Direct Dioxygen Radical Coupling Driven by Octahedral Ruthenium–Oxygen–Cobalt Collaborative Coordination for Acidic Oxygen Evolution Reaction

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(32), P. 17995 - 18006

Published: Aug. 7, 2023

The acidic oxygen evolution reaction (OER) has long been the bottleneck of proton exchange membrane water electrolyzers given its harsh oxidative and corrosive environments. Herein, we suggest an effective strategy to greatly enhance both OER activity stability Co3O4 spinel by atomic Ru selective substitution on octahedral Co sites. resulting highly symmetrical Ru-O-Co collaborative coordination with strong electron coupling effect enables direct dioxygen radical pathway. Indeed, experiments theoretical calculations reveal a thermodynamically breakthrough heterogeneous diatomic mechanism. Additionally, active units are well-maintained upon thanks transfer from surrounding electron-enriched tetrahedral atoms via bridging bonds that suppresses overoxidation thus dissolution species. Consequently, prepared catalyst, even low mass loading ca. 42.8 μg cm-2, exhibits attractive performance overpotential 200 mV potential decay rate 0.45 h-1 at 10 mA cm-2. Our work suggests significantly low-cost electrocatalysts.

Language: Английский

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Deficiency and surface engineering boosting electronic and ionic kinetics in NH4V4O10 for high-performance aqueous zinc-ion battery

Energy storage materials, Journal Year: 2021, Volume and Issue: 44, P. 197 - 205

Published: Oct. 2, 2021

Language: Английский

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Electrocatalysts for the Oxygen Evolution Reaction in Acidic Media

Advanced Materials, Journal Year: 2022, Volume and Issue: 35(22)

Published: Dec. 15, 2022

Abstract The well‐established proton exchange membrane (PEM)‐based water electrolysis, which operates under acidic conditions, possesses many advantages compared to alkaline such as compact design, higher voltage efficiency, and gas purity. However, PEM‐based electrolysis is hampered by the low instability, high cost of anodic electrocatalysts for oxygen evolution reaction (OER). In this review, recently reported OER are comprehensively summarized, classified, discussed. related fundamental studies on mechanisms relationship between activity stability particularly highlighted in order provide an atomistic‐level understanding catalysis. A test protocol suggested evaluate intrinsic degradation. Some current challenges unresolved questions, usage carbon‐based materials differences electrocatalyst performances electrolytes electrolyzers also Finally, suggestions most promising a perspective future research outlined. This review presents fresh impetus guideline rational design synthesis high‐performance electrolysis.

Language: Английский

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Marriage of Ultralow Platinum and Single-Atom MnN₄ Moiety for Augmented ORR and HER Catalysis

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(6), P. 4012 - 4020

Published: March 8, 2023

Hitherto, Pt-based catalysts still are state of the art for oxygen reduction reaction (ORR) and hydrogen evolution (HER), but high dosage, low atom-utilization efficiency, uncontrollable size Pt species seriously impede their applications. Given this, we propose an effective way by enhancing Pt–transition metal single-atom interaction. Due to strong interaction between Mn sites in Mn–N–C species, overgrowth is effectively limited with average smaller than 2.5 nm. Meanwhile, regulated electronic structure drives electron transfer from adjacent sites, endowing reduced energy barrier higher intrinsic activity. As expected, obtained Pt@Mn-SAs/N-C nanocatalyst ideal ultralow loading (1.98 wt %) exhibits extraordinarily ORR mass activity at 0.9 V acidic alkaline media, which 11.1 14.7 times larger that commercial Pt/C, respectively. Moreover, 30 mV, its HER even 33.4 18.7 Pt/C. Theory calculation results show favorable charge density rearrangement resulting electron-enriched negatively shifted d-band centers, weaken surface adsorption key intermediates, boosting ORR/HER This work provides enlightenment integration multiple active centers catalysts.

Language: Английский

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Recent Advances in Engineered Ru‐Based Electrocatalysts for the Hydrogen/Oxygen Conversion Reactions

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(41)

Published: Sept. 1, 2022

Abstract The application of renewable energy conversion devices is considered as one the effective ways to alleviate shortage and environmental pollution. Designing electrocatalysts with excellent performance affordable price promising accelerate reaction process large‐scale application. At present, ruthenium (Ru)‐based nanomaterials have shown similar catalytic activity but superior demand compared commercial Pt/C. This undoubtedly makes Ru‐based a perfect candidate replace advanced Pt catalysts. Significant progress made in rational design electrocatalysts, an in‐depth understanding engineering strategies induced effects still at early stage. review summarizes modification for enhancing Ru, including surface structure, metal element, nonmetal size, bimetallic oxides, heterostructure strategies. Then electronic modulation generated by intramolecular intermolecular are elucidated. Further, engineered hydrogen oxygen reactions highlighted, correlations strategies, activity, pathways elaborated. Finally, challenges prospects presented future development practical nanomaterials.

Language: Английский

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Highly efficient electrocatalytic hydrogen evolution coupled with upcycling of microplastics in seawater enabled via Ni3N/W5N4 janus nanostructures

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 307, P. 121198 - 121198

Published: Feb. 10, 2022

Language: Английский

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Interfacial component coupling effects towards precise heterostructure design for efficient electrocatalytic water splitting

Nano Energy, Journal Year: 2022, Volume and Issue: 103, P. 107753 - 107753

Published: Aug. 27, 2022

Language: Английский

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Recent advances in Ru-based electrocatalysts for oxygen evolution reaction

Journal of Materials Chemistry A, Journal Year: 2022, Volume and Issue: 11(4), P. 1634 - 1650

Published: Dec. 29, 2022

Recently reported ruthenium (Ru)-based catalysts for the oxygen evolution reaction (OER) falling in Ru metal and compound subclasses are summarized with special emphasis being given to a discussion of activity/stability-enhancing strategies.

Language: Английский

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Oxygen Radical Coupling on Short-Range Ordered Ru Atom Arrays Enables Exceptional Activity and Stability for Acidic Water Oxidation

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(19), P. 12958 - 12968

Published: May 2, 2024

The discovery of efficient and stable electrocatalysts for oxygen evolution reaction (OER) in acid is vital the commercialization proton-exchange membrane water electrolyzer. In this work, we demonstrate that short-range Ru atom arrays with near-ideal Ru–Ru interatomic distances a unique Ru–O hybridization state can trigger direct O*–O* radical coupling to form an intermediate O*–O*-Ru configuration during acidic OER without generating OOH* species. Further, suppress participation lattice dissolution active Ru. Benefiting from these advantages, as-designed array-Co3O4 electrocatalyst breaks activity/stability trade-off plagues RuO2-based electrocatalysts, delivering excellent overpotential only 160 mV at 10 mA cm–2 0.5 M H2SO4 outstanding durability 1500 h operation, representing one best acid-stable reported date. 18O-labeled operando spectroscopic measurements together theoretical investigations revealed switched on oxide path mechanism (OPM) OER. Our work not guides design improved catalysts but also encourages pursuit metal array-based other electrocatalytic reactions.

Language: Английский

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Atom Doping Engineering of Transition Metal Phosphides for Hydrogen Evolution Reactions

Electrochemical Energy Reviews, Journal Year: 2022, Volume and Issue: 5(S2)

Published: Nov. 8, 2022

Language: Английский

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