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

Nano Research, Journal Year: 2022, Volume and Issue: 15(9), P. 7806 - 7839

Published: June 2, 2022

Language: Английский

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Metal-metal interactions in correlated single-atom catalysts

Science Advances, Journal Year: 2022, Volume and Issue: 8(17)

Published: April 29, 2022

Single-atom catalysts (SACs) include a promising family of electrocatalysts with unique geometric structures. Beyond conventional ones fully isolated metal sites, an emerging class the adjacent single atoms exhibiting intersite metal-metal interactions appear in recent years and can be denoted as correlated SACs (C-SACs). This type provides more opportunities to achieve substantial structural modification performance enhancement toward wider range electrocatalytic applications. On basis clear identification interactions, this review critically examines research progress C-SACs. It shows that control enables regulation atomic structure, local coordination, electronic properties atoms, which facilitate modulation behavior Last, we outline directions for future work design development C-SACs, is indispensable creating high-performing new SAC architectures.

Language: Английский

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Long‐Range Interactions in Diatomic Catalysts Boosting Electrocatalysis

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(52)

Published: Oct. 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.

Language: Английский

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Theoretically Revealed and Experimentally Demonstrated Synergistic Electronic Interaction of CoFe Dual-Metal Sites on N-doped Carbon for Boosting Both Oxygen Reduction and Evolution Reactions

Nano Letters, Journal Year: 2022, Volume and Issue: 22(8), P. 3392 - 3399

Published: April 18, 2022

Heteronuclear double-atom catalysts, unlike single atom may change the charge density of active metal sites by introducing another atom, thereby modifying adsorption energies reaction intermediates and increasing catalytic activities. First, functional theory calculations are used to figure out best combination modeling two transition-metal atoms from Fe, Co, Ni onto N-doped graphene. Generally, Fe Co highly for oxygen reduction (ORR) evolution (OER), respectively. The form CoFe-N-C not only further improves Fe's ORR Co's OER activities but also greatly enhances site's Then, we synthesize a two-step pyrolysis process find that exhibits exceptional electrocatalytic in alkaline media, significantly superior Fe-N-C Co-N-C even commercial catalysts.

Language: Английский

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

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(31)

Published: Feb. 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.

Language: Английский

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Atomically Dispersed Ni–Cu Catalysts for pH‐Universal CO₂ Electroreduction

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(13)

Published: Jan. 10, 2023

CO2 electroreduction is of great significance to reduce emissions and complete the carbon cycle. However, unavoidable carbonate formation low utilization efficiency in neutral or alkaline electrolytes hinder its application at commercial scale. The development reduction under acidic conditions provides a promising strategy, but inhibition hydrogen evolution reaction difficult. Herein, first work design Ni-Cu dual atom catalyst supported on hollow nitrogen-doped reported for pH-universal CO. shows high CO Faradaic ≈99% acidic, neutral, electrolytes, partial current densities reach 190 ± 11, 225 10, 489 14 mA cm-2 , respectively. In particular, reaches 64.3%, which twice as that conditions. Detailed study indicates existence electronic interaction between Ni Cu atoms. atoms push d-band center further toward Fermi level, thereby accelerating *COOH. addition, operando characterizations density functional theory calculation are used elucidate possible mechanism electrolytes.

Language: Английский

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Review of Carbon Support Coordination Environments for Single Metal Atom Electrocatalysts (SACS)

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(1)

Published: April 20, 2023

This topical review focuses on the distinct role of carbon support coordination environment single-atom catalysts (SACs) for electrocatalysis. The article begins with an overview atomic configurations in SACs, including a discussion advanced characterization techniques and simulation used understanding active sites. A summary key electrocatalysis applications is then provided. These processes are oxygen reduction reaction (ORR), evolution (OER), hydrogen (HER), nitrogen (NRR), dioxide (CO

Language: Английский

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Interatomic Electronegativity Offset Dictates Selectivity When Catalyzing the CO₂ Reduction Reaction

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(26)

Published: June 1, 2022

Abstract Achieving efficient efficiency and selectivity for the electroreduction of CO 2 to value‐added feedstocks has been challenging, due thermodynamic stability molecules competing hydrogen evolution reaction. Herein, a dual‐single‐atom catalyst consisting atomically dispersed CuN 4 NiN bimetal sites is synthesized with electrospun carbon nanofibers (CuNi‐DSA/CNFs). Theoretical experimental studies reveal strong electron interactions induced by electronegativity offset between Cu Ni atoms. The delicately averaged compensated electronic structures result in an effect that optimizes adsorption strength *COOH intermediate boosts reduction reaction (CO RR) kinetics, notably promoting intrinsic activity catalyst. CuNi‐DSA/CNFs exhibits outstanding FE 99.6% across broad potential window −0.78– −1.18 V (vs reversible electrode), high turnover frequency 2870 h –1 , excellent durability (25 h). Furthermore, aqueous Zn‐CO battery power conversion constructed. This atomic‐level dual‐atom provides appealing direction develop advanced electrocatalysts RR.

Language: Английский

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Co-catalytic metal–support interactions in single-atom electrocatalysts

Nature Reviews Materials, Journal Year: 2024, Volume and Issue: 9(3), P. 173 - 189

Published: Jan. 10, 2024

Language: Английский

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Efficient Photoreduction of Diluted CO₂to Tunable Syngas by Ni−Co Dual Sites through d‐band Center Manipulation

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(42)

Published: Aug. 29, 2022

Photocatalytic conversion of CO2 into syngas is a promising way to address the energy and environmental challenges. Here we report integration Ni-Co dual sites on Ni doped Co3 O4 ultrathin nanosheets assembled double-hollow nanotube (Ni-Co3 NSDHN) for efficient photoreduction low-concentration . Quasi in situ spectra density functional theory calculations demonstrate that declining d-band center enables electrons accumulation dxz /dyz -2π* dz2 -5σ orbitals. As result, binding strength *CO weakened *H adsorption site modulated from metal an oxygen site. Remarkably, Ni-Co3 NSDHN exhibits superior diluted photoconversion activity controllable selectivity under irradiation visible light or even natural sunlight. A evolution rate 170.0 mmol g-1 h-1 with apparent quantum yield 3.7 % continuously adjustable CO/H2 ratios 1 : 10 are achieved.

Language: Английский

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