Electronic Structure Regulation of MnCo₂O₄ via Surface‐Phosphorization Coupling to Monolithic Carbon for Oxygen Electrocatalysis in Zn–Air Batteries

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

Published: July 1, 2024

Abstract An urgent challenge to the development of rechargeable Zn–air batteries (RZABs) is highly active, durable, and low‐cost catalysts for oxygen reduction reaction evolution (ORR OER). Herein, a carbon‐based monolithic catalyst designed via anchoring P‐modified MnCo 2 O 4 inverse spinel nanoparticles on biomass‐derived carbon (P‐MnCo @PWC). The introduction surface P atoms regulates electronic structures valences metal by adjusting coordination fields (P‐O) δ– Metal‐P. optimization adsorption behavior key intermediates facilitates activation conversion species. structure beneficial construction three‐phase interface efficient mass transfer high electrical conductivity. P‐MnCo @PWC displays outstanding bifunctional catalytic properties with thin Δ E (the difference between OER potential at 10 mA cm – ORR halfwave potential) 0.66 V. RZAB as cathode delivers an exceptional peak power density (160 mW ) remarkable cycle life (over 1200 cycles), overcoming those noble counterparts. This research provides promising general surface‐phosphorization way design electrocatalysts high‐value utilization biomass.

Language: Английский

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Precisely designing asymmetrical selenium-based dual-atom sites for efficient oxygen reduction

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Jan. 7, 2025

Owing to their synergistic interactions, dual-atom catalysts (DACs) with well-defined active sites are attracting increasing attention. However, more experimental research and theoretical investigations needed further construct explicit understand the synergy that facilitates multistep catalytic reactions. Herein, we precisely design a series of asymmetric selenium-based comprise heteronuclear SeN2–MN2 (M = Fe, Mn, Co, Ni, Cu, Mo, etc.) for efficient oxygen reduction reaction (ORR). Spectroscopic characterisation calculations revealed selenium atoms can efficiently polarise charge distribution other metal through short-range regulation. In addition, compared Se or Fe single-atom sites, SeFe facilitate in conversion energy barrier from *O *OH via coadsorption intermediates. Among these designed catalysts, selenium-iron achieves superior alkaline ORR performance, half-wave potential 0.926 V vs. reversible hydrogen electrode. SeN2–FeN2-based Zn–air battery has high specific capacity (764.8 mAh g−1) maximum power density (287.2 mW cm−2). This work may provide good perspective designing DACs improve efficiency. Dual-atom precise gaining attention, but studies optimise construction synergy. Here authors report dual- atom reaction.

Language: Английский

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Transforming Adsorbate Surface Dynamics in Aqueous Electrocatalysis: Pathways to Unconstrained Performance

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

Published: Jan. 28, 2025

Abstract Developing highly efficient catalysts to accelerate sluggish electrode reactions is critical for the deployment of sustainable aqueous electrochemical technologies, yet remains a great challenge. Rationally integrating functional components tailor surface adsorption behaviors and adsorbate dynamics would divert reaction pathways alleviate energy barriers, eliminating conventional thermodynamic constraints ultimately optimizing flow within systems. This approach has, therefore, garnered significant interest, presenting substantial potential developing that simultaneously enhance activity, selectivity, stability. The immense promise rapid evolution this design strategy, however, do not overshadow challenges ambiguities persist, impeding realization breakthroughs in electrocatalyst development. review explores latest insights into principles guiding catalytic surfaces enable favorable contexts hydrogen oxygen electrochemistry. Innovative approaches tailoring adsorbate‐surface interactions are discussed, delving underlying govern these dynamics. Additionally, perspectives on prevailing presented future research directions proposed. By evaluating core identifying gaps, seeks inspire rational design, discovery novel mechanisms concepts, ultimately, advance large‐scale implementation electroconversion technologies.

Language: Английский

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Regulating nonmetallic species beyond the first coordination shell of single-atom catalysts for high-performance electrocatalysis

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(9), P. 3679 - 3710

Published: Jan. 1, 2023

Nonmetallic functional species beyond the first coordination shell can affect or even dictate electrocatalytic performance of single-atom catalysts via indirect, long-range interaction with metal atoms.

Language: Английский

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Unified ORR mechanism criteria via charge–spin–coordination of Fe functional units

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 17(1), P. 27 - 48

Published: Nov. 10, 2023

The “charge–spin–coordination” relationship was introduced into Fe functional units (Fe-FUs) in multiple forms to comprehensively analyze their activity sources and degradation mechanisms during the ORR process.

Language: Английский

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Recent advances in Fe-N-C- and Co-N-C-based materials as bifunctional electrocatalysts for oxygen reduction and oxygen evolution

Science China Chemistry, Journal Year: 2023, Volume and Issue: 67(4), P. 1137 - 1160

Published: Dec. 5, 2023

Language: Английский

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Co/Co₃O₄ Heterojunctions Encased in Porous N-Doped Carbon Nanocapsules for High-Performance Cathode of Rechargeable Zinc–Air Batteries

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(8), P. 3702 - 3711

Published: Feb. 9, 2024

A long-term goal of rechargeable zinc-air batteries (ZABs) has always been to design bifunctional electrocatalysts that are robust, effective, and affordable for the oxygen reduction reaction (ORR) evolution (OER). It become a feasible method construct metal/metal oxide interfaces achieve superior electrocatalytic performance ORR OER by enhanced charge transfer. In this study, Co/Co

Language: Английский

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Engineering Synergetic Fe‐Co Atomic Pairs Anchored on Porous Carbon for Enhanced Oxygen Reduction Reaction

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

Published: July 28, 2024

Abstract The rational design of heteronuclear dual‐atom catalyst (DAC) is intricate due to the random dispersion metal atoms under thermal treatment. Herein, a novel precursor pre‐orientation strategy reported construct Fe‐Co diatomic sites atomically dispersed on nitrogen doped carbon (Fe‐Co‐NC) via cubic Prussian blue analogue as source. Due specific synergy between Fe and Co centers, obtained Fe‐Co‐NC renders outstanding oxygen reduction reaction (ORR) performance with positive half‐wave potential good durability in wide pH range. Density functional theory further clarifies active centers reveals that dual atomic follows modulation mechanism, where intermediates tended adsorb site, while neighboring atom can assist by lowering d ‐band center site. Experimentally theoretically emphasizes priority catalysts over homonuclear Fe‐Fe‐NC Co‐Co‐NC DAC. Moreover, Zn‐Air battery (ZAB) microbial fuel cell (MFC) assembled cathodes both exhibit splendid power density (382 mW cm −2 for ZAB, 2034 ± 103 m MFC) well excellent stability. This work provides new perspective construction precise regulation catalysts.

Language: Английский

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Molecular Fe─N₄ Moieties Coupled with Atomic Co─N₄ Sites Toward Improved Oxygen Reduction Performance

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(32)

Published: March 28, 2024

Abstract Research on high‐efficiency and cost‐efficient catalysts for oxygen reduction reaction (ORR) is still a vital but challenging issue commercializing metal–air batteries. Herein, single‐molecule/atom hybrid catalyst developed to boost the ORR, in which iron phthalocyanine molecules containing molecular Fe─N 4 moieties couple with atomic Co─N sites surface of polyhedral carbon. Density functional theory calculations reveal that face‐to‐face laminated construction can effectively modulate electronic structure active atoms reduce energy barrier rate‐determining step ORR. As result, this demonstrates excellent ORR performance, featuring half‐wave potential 0.904 V, peak power density 238.3 mW cm −2 zinc–air battery, outstanding electrocatalytic stability. This work offers distinctive robust molecular/atomic engineering approach creating efficient electrocatalysts, advancing fields

Language: Английский

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Insight into synergy for oxygen reduction electrocatalysis of iron-nitrogen-carbon

Chem, Journal Year: 2024, Volume and Issue: 10(7), P. 1994 - 2030

Published: July 1, 2024

Language: Английский

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