Non-carbon-supported single-atom site catalysts for electrocatalysis

Energy & Environmental Science, Год журнала: 2021, Номер 14(5), С. 2809 - 2858

Опубликована: Янв. 1, 2021

Non-carbon supported SACs were classified into eight categories based on the nature of their substrates for first time, and corresponding anchoring stabilization mechanisms have been systematically summarized discussed.

Язык: Английский

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Single‐Atom Fe Catalysts for Fenton‐Like Reactions: Roles of Different N Species

Advanced Materials, Год журнала: 2022, Номер 34(17)

Опубликована: Март 8, 2022

Recognizing and controlling the structure-activity relationships of single-atom catalysts (SACs) is vital for manipulating their catalytic properties various practical applications. Herein, Fe SACs supported on nitrogen-doped carbon (SA-Fe/CN) are reported, which show high reactivity (97% degradation bisphenol A in only 5 min), stability (80% maintained after five runs), wide pH suitability (working range 3-11) toward Fenton-like reactions. The roles different N species these reactions further explored, both experimentally theoretically. It discovered that graphitic an adsorptive site target molecule, pyrrolic coordinates with Fe(III) plays a dominant role reaction, pyridinic N, coordinated Fe(II), minor contributor to SA-Fe/CN. Density functional theory (DFT) calculations reveal lower d-band center location pyrrolic-type sites leads easy generation Fe-oxo intermediates, thus, excellent properties.

Язык: Английский

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Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis

Nano Research, Год журнала: 2022, Номер 15(9), С. 7806 - 7839

Опубликована: Июнь 2, 2022

Язык: Английский

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Ru–Co Pair Sites Catalyst Boosts the Energetics for the Oxygen Evolution Reaction

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(32)

Опубликована: Май 31, 2022

Abstract Manipulating the coordination environment of active center via anion modulation to reveal tailored activity and selectivity has been widely achieved, especially for carbon‐based single‐atom site catalysts (SACs). However, tuning ligand fields by single‐site metal cation regulation identifying effects on resulting electronic configuration is seldom explored. Herein, we propose a Ru strategy engineer properties constructing Ru/LiCoO 2 SAC with atomically dispersed Ru−Co pair sites. Benefitting from strong coupling between Co sites, catalyst possesses an enhanced electrical conductivity achieves near‐optimal oxygen adsorption energies. Therefore, optimized delivers superior evolution reaction (OER) low overpotential, high mass 1000 A g oxide −1 at small overpotential 335 mV, excellent long‐term stability. It also exhibits rapid kinetics rate capability outstanding durability in zinc–air battery.

Язык: Английский

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P and Cu Dual Sites on Graphitic Carbon Nitride for Photocatalytic CO₂Reduction to Hydrocarbon Fuels with High C₂H₆Evolution

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(40)

Опубликована: Авг. 15, 2022

The light-driven CO2 reduction to multi-carbon products is especially meaningful, while the low efficiency of multi-electron transfer and sluggish C-C coupling greatly hinder its development. Herein, we report a photocatalyst comprising P Cu dual sites anchored on graphitic carbon nitride (P/Cu SAs@CN), which achieves high C2 H6 evolution rate 616.6 μmol g-1 h-1 in reducing hydrocarbons. detailed spectroscopic characterizations identify formation charge-enriched sites, where isolated atoms serve as hole capture during photocatalysis. Theoretical simulations combined with situ FTIR measurement reveal kinetically feasible process for intermediate (*OC-COH) confirm favorable production P/Cu SAs@CN photocatalyst. This work offers new insights into design atomic precision toward highly efficient photocatalytic conversion value-added products.

Язык: Английский

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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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Long‐Range Interactions in Diatomic Catalysts Boosting Electrocatalysis

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(52)

Опубликована: Окт. 6, 2022

Abstract The simultaneous presence of two active metal centres in diatomic catalysts (DACs) leads to the occurrence specific interactions between sites. Such interactions, referred as long‐range (LRIs), play an important role determining rate and selectivity a reaction. optimal combination must be determined achieve targeted efficiency. To date, various types DACs have been synthesised applied electrochemistry. However, LRIs not systematically summarised. Herein, regulation, mechanism, electrocatalytic applications are comprehensively summarised discussed. In addition basic information above, challenges, opportunities, future development proposed order present overall view reference for research.

Язык: Английский

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A Site Distance Effect Induced by Reactant Molecule Matchup in Single‐Atom Catalysts for Fenton‐Like Reactions

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(33)

Опубликована: Июнь 20, 2022

Abstract Understanding the site interaction nature of single‐atom catalysts (SACs), especially densely populated SACs, is vital for their application to various catalytic reactions. Herein, we report a distance effect, which emphasizes how well adjacent copper atoms (denoted as d Cu1−Cu1 ) matches with reactant peroxydisulfate (PDS) molecular size determine Fenton‐like reaction reactivity on carbon‐supported SACs. The optimized in range 5–6 Å, PDS, endows catalyst nearly two times higher turnover frequency than that beyond this range, accordingly achieving record‐breaking kinetics oxidation emerging organic contaminants. Further studies suggest effect originates from alteration PDS adsorption dual‐site structure Cu 1 −Cu sites when falls within significantly enhancing interfacial charge transfer and consequently resulting most efficient activation so far.

Язык: Английский

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Single‐atom catalysis for carbon neutrality

Carbon Energy, Год журнала: 2022, Номер 4(6), С. 1021 - 1079

Опубликована: Июль 14, 2022

Abstract Currently, more than 86% of global energy consumption is still mainly dependent on traditional fossil fuels, which causes resource scarcity and even emission high amounts carbon dioxide (CO 2 ), resulting in a severe “Greenhouse effect.” Considering this situation, the concept “carbon neutrality” has been put forward by 125 countries one after another. To achieve goals neutrality,” two main strategies to reduce CO emissions develop sustainable clean can be adopted. Notably, these are crucial for synthesis advanced single‐atom catalysts (SACs) energy‐related applications. In review, we highlight unique SACs conversion into high‐efficiency energy, example, through photocatalytic, electrocatalytic, thermal catalytic hydrogenation technologies, convert hydrocarbon fuels (CO, CH 4 , HCOOH, 3 OH, multicarbon [C 2+ ] products). addition, introduce technologies devices replace polluting such as photocatalytic electrocatalytic water splitting produce hydrogen oxygen reduction reaction (ORR) fuel cells. Impressively, several representative examples (including d ‐, ds p f ‐blocks) conversion, H ORR discussed describe methods, characterization, corresponding activity. Finally, review concludes with description challenges outlooks future applications contributing toward neutrality.

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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