light on better rational design precise synthesis multi‐site or discerning distinct contributions various catalytic sites.

Language: Английский

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Cerium Oxide‐Induced Synchronous Lattice Oxygen Activation and Accelerated Deprotonation Kinetics in Cobalt (oxy)Hydroxide for Robust Water Oxidation

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

Published: Feb. 19, 2025

Abstract Theoretically, triggering the lattice oxygen mechanism (LOM) of catalysts during alkaline evolution reaction (OER) can effectively break through thermodynamic limitations, while following this path, rate simultaneous deprotonation also determines overall kinetics. A cerium oxide units‐modified cobalt (oxy)hydroxide nanocomposite CeO 2 ‐CoOOH/NF is proposed, where Ce(4f)‐O(2p)‐Co (3d) coupling with sites interaction mediates Co─O Mott–Hubbard splitting state to trigger efficient LOM. Meanwhile, 4f orbital electron‐rich near Fermi level favorable for proceeding electron‐involved behavior. All these empower considerable OER activity, which delivers an overpotential 249 mV at 10 mA cm −2 , and commercial Pt/C in anion exchange membrane water electrolyze (AEMWE) realize energy‐saving hydrogen production. This work instructive design high‐performance controlling electron orbitals hybridization synchronously accelerate kinetics each link OER.

Language: Английский

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Reductive Supramolecular In Situ Construction of Nano‐Platinum Effectively Couples Cathodic Hydrogen Evolution and Anodic Alcohol Oxidation

Advanced Science, Journal Year: 2025, Volume and Issue: unknown

Published: April 3, 2025

The deployment of high-performance catalysts and the acceleration anodic reaction kinetics are key measures to achieve maximum energy efficiency in overall water electrolysis hydrogen production systems. Here, an innovative strategy is developed by directly constructing a supramolecular framework embedded with boron clusters cucurbituril as reducing agent. This approach enabled situ conversion Pt⁴⁺ into highly dispersed, small-sized nano-platinum, which subsequently distributed on boron-carbon-nitrogen (BCN) matrix. resulting Pt/BNHCSs catalyst demonstrates ability facilitate electrocatalytic splitting for across multiple scenarios while simultaneously accelerating methanol oxidation kinetics, significantly outperforming commercial Pt/C various aspects. cathodic evolution-anodic coupling system constructed using greatly reduces consumption system. In attenuated total reflection Fourier transform infrared online differential electrochemical mass spectrometry reveals that interface enhances H₂O adsorption promotes CH₃OH→CO process, density functional theory calculations indicated BCN support facilitated evolution H₂ CH₃OH CO, elucidating mechanism promoted oxidation.

Language: Английский

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Cobalt Nanoclusters-Modulated Platinum–Tin Intermetallic for pH-Universal Hydrogen Evolution Electrocatalysis

ACS Materials Letters, Journal Year: 2025, Volume and Issue: unknown, P. 1760 - 1767

Published: April 7, 2025

Language: Английский

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A Synergistic Advancement of rGO-supported perovskite oxide composite for sustainable energy system

Journal of the Indian Chemical Society, Journal Year: 2025, Volume and Issue: unknown, P. 101757 - 101757

Published: May 1, 2025

Language: Английский

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