Understanding the structure-performance relationship of active sites at atomic scale

Nano Research, Год журнала: 2022, Номер 15(8), С. 6888 - 6923

Опубликована: Июнь 14, 2022

Язык: Английский

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MIL‐101‐Derived Mesoporous Carbon Supporting Highly Exposed Fe Single‐Atom Sites as Efficient Oxygen Reduction Reaction Catalysts

Advanced Materials, Год журнала: 2021, Номер 33(23)

Опубликована: Апрель 29, 2021

Abstract Fe single‐atom catalysts (Fe SACs) with atomic FeN x active sites are very promising alternatives to platinum‐based for the oxygen reduction reaction (ORR). The pyrolysis of metal–organic frameworks (MOFs) is a common approach preparing SACs, though most MOF‐derived reported date microporous and thus suffer from poor mass transfer high proportion catalytically inaccessible sites. Herein, NH 2 ‐MIL‐101(Al), MOF possessing mesoporous cage architecture, used as precursor prepare series N‐doped carbon supports (denoted herein NC‐MIL101‐T) well‐defined structure at different temperatures. NC‐MIL101‐T then impregnated Fe(II)‐phenanthroline complex, heated again yield SAC‐MIL101‐T rich in accessible single atom best performing SAC‐MIL101‐1000 catalyst offers outstanding ORR activity alkaline media, evidenced by an half‐wave potential 0.94 V (vs RHE) 0.1 m KOH, well excellent performance both aqueous primary zinc–air batteries (a near maximum theoretical energy density 984.2 Wh kg Zn −1 ) solid‐state peak power 50.6 mW cm −2 specific capacity 724.0 mAh ).

Язык: Английский

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MOF-on-MOF hybrids: Synthesis and applications

Coordination Chemistry Reviews, Год журнала: 2021, Номер 432, С. 213743 - 213743

Опубликована: Янв. 22, 2021

Язык: Английский

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Atomically Dispersed Fe–Co Dual Metal Sites as Bifunctional Oxygen Electrocatalysts for Rechargeable and Flexible Zn–Air Batteries

ACS Catalysis, Год журнала: 2022, Номер 12(2), С. 1216 - 1227

Опубликована: Янв. 5, 2022

Single-metal site catalysts have exhibited highly efficient electrocatalytic properties due to their unique coordination environments and adjustable local structures for reactant adsorption electron transfer. They been widely studied many electrochemical reactions, including oxygen reduction reaction (ORR) evolution (OER). However, it remains a significant challenge realize high-efficiency bifunctional catalysis (ORR/OER) with single-metal-type active sites. Herein, we report atomically dispersed Fe–Co dual metal sites (FeCo–NC) derived from Fe Co co-doped zeolitic imidazolate frameworks (ZIF-8s), aiming build up multiple ORR/OER catalysts. The FeCo–NC catalyst shows excellent catalytic activity in alkaline media the ORR (E1/2 = 0.877 V) OER (Ej=10 1.579 V). Moreover, its outstanding stability during is comparable noble-metal (Pt/C RuO2). atomic dispersion state, structure, charge density difference of were characterized determined using advanced physical characterization functional theory (DFT) calculations. FeCo–N6 moieties are likely main simultaneously improved performance relative traditional single We further incorporated into an air electrode fabricating rechargeable flexible Zn–air batteries, generating superior power (372 mW cm–2) long-cycle (over 190 h) stability. This work would provide method design synthesize multi-metal electrocatalysis.

Язык: Английский

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Porphyrin-based frameworks for oxygen electrocatalysis and catalytic reduction of carbon dioxide

Chemical Society Reviews, Год журнала: 2021, Номер 50(4), С. 2540 - 2581

Опубликована: Янв. 1, 2021

The recent progress made on porphyrin-based frameworks and their applications in energy-related conversion technologies (e.g., ORR, OER CO₂RR) storage Zn–air batteries).

Язык: Английский

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Superiority of Dual‐Atom Catalysts in Electrocatalysis: One Step Further Than Single‐Atom Catalysts

Advanced Energy Materials, Год журнала: 2022, Номер 12(9)

Опубликована: Янв. 18, 2022

Abstract In recent years, dual‐atom catalysts (DACs) have attracted extensive attention, as an extension of single‐atom (SACs). Compared with SACs, DACs higher metal loading and more complex flexible active sites, thus achieving better catalytic performance providing opportunities for electrocatalysis. This review introduces the research progress in years on how to design new enhance Firstly, advantages increasing are introduced. Then, role changing adsorption condition reactant molecules atoms is discussed. Moreover, ways which can reduce reaction energy barrier key steps change path explored. Catalytic applications different electrocatalytic reactions, including carbon dioxide reduction reaction, oxygen evolution hydrogen nitrogen followed. Finally, a brief summary made challenges prospects

Язык: Английский

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Recent Advances in MOF‐Derived Single Atom Catalysts for Electrochemical Applications

Advanced Energy Materials, Год журнала: 2020, Номер 10(38)

Опубликована: Авг. 13, 2020

Abstract Electrocatalysis plays a critical role in clean energy conversion, enabling great improvement for future sustainable technologies. Single atom catalysts (SACs) derived from metal–organic framework (MOF) are emerging extraordinary materials electrochemical catalytic applications. Covering the merits of unique electronic structure, low‐coordination environment, quantum size effect, and metal–support interaction, SACs promise enhanced electrocatalytic activity, stability, selectivity field conversion. In this article, MOF synthesis routes to afford well‐dispersed along with respective mechanism systematically reviewed first, typical examples each strategy carefully discussed. Then characterization techniques understanding isolated spatial distribution, local coordination environment SACs, insights into stable mechanisms provided by density functional theory (DFT) calculations summarized. addition, several important applications MOF‐derived including oxygen reduction reaction, CO 2 nitrogen hydrogen evolution etc., highlighted. To facilitate development high‐performing technical challenges corresponding research directions proposed.

Язык: Английский

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Dual-ligand and hard-soft-acid-base strategies to optimize metal-organic framework nanocrystals for stable electrochemical cycling performance

National Science Review, Год журнала: 2021, Номер 9(7)

Опубликована: Окт. 29, 2021

Most metal-organic frameworks (MOFs) hardly maintain their physical and chemical properties after exposure to acidic, neutral, or alkaline aqueous solutions, resulting in insufficient stability, therefore limiting applications. Thus, the design synthesis of stable size/morphology-controlled MOF nanocrystals is critical but challenging. In this study, dual-ligand hard-soft-acid-base strategies were used fabricate a variety 3D pillared-layer [Ni(thiophene-2,5-dicarboxylate)(4,4'-bipyridine)]n (1D nanofibers, 2D nanosheets aggregates) with controllable morphology by varying concentration 4,4'-bipyridine thus controlling crystal growth direction. Owing shorter ion diffusion length, enhanced electron/ion transfer strong interactions between thiophene-2,5-dicarboxylate 4,4'-bipyridine, showed much larger specific capacitance than 1D nanofibers aggregates. A single device an output voltage as high 3.0 V exceptional cycling performance (95% retention 5000 cycles at 3 mA cm-2) was realized configuring two asymmetric supercapacitive devices series. The excellent property charge-discharge mechanism are consistent theory.

Язык: Английский

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Noble-metal single-atoms in thermocatalysis, electrocatalysis, and photocatalysis

Energy & Environmental Science, Год журнала: 2021, Номер 14(5), С. 2954 - 3009

Опубликована: Янв. 1, 2021

This review summarizes the recent advances about noble-metal single-atom catalysts in thermocatalysis, electrocatalysis, and photocatalysis.

Язык: Английский

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“More is Different:” Synergistic Effect and Structural Engineering in Double‐Atom Catalysts

Advanced Functional Materials, Год журнала: 2020, Номер 31(3)

Опубликована: Ноя. 16, 2020

Abstract Double‐atom catalysts (DACs) have emerged as a novel frontier in heterogeneous catalysis because the synergistic effect between adjacent active sites can promote their catalytic activity while maintaining high atomic utilization efficiency, good selectivity, and stability originating from atomically dispersed nature. In this review, recent progress both experimental theoretical research on DACs for various reactions is focused. Specifically, central tasks design of DACs—manipulating engineering electronic structures catalysts—are systematically reviewed, along with prevailing experimental, characterization, computational modeling approaches. Furthermore, practical applications water splitting, oxygen reduction reaction, nitrogen carbon dioxide reaction are addressed. Finally, future challenges summarized an outlook further investigations toward high‐performance energy environmental provided.

Язык: Английский

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