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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Synergistic Fe−Se Atom Pairs as Bifunctional Oxygen Electrocatalysts Boost Low‐Temperature Rechargeable Zn‐Air Battery

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(15)

Опубликована: Фев. 18, 2023

Herein, we successfully construct bifunctional electrocatalysts by synthesizing atomically dispersed Fe-Se atom pairs supported on N-doped carbon (Fe-Se/NC). The obtained Fe-Se/NC shows a noteworthy oxygen catalytic performance with low potential difference of 0.698 V, far superior to that reported Fe-based single-atom catalysts. theoretical calculations reveal p-d orbital hybridization around the leads remarkably asymmetrical polarized charge distributions. based solid-state rechargeable Zn-air batteries (ZABs-Fe-Se/NC) present stable charge/discharge 200 h (1090 cycles) at 20 mA cm-2 25 °C, which is 6.9 times ZABs-Pt/C+Ir/C. At extremely temperature -40 ZABs-Fe-Se/NC displays an ultra-robust cycling 741 (4041 1 , about 11.7 More importantly, could be operated for 133 (725 even 5 °C.

Язык: Английский

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Dual‐Atom Support Boosts Nickel‐Catalyzed Urea Electrooxidation

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(22)

Опубликована: Март 24, 2023

Nickel-based catalysts have been regarded as one of the most promising electrocatalysts for urea oxidation reaction (UOR), however, their activity is largely limited by inevitable self-oxidation Ni species (NSOR) during UOR. Here, we proposed an interface chemistry modulation strategy to trigger occurrence UOR before NSOR via constructing a 2D/2D heterostructure that consists ultrathin NiO anchored Ru-Co dual-atom support (Ru-Co DAS/NiO). Operando spectroscopic characterizations confirm this unique triggering mechanism on surface DAS/NiO. Consequently, fabricated catalyst exhibits outstanding with low potential 1.288 V at 10 mA cm-2 and remarkable long-term durability more than 330 h operation. DFT calculations demonstrate favorable electronic structure induced heterointerface endows energetically NSOR.

Язык: Английский

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Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application

Advanced Materials, Год журнала: 2023, Номер 35(31)

Опубликована: Фев. 23, 2023

Single/dual-metal atoms supported on carbon matrix can be modulated by coordination structure and neighboring active sites. Precisely designing the geometric electronic uncovering structure-property relationships of single/dual-metal confront with grand challenges. Herein, this review summarizes latest progress in microenvironment engineering single/dual-atom sites via a comprehensive comparison single-atom catalyst (SACs) dual-atom catalysts (DACs) term design principles, modulation strategy, theoretical understanding structure-performance correlations. Subsequently, recent advances several typical electrocatalysis process are discussed to get general reaction mechanisms finely-tuned SACs DACs. Finally, full-scaled summaries challenges prospects given for This will provide new inspiration development atomically dispersed electrocatalytic application.

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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Electrocatalytic water splitting: Mechanism and electrocatalyst design

Nano Research, Год журнала: 2023, Номер 16(7), С. 9142 - 9157

Опубликована: Апрель 2, 2023

Язык: Английский

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Liquid Fluxional Ga Single Atom Catalysts for Efficient Electrochemical CO₂Reduction

Angewandte Chemie International Edition, Год журнала: 2022, Номер 62(3)

Опубликована: Ноя. 18, 2022

Precise design and tuning of the micro-atomic structure single atom catalysts (SACs) can help efficiently adapt complex catalytic systems. Herein, we inventively found that when active center main group element gallium (Ga) is downsized to atomic level, whose characteristic has significant differences from conventional bulk rigid Ga catalysts. The SACs with a P, S coordination environment display specific flow properties, showing CO products FE ≈92 % at -0.3 V vs. RHE in electrochemical CO2 reduction (CO2 RR). Theoretical simulations demonstrate adaptive dynamic transition optimizes adsorption energy *COOH intermediate renews sites time, leading excellent RR selectivity stability. This liquid system interfaces lays foundation for future exploration synthesis catalysis.

Язык: Английский

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Construction of Co₄ Atomic Clusters to Enable Fe−N₄ Motifs with Highly Active and Durable Oxygen Reduction Performance

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(30)

Опубликована: Май 24, 2023

Abstract Fe−N−C catalysts with single‐atom Fe−N 4 configurations are highly needed owing to the high activity for oxygen reduction reaction (ORR). However, limited intrinsic and dissatisfactory durability have significantly restrained practical application of proton‐exchange membrane fuel cells (PEMFCs). Here, we demonstrate that constructing adjacent metal atomic clusters (ACs) is effective in boosting ORR performance stability catalysts. The integration uniform Co ACs on N‐doped carbon substrate (Co @/Fe 1 @NC) realized through a “pre‐constrained” strategy using molecular Fe(acac) 3 implanted precursors. as‐developed @NC catalyst exhibits excellent half‐wave potential ( E 1/2 ) 0.835 V vs. RHE acidic media peak power density 840 mW cm −2 H 2 −O cell test. First‐principles calculations further clarify catalytic mechanism identified modified ACs. This work provides viable precisely establishing atomically dispersed polymetallic centers efficient energy‐related catalysis.

Язык: Английский

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Continuous Modulation of Electrocatalytic Oxygen Reduction Activities of Single‐Atom Catalysts throughp‐nJunction Rectification

Angewandte Chemie International Edition, Год журнала: 2022, Номер 62(5)

Опубликована: Ноя. 16, 2022

Fine-tuning single-atom catalysts (SACs) to surpass their activity limit remains challenging at atomic scale. Herein, we exploit p-type semiconducting character of SACs having a metal center coordinated nitrogen donors (MeNx ) and rectify local charge density by an n-type semiconductor support. With iron phthalocyanine (FePc) as model SAC, introducing gallium monosulfide that features low work function generates space-charged region across the junction interface, causes distortion FeN4 moiety spin-state transition in FeII center. This catalyst shows over two-fold higher specific oxygen-reduction than pristine FePc. We further employ three other chalcogenides varying supports, discover linear correlation between activities supported rectification degrees, which clearly indicates can be continuously tuned this strategy.

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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