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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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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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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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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Nanoscale Metal Particle Modified Single‐Atom Catalyst: Synthesis, Characterization, and Application

Advanced Materials, Год журнала: 2023, Номер 36(2)

Опубликована: Июль 13, 2023

Single-atom catalysts (SACs) have attracted considerable attention in heterogeneous catalysis because of their well-defined active sites, maximum atomic utilization efficiency, and unique unsaturated coordinated structures. However, effectiveness is limited to reactions requiring sites containing multiple metal atoms. Furthermore, the loading amounts single-atom must be restricted prevent aggregation, which can adversely affect catalytic performance despite high activity individual The introduction nanoscale particles (NMPs) into SACs (NMP-SACs) has proven an efficient approach for improving performance. A comprehensive review urgently needed systematically introduce synthesis, characterization, application NMP-SACs mechanisms behind superior This first presents classifies different through NMPs enhance SACs. It then summarizes currently reported synthetic strategies state-of-the-art characterization techniques NMP-SACs. Moreover, electro/thermo/photocatalysis, reasons are discussed. Finally, challenges perspectives future design advanced addressed.

Язык: Английский

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Engineering a Copper Single‐Atom Electron Bridge to Achieve Efficient Photocatalytic CO₂ Conversion

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(13)

Опубликована: Фев. 7, 2023

Developing highly efficient and stable photocatalysts for the CO2 reduction reaction (CO2 RR) remains a great challenge. We designed Z-Scheme photocatalyst with N-Cu1 -S single-atom electron bridge (denoted as Cu-SAEB), which was used to mediate RR. The production of CO O2 over Cu-SAEB is high 236.0 120.1 μmol g-1 h-1 in absence sacrificial agents, respectively, outperforming most previously reported photocatalysts. Notably, as-designed throughout 30 cycles, totaling 300 h, owing strengthened contact interface Cu-SAEB, mediated by atomic structure. Experimental theoretical calculations indicated that SAEB greatly promoted Z-scheme interfacial charge-transport process, thus leading enhancement photocatalytic RR Cu-SAEB. This work represents promising platform development have potential conversion applications.

Язык: Английский

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Coordinating the Edge Defects of Bismuth with Sulfur for Enhanced CO₂ Electroreduction to Formate

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(25)

Опубликована: Апрель 20, 2023

Bismuth-based materials have been recognized as promising catalysts for the electrocatalytic CO2 reduction reaction (ECO2 RR). However, they show poor selectivity due to competing hydrogen evolution (HER). In this study, we developed an edge defect modulation strategy Bi by coordinating defects of bismuth (Bi) with sulfur, promote ECO2 RR and inhibit HER. The prepared demonstrate excellent product selectivity, a high HCOO- Faraday efficiency ≈95 % partial current ≈250 mA cm-2 under alkaline electrolytes. Density function theory calculations reveal that sulfur tends bind defects, reducing coordination-unsaturated sites (*H adsorption sites), regulating charge states neighboring improve *OCHO adsorption. This work deepens our understanding mechanism on bismuth-based catalysts, guiding design advanced catalysts.

Язык: Английский

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Coordination engineering in single-site catalysts: General principles, characterizations, and recent advances

Chem, Год журнала: 2023, Номер 10(1), С. 48 - 85

Опубликована: Сен. 21, 2023

Язык: Английский

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Directional and Ultrafast Charge Transfer in Oxygen‐Vacancy‐Rich ZnO@Single‐Atom Cobalt Core‐Shell Junction for Photo‐Fenton‐Like Reaction

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

Опубликована: Май 31, 2023

In photosynthesis, solar energy is harvested by photosensitizers, and then, the excited electrons transfer via a Z-Scheme mode to enzymatic catalytic centers trigger redox reactions. Herein, we constructed core-shell Z-scheme heterojunction of semiconductor@single-atom catalysts (SACs). The oxygen-vacancy-rich ZnO core single-atom Co-N4 sites supported on nitrogen-rich carbon shell (SA-Co-CN) act as photosensitizer enzyme-mimicking active centers, respectively. Driven built-in electric field across heterojunction, photoexcited could rapidly (2 ps) from n-type p-type SA-Co-CN shell, finally boosting performance surface-exposed for peroxymonosulfate (PMS) activation under light irradiation. synergies between photocatalysis heterogeneous Fenton-like reaction lead phenomenally enhanced production various reactive oxygen species rapid degradation microcontaminants in water. Experimental theoretical results validate that interfacial coupling with greatly facilitates PMS adsorption reducing enhancing cascade electron processes photo-Fenton-like reaction.

Язык: Английский

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