Atomically Dispersed Co₂–N₆ and Fe–N₄ Costructures Boost Oxygen Reduction Reaction in Both Alkaline and Acidic Media

Advanced Materials, Год журнала: 2021, Номер 33(49)

Опубликована: Окт. 8, 2021

Abstract Polynary transition‐metal atom catalysts are promising to supersede platinum (Pt)‐based for oxygen reduction reaction (ORR). Regulating the local configuration of atomic is key catalyst performance enhancement. Different from previously reported single‐atom or dual‐atom configurations, a new type ternary‐atom catalyst, which consists atomically dispersed, nitrogen‐coordinated Co–Co dimers, and Fe single sites (i.e., Co 2 –N 6 Fe–N 4 structures) that coanchored on highly graphitized carbon supports developed. This unique ORR outperforms with only in both alkaline acid conditions. Density functional theory calculations clearly unravels synergistic effect sites, can induce higher filling degree Fe–d orbitals favors binding capability *OH intermediates (the rate determining step). may be alternative Pt drive cathodic zinc–air batteries.

Язык: Английский

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Quasi-solid-state Zn-air batteries with an atomically dispersed cobalt electrocatalyst and organohydrogel electrolyte

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Июнь 27, 2022

Abstract Quasi-solid-state Zn-air batteries are usually limited to relatively low-rate ability (<10 mA cm −2 ), which is caused in part by sluggish oxygen electrocatalysis and unstable electrochemical interfaces. Here we present a high-rate robust quasi-solid-state battery enabled atomically dispersed cobalt sites anchored on wrinkled nitrogen doped graphene as the air cathode polyacrylamide organohydrogel electrolyte with its hydrogen-bond network modified addition of dimethyl sulfoxide. This design enables cycling current density 100 over 50 h at 25 °C. A low-temperature stability 300 (at 0.5 ) 90% capacity retention −60 °C broad temperature adaptability (−60 60 °C) also demonstrated.

Язык: Английский

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Single-Atom (Iron-Based) Catalysts: Synthesis and Applications

Chemical Reviews, Год журнала: 2021, Номер 121(21), С. 13620 - 13697

Опубликована: Окт. 13, 2021

Supported single-metal atom catalysts (SACs) are constituted of isolated active metal centers, which heterogenized on inert supports such as graphene, porous carbon, and oxides. Their thermal stability, electronic properties, catalytic activities can be controlled via interactions between the center neighboring heteroatoms nitrogen, oxygen, sulfur. Due to atomic dispersion amount required for catalysis decreased, thus offering new possibilities control selectivity a given transformation well improve catalyst turnover frequencies numbers. This review aims comprehensively summarize synthesis Fe-SACs with focus anchoring single atoms (SA) carbon/graphene supports. The characterization these advanced materials using various spectroscopic techniques their applications in diverse research areas described. When applicable, mechanistic investigations conducted understand specific behavior Fe-SACs-based highlighted, including use theoretical models.

Язык: Английский

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Designing a Built-In Electric Field for Efficient Energy Electrocatalysis

ACS Nano, Год журнала: 2022, Номер 16(12), С. 19959 - 19979

Опубликована: Дек. 15, 2022

To utilize intermittent renewable energy as well achieve the goals of peak carbon dioxide emissions and neutrality, various electrocatalytic devices have been developed. However, reactions, e.g., hydrogen evolution reaction/oxygen reaction in overall water splitting, polysulfide conversion lithium–sulfur batteries, formation/decomposition lithium peroxide lithium–oxygen nitrate reduction to degrade sewage, suffer from sluggish kinetics caused by multielectron transfer processes. Owing merits accelerated charge transport, optimized adsorption/desorption intermediates, raised conductivity, regulation microenvironment, ease combine with geometric characteristics, built-in electric field (BIEF) is expected overcome above problems. Here, we give a Review about very recent progress BIEF for efficient electrocatalysis. First, construction strategies characterization methods (qualitative quantitative analysis) are summarized. Then, up-to-date overviews engineering electrocatalysis, attention on electron structure optimization microenvironment modulation, analyzed discussed detail. In end, challenges perspectives proposed. This gives deep understanding design electrocatalysts next-generation storage devices.

Язык: Английский

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A pH-universal ORR catalyst with single-atom iron sites derived from a double-layer MOF for superior flexible quasi-solid-state rechargeable Zn–air batteries

Energy & Environmental Science, Год журнала: 2021, Номер 14(12), С. 6455 - 6463

Опубликована: Янв. 1, 2021

The pH-universal ORR performance and reaction-mechanism scheme of the Fe 1 /d-CN catalyst, which acts as cathode for flexible quasi-solid-state alkaline/neutral rechargeable Zn–air batteries.

Язык: Английский

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Recent Advances and Applications Toward Emerging Lithium–Sulfur Batteries: Working Principles and Opportunities

Energy & environment materials, Год журнала: 2021, Номер 5(3), С. 777 - 799

Опубликована: Авг. 7, 2021

Lithium–sulfur (Li‐S) batteries have been considered as promising candidates for large‐scale high energy density devices due to the potentially density, low cost, and more pronounced ecological compatibility. However, complex Li‐S conversion reactions, unsatisfactory battery performance, unsafe metallic Li anode restrict development of achieve commercialization. This review mainly focuses on three aspects which are remaining challenges, recent advances, applications in batteries. Firstly, this portrays chemistry involving multi‐step multi‐electron reaction mechanism, well challenges. Then, scientific strategies very advances cathode, electrolyte, lithium anode, other constituent parts detailly summed up, their advantages limitations. For sake promoting practicalization, next section is primarily concerned with problems, corresponding solutions, application scenarios practical pouch cells. Finally, important findings guidelines some future directions trends developing emerging briefly summarized.

Язык: Английский

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Ultrastable FeCo Bifunctional Electrocatalyst on Se-Doped CNTs for Liquid and Flexible All-Solid-State Rechargeable Zn–Air Batteries

Nano Letters, Год журнала: 2021, Номер 21(5), С. 2255 - 2264

Опубликована: Фев. 18, 2021

The rechargeable Zn–air batteries as an environmentally friendly sustainable energy technology have been extensively studied. However, it is still a challenge to develop non-noble metal bifunctional catalysts with high oxygen reduction well evolution reaction (ORR and OER) activity superior durability, which limit the large-scale application of batteries. Herein, we synthesized ultrastable FeCo electrocatalyst on Se-doped CNTs (FeCo/Se-CNT) via gravity guided chemical vapor deposition (CVD) strategy. catalyst exhibits excellent ORR (E1/2 = 0.9 V) OER (overpotential at 10 mA cm–2 340 mV) properties simultaneously, surpassing commercial Pt/C RuO2/C catalysts. More importantly, shows unordinary stability, that is, no obvious decrease after 30K cycles accelerated durability test for processes. small potential gap (0.75 represents activities FeCo/Se-CNT catalyst. possesses outstanding electrochemical performance liquid flexible all-solid-state batteries, example, open circuit voltage (OCV) peak power density 1.543 1.405 V 173.4 37.5 mW cm–2, respectively.

Язык: Английский

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Graphene‐Supported Atomically Dispersed Metals as Bifunctional Catalysts for Next‐Generation Batteries Based on Conversion Reactions

Advanced Materials, Год журнала: 2021, Номер 34(5)

Опубликована: Окт. 22, 2021

Next-generation batteries based on conversion reactions, including aqueous metal-air batteries, nonaqueous alkali metal-O2 and -CO2 metal-chalcogen metal-ion have attracted great interest. However, their use is restricted by inefficient reversible of active agents. Developing bifunctional catalysts to accelerate the reaction kinetics in both discharge charge processes urgently needed. Graphene-, or graphene-like carbon-supported atomically dispersed metal (G-ADMCs) been demonstrated show excellent activity various electrocatalytic making them promising candidates. Different from G-ADMCs for catalysis, which only require high one direction, rechargeable should provide discharging charging. This review provides guidance design fabrication next-generation reactions. The key challenges that prevent conversion, origin G-ADMCs, current principles highly analyzed highlighted each conversion-type battery. Finally, a summary outlook development G-ADMC materials with energy density efficiency are given.

Язык: Английский

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Strain Engineering in Electrocatalysts: Fundamentals, Progress, and Perspectives

Advanced Energy Materials, Год журнала: 2021, Номер 12(5)

Опубликована: Дек. 22, 2021

Abstract Strain engineering of nanomaterials, namely, designing, tuning, or controlling surface strains nanomaterials is an effective strategy to achieve outstanding performance in different for their various applications. This article summarizes recent progress and achievements the development strain‐rich electrocatalysts (SREs) applications field electrochemical energy conversion technologies. It starts from definition lattice strains, followed by classification where mechanisms strain formation reported methods regulate related are elaborated. The SRE characterization techniques overviewed, focusing deeply on clarification strain‐property relationship these SREs. Their electrocatalytic reactions further highlighted, including hydrogen evolution reaction, oxygen reduction alcohol oxidation carbon dioxide nitrogen reaction. Related reaction SREs interpreted after taking catalytic performance, as well between properties into account. challenges future opportunities finally outlined discussed together with potential fields.

Язык: Английский

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Atomically precise electrocatalysts for oxygen reduction reaction

Chem, Год журнала: 2023, Номер 9(2), С. 280 - 342

Опубликована: Фев. 1, 2023

Язык: Английский

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