Atomically dispersed materials: Ideal catalysts in atomic era

Nano Research, Год журнала: 2023, Номер 17(1), С. 18 - 38

Опубликована: Май 25, 2023

Язык: Английский

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The reformation of catalyst: From a trial-and-error synthesis to rational design

Nano Research, Год журнала: 2023, Номер 17(4), С. 3261 - 3301

Опубликована: Сен. 27, 2023

Язык: Английский

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Engineering the Electronic Structure of Single‐Atom Iron Sites with Boosted Oxygen Bifunctional Activity for Zinc–Air Batteries

Advanced Materials, Год журнала: 2022, Номер 35(9)

Опубликована: Дек. 19, 2022

Abstract Rechargeable zinc–air batteries typically require efficient, durable, and inexpensive bifunctional electrocatalysts to support oxygen reduction/evolution reactions (ORR/OER). However, sluggish kinetics mass transportation challenges must be addressed if the performance of these catalysts is enhanced. Herein, a strategy fabricate catalyst comprising atomically dispersed iron atoms supported on mesoporous nitrogen‐doped carbon (Fe SAs/NC) with accessible metal sites optimized electronic metal–support interactions developed. Both experimental results theoretical calculations reveal that engineered structures active can regulate charge distribution Fe centers optimize adsorption/desorption oxygenated intermediates. The SAs/NC containing 1 N 4 O achieves remarkable ORR activity over entire pH range, half‐wave potentials 0.93, 0.83, 0.75 V (vs reversible hydrogen electrode) in alkaline, acidic, neutral electrolytes, respectively. In addition, it demonstrates promising low overpotential 320 mV at 10 mA cm −2 for OER alkaline conditions. battery assembled exhibits superior than Pt/C+RuO 2 counterpart terms peak power density, specific capacity, cycling stability. These findings demonstrate importance structure engineering directing catalytic activity.

Язык: Английский

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Geometric and Electronic Engineering of Atomically Dispersed Copper‐Cobalt Diatomic Sites for Synergistic Promotion of Bifunctional Oxygen Electrocatalysis in Zinc–Air Batteries

Advanced Materials, Год журнала: 2023, Номер 35(25)

Опубликована: Апрель 11, 2023

The development of rechargeable zinc-air batteries is heavily dependent on bifunctional oxygen electrocatalysts to offer exceptional reduction/evolution reaction (ORR/OER) activities. However, the design such with high activity and durability challenging. Herein, a strategy proposed create an electrocatalyst comprised copper-cobalt diatomic sites highly porous nitrogen-doped carbon matrix (Cu-Co/NC) abundantly accessible metal optimal geometric electronic structures. Experimental findings theoretical calculations demonstrate that synergistic effect Cu-Co dual-metal metal-N4 coordination induce asymmetric charge distributions moderate adsorption/desorption behavior intermediates. This exhibits extraordinary electrocatalytic activities in alkaline media, half-wave potential 0.92 V for ORR low overpotential 335 mV at 10 mA cm-2 OER. In addition, it demonstrates acidic (0.85 V) neutral (0.74 media. When applied battery, achieves operational performance outstanding (510 h), ranking as one most efficient reported date. work importance engineering isolated boosting electrochemical energy devices.

Язык: Английский

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Carbon nitride based materials: more than just a support for single-atom catalysis

Chemical Society Reviews, Год журнала: 2023, Номер 52(15), С. 4878 - 4932

Опубликована: Янв. 1, 2023

Recently, the missing link between homogeneous and heterogeneous catalysis has been found it was named single-atom (SAC). However, SAC field still faces important challenges, one of which is controlling bonding/coordination single atoms support in order to compensate for increase surface energy when particle size reduced due atomic dispersion. Excellent candidates meet this requirement are carbon nitride (CN)-based materials. Metal can be firmly trapped nitrogen-rich coordination sites CN materials, makes them a unique class hosts preparing catalysts (SACs). As most promising two-dimensional supports stabilize isolated metal atoms, materials have increasingly employed SACs. Herein, we will cover recent advances single-atoms supported by In review, characterization techniques challenges faced topic discussed, commonly synthetic methods delineated different Finally, catalytic performance SACs based on nitrides reviewed with special focus their photocatalytic applications. particular, prove as non-innocent support. The relationship two-way, where change electronic properties support, while features matrix tune activity reactions. highlight frontiers field, including analytical method development, truly controlled methods, allowing fine control loading multi-element synthesis, how understanding two-way exchange behind push next level.

Язык: Английский

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Recent advances of single-atom catalysts in CO₂conversion

Energy & Environmental Science, Год журнала: 2023, Номер 16(7), С. 2759 - 2803

Опубликована: Янв. 1, 2023

The catalytic transformation of CO 2 into valuable fuels/chemicals is a promising and economically profitable process because it offers an alternative toward fossil feedstocks the benefit transforming cycling on scale-up.

Язык: Английский

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Hydrogen Radical-Induced Electrocatalytic N₂ Reduction at a Low Potential

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(18), С. 10259 - 10267

Опубликована: Апрель 25, 2023

Realizing efficient hydrogenation of N2 molecules in the electrocatalytic nitrogen reduction reaction (NRR) is crucial achieving high activity at a low potential because it theoretically requires higher equilibrium than other steps. Analogous to metal hydride complexes for reduction, this step by chemical can weaken dependence initial process. However, strategy rarely reported NRR, and catalytic mechanism remains ambiguous lacks experimental evidence. Here, we show highly electrocatalyst (ruthenium single atoms anchored on graphdiyne/graphene sandwich structures) with hydrogen radical-transferring mechanism, which graphdiyne (GDY) generates radicals (H•), effectively activate generate NNH (•NNH). A dual-active site constructed suppress competing evolution, where preferentially adsorbs GDY Ru serve as adsorption •NNH promote further NH3 synthesis. As result, selectivity are obtained simultaneously -0.1 V versus reversible electrode. Our findings illustrate novel transfer that greatly reduce maintain NRR provide powerful guidelines design concept electrocatalysts.

Язык: Английский

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Selective Photocatalytic Reduction of CO₂ to CO Mediated by Silver Single Atoms Anchored on Tubular Carbon Nitride

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(26)

Опубликована: Апрель 28, 2023

Artificial photosynthesis is a promising strategy for converting carbon dioxide (CO2 ) and water (H2 O) into fuels value-added chemical products. However, photocatalysts usually suffered from low activity product selectivity due to the sluggish dynamic transfer of photoexcited charge carriers. Herein, we describe anchoring Ag single atoms on hollow porous polygonal C3 N4 nanotubes (PCN) form photocatalyst Ag1 @PCN with Ag-N3 coordination CO2 photoreduction using H2 O as reductant. The as-synthesized exhibits high CO production rate 0.32 μmol h-1 (mass catalyst: 2 mg), (>94 %), an excellent stability in long term. Experiments density functional theory (DFT) reveal that strong metal-support interactions (Ag-N3 favor *CO2 adsorption, *COOH generation desorption, accelerate carriers between atoms, thereby accounting enhanced selectivity. This work provides deep insight important role enhancing photoactivity photoreduction.

Язык: Английский

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Bioinspired porous three-coordinated single-atom Fe nanozyme with oxidase-like activity for tumor visual identification via glutathione

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Ноя. 6, 2023

Inspired by structures of natural metalloenzymes, a biomimetic synthetic strategy is developed for scalable synthesis porous Fe-N3 single atom nanozymes (pFeSAN) using hemoglobin as Fe-source and template. pFeSAN delivers 3.3- 8791-fold higher oxidase-like activity than Fe-N4 Fe3O4 nanozymes. The high catalytic performance attributed to (1) the suppressed aggregation atomically dispersed Fe; (2) facilitated mass transfer maximized exposure active sites created mesopores thermal removal (2 ~ 3 nm); (3) unique electronic configuration oxygen-to-water oxidation pathway (analogy with cytochrome c oxidase). successfully demonstrated rapid colorimetric detection glutathione low limit (2.4 nM) wide range (50 nM-1 mM), further real-time, facile, (~6 min) precise visualization analysis methodology tumors via level, showing its potentials diagnostic clinic applications.

Язык: Английский

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Mn-Co dual sites relay activation of peroxymonosulfate for accelerated decontamination

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 330, С. 122656 - 122656

Опубликована: Март 21, 2023

Язык: Английский

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