Distribution of Oxygen Vacancies in RuO2 Catalysts and Their Roles in Activity and Stability in Acidic Oxygen Evolution Reaction DOI
Zhe Shang, Hui Li

The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: unknown, P. 5418 - 5428

Published: May 22, 2025

By combining density functional theory (DFT) calculations and the cluster expansion (CE) model in an active-learning framework, we comprehensively studied distribution features of oxygen vacancies (OV's) as well their contributions to stability activity RuO2 catalyst acidic evolution reaction (OER). The results show that OV's prefer be located at bridge sites on RuO2(110) surface next-nearest-neighbor trans positions RuO6 octahedra pairs due interactions between two OV's, high concentrations exhibit a continuous zigzag (110) plane RuO2. vacancy can explained by charge repulsion low-valent Ru O, which is referred "heterovalent ion-oxygen exclusion principle". In addition, DFT presence cannot improve inherent OER specific since hinder deprotonation second water molecule. Nevertheless, suppressing lattice mechanism (LOM) path. summary, this work provides deeper insights into with media possible way performance using engineering.

Language: Английский

Ru Single Atoms Anchored on Co3O4 Nanorods for Efficient Overall Water Splitting under pH‐Universal Conditions DOI Creative Commons

Yongfang Zhou,

Yu Mao, Cuizhu Ye

et al.

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 2, 2025

Abstract Single‐atom catalysts (SACs) show great promise for electrocatalytic water splitting due to their exceptional metal atom utilization efficiency. Herein, it is demonstrated that Ru single atoms (SAs) anchored on Co 3 O 4 nanorod arrays (Ru x ‐Co , where the loading in weight percent) afford outstanding performance and durability oxygen evolution reaction (OER), hydrogen (HER), overall across a wide pH range (0.3–14). 8% achieves 10 mA cm⁻ 2 at overpotentials of only 214, 286, 138 mV OER, 13, 72, 59 HER, 1 m KOH, 0.1 PBS, 0.5 H SO respectively, outperforming benchmark RuO Pt/C catalysts. When utilized as anode cathode an anion exchange membrane electrolyzer (AEMWE), cell voltage 2.06 V required achieve A . Chronopotentiometry verified possesses excellent stability during both OER HER 100 acidic, neutral, alkaline media. Density functional theory (DFT) calculations reveal abundant Ru‐O‐Co interfaces shift d‐band center from −1.72 eV (for cluster/Co ) −1.58 SA/Co ), creating more energetically favorable pathways HER.

Language: Английский

Citations

2
Molecular Anodes for Electrocatalytic Water Oxidation Based on Self-Assembled Bilayers Driven by Electron Transfer Mediators DOI
Paula Tris-Marzo, Daniele Veclani, Alessandro Venturini

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: April 8, 2025

The generation of solar fuels via water splitting with sunlight requires, among others, robust and efficient electrodes for the oxidation reaction. For this purpose, combination powerful molecular catalysts graphitic materials has been shown to work outstandingly well. However, in oxide-based materials, that are enormous importance as conductive or semiconductive either do not transformed into corresponding oxides. Here, we use a supramolecular strategy based on self-assembled bilayers where silanolate long alkyl chains is bonded electrode surface acts platform supramolecularly interact multiple attached catalyst. In manner, catalyst electrolyte assembly isolated from oxide surface, conferring great stability, but at same time, they sufficiently close so electron transfer can take place electrode. Our best hybrid anode works efficiently pH 7 without practically any activity losses, current densities 0.40 mA/cm2 15 h, giving more than 33,800 TONs Faradaic efficiency over 92% while maintaining intact its nature. This provides successful proof concept benefit properly combining obtain both worlds.

Language: Английский

Citations

1
Enhancing the Activity and Stability of Pt Nanoparticles Supported on Multiscale Porous Antimony Tin Oxide for Oxygen Reduction Reaction DOI
Li Hao, Muhammad Ajmal, Xinquan Wu

et al.

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

Published: April 8, 2025

Abstract Pt nanoparticles dispersed on carbon supports (Pt/C) are the benchmark oxygen reduction reaction (ORR) catalysts in proton exchange membrane fuel cells (PEMFCs). However, their widespread application is hindered by severe stability degradation under high potentials and acidic environments, primarily due to support corrosion. To address this challenge, a multiscale template‐assisted method proposed, combined with ethylene glycol reduction, fabricate supported onto porous conductive antimony tin oxides (Pt/PT‐SSO). Both theoretical experimental approaches have shown that strong interaction between markedly accelerates electron transfer optimizes adsorption strength of key intermediates surface. Furthermore, unique structure not only provides an ideal platform for uniform dispersion but also greatly enhances confinement effect, effectively preventing aggregation. As result, Pt/PT‐SSO exhibits superior ORR activity durability compared commercial Pt/C catalysts. Specifically, its mass at 0.9 V (vs RHE) reaches 0.617 A mgPt⁻¹, which twice Pt/C, while maintaining outstanding over 50 h. Notably, PEMFCs utilizing achieve power density 1.173 W cm⁻ 2 retain 94.9% after 30,000 cycles accelerated testing.

Language: Английский

Citations

0
Recent Advances of Ruthenium‐Based Electrocatalysts for Industrial Water Electrolyzers DOI
Wentao Zhou,

Chen Gu,

Lingbin Xie

et al.

Advanced Sustainable Systems, Journal Year: 2025, Volume and Issue: unknown

Published: April 10, 2025

Abstract Hydrogen production by electrochemical water splitting is considered to be a key strategic energy technology, and proton exchange membrane electrolyzers (PEMWEs) anion (AEMWEs) are ideal technologies for green hydrogen in recent years. However, PEMWEs AEMWEs lack low‐cost high‐performance acidic oxygen evolution reaction (OER) alkaline (HER) electrocatalysts respectively, limiting their large‐scale development. Recently, ruthenium (Ru)‐based have received lot of attention because activity better than that commercial catalysts price more affordable, showing great potential OER HER. there still obstacles Ru‐based practical applications industrial electrolyzers, regulatory strategies need developed further optimize its performance. Herein, comprehensive review presented concerning it. First, fundamental principles focus the basic content application discussed. Then, summarized, providing detailed analysis elucidate mechanisms, properties, electrolyzers. Finally, outlooks prospects challenges future proposed.

Language: Английский

Citations

0
Hollow RuO2 Fibers with B-Modification for Enhanced Water Oxidation Electrocatalysis in Both Acidic and Alkaline Media DOI
Zelun Zhi, Xiaokun Fan, Xing Tian

et al.

Composites Communications, Journal Year: 2025, Volume and Issue: unknown, P. 102452 - 102452

Published: May 1, 2025

Language: Английский

Citations

0
Single-Atom Ru-Triggered Lattice Oxygen Redox Mechanism for Enhanced Acidic Water Oxidation DOI
Menghui Qi,

Xiangbowen Du,

Xiaoyun Shi

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: May 15, 2025

Activating the oxygen anionic redox presents a promising avenue for developing highly active evolution reaction (OER) electrocatalysts proton-exchange membrane water electrolyzers (PEMWE). Here, we engineered lattice-confined Ru single atom dispersed on lamellar manganese oxide (MnO2) cation site. The strong Ru-O bond induced an upward shift in O 2p band, enhancing metal-oxygen covalency and reshaping OER mechanism toward lattice oxidation pathway with increased activity. In situ spectral characterization combined density functional theory (DFT) calculations revealed that electron transfer from Mn to alleviates Jahn-Teller effect within MnO6 octahedral structure, stabilizing lattice. layered Ru/MnO2 architecture also promotes rapid replenishment of vacancies, preventing structural collapse. As result, optimized electrocatalyst achieves overpotential only 179 mV at 10 mA cm-2 0.5 M H2SO4, along exceptional durability over 1000 h 100 cm-2. Moreover, Ru/MnO2-based PEM device requires 1.71 V reach 1 A shows 500

Language: Английский

Citations

0
Recent progress in Ru electrocatalyst design for acidic oxygen evolution reaction DOI
Yingde Cui, Yan Zhao, Zhen Han

et al.

Journal of Materials Chemistry A, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

This review surveys recent advances in Ru-based electrocatalysts for the acidic OER, focusing on strategies to enhance activity and stability, mitigate Ru dissolution performance degradation, inform design of robust PEMWE.

Language: Английский

Citations

0
Distribution of Oxygen Vacancies in RuO2 Catalysts and Their Roles in Activity and Stability in Acidic Oxygen Evolution Reaction DOI
Zhe Shang, Hui Li

The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: unknown, P. 5418 - 5428

Published: May 22, 2025

By combining density functional theory (DFT) calculations and the cluster expansion (CE) model in an active-learning framework, we comprehensively studied distribution features of oxygen vacancies (OV's) as well their contributions to stability activity RuO2 catalyst acidic evolution reaction (OER). The results show that OV's prefer be located at bridge sites on RuO2(110) surface next-nearest-neighbor trans positions RuO6 octahedra pairs due interactions between two OV's, high concentrations exhibit a continuous zigzag (110) plane RuO2. vacancy can explained by charge repulsion low-valent Ru O, which is referred "heterovalent ion-oxygen exclusion principle". In addition, DFT presence cannot improve inherent OER specific since hinder deprotonation second water molecule. Nevertheless, suppressing lattice mechanism (LOM) path. summary, this work provides deeper insights into with media possible way performance using engineering.

Language: Английский

Citations

0