Recent advances of metal suboxide catalysts for carbon‐neutral energy applications

EcoEnergy, Journal Year: 2024, Volume and Issue: 2(1), P. 45 - 82

Published: Feb. 22, 2024

Abstract Metal suboxides have emerged as a class of promising candidates for many electrocatalytic applications owing to their enhanced electrical conductivity and chemical activities. In this review, we summarized the recent progress metal suboxides. We firstly introduced discovery suboxides, categories according element tables. Then various synthetic methods been systematically illustrated involving solid‐state synthesis, high‐temperature low‐temperature synthesis plasma‐driven methods, etc. addition, demonstrated in field water, carbon nitrogen cycle‐based energy catalysis technologies electrochemical hydrogen evolution reaction, oxygen reduction dioxide reduction, urea oxidation methanol reaction nitrate Finally, make brief conclusion about developments giving an outlook future research challenges. These insights are expected hold promise developing suboxide catalysts toward practical applications.

Language: Английский

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Sulfur‐Bridged Asymmetric CuNi Bimetallic Atom Sites for CO₂ Reduction with High Efficiency

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(33)

Published: June 25, 2024

Abstract Double‐atom catalysts (DACs) with asymmetric coordination are crucial for enhancing the benefits of electrochemical carbon dioxide reduction and advancing sustainable development, however, rational design DACs is still challenging. Herein, this work synthesizes atomically dispersed novel sulfur‐bridged Cu‐S‐Ni sites (named Cu‐S‐Ni/SNC), utilizing biomass wool keratin as precursor. The plentiful disulfide bonds in overcome limitations traditional gas‐phase S ligand etching process enable one‐step formation S‐bridged sites. X‐ray absorption spectroscopy (XAS) confirms existence bimetallic N 2 Cu‐S‐NiN moiety. In H‐cell, Cu‐S‐Ni/SNC shows high CO Faraday efficiency 98.1% at −0.65 V versus RHE. Benefiting from charge tuning effect between metal site bridged sulfur atoms, a large current density 550 mA cm −2 can be achieved −1.00 flow cell. Additionally, situ XAS, attenuated total reflection surface‐enhanced infrared (ATR‐SEIRAS), functional theory (DFT) calculations show Cu main adsorption dual‐regulated by Ni which enhances activation accelerates *COOH intermediates. This kind atom may open new pathways precision preparation performance regulation atomic materials toward energy applications.

Language: Английский

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p-d Orbital Hybridization Induced by Asymmetrical FeSn Dual Atom Sites Promotes the Oxygen Reduction Reaction

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(31), P. 21357 - 21366

Published: July 25, 2024

With more flexible active sites and intermetal interaction, dual-atom catalysts (DACs) have emerged as a new frontier in various electrocatalytic reactions. Constructing typical p-d orbital hybridization between p-block d-block metal atoms may bring avenues for manipulating the electronic properties thus boosting activities. Herein, we report distinctive heteronuclear dual-metal atom catalyst with asymmetrical FeSn dual embedded on two-dimensional C2N nanosheet (FeSn–C2N), which displays excellent oxygen reduction reaction (ORR) performance half-wave potential of 0.914 V an alkaline electrolyte. Theoretical calculations further unveil powerful stannum ferrum sites, triggers electron delocalization lowers energy barrier *OH protonation, consequently enhancing ORR activity. In addition, FeSn–C2N-based Zn–air battery provides high maximum power density (265.5 mW cm–2) specific capacity (754.6 mA h g–1). Consequently, this work validates immense along perception into logical design DACs.

Language: Английский

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Achieving Negatively Charged Pt Single Atoms on Amorphous Ni(OH)2 Nanosheets with Promoted Hydrogen Absorption in Hydrogen Evolution

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 16(1)

Published: May 23, 2024

Single-atom (SA) catalysts with nearly 100% atom utilization have been widely employed in electrolysis for decades, due to the outperforming catalytic activity and selectivity. However, most of reported SA are fixed through strong bonding between dispersed single metallic atoms nonmetallic substrates, which greatly limits controllable regulation electrocatalytic catalysts. In this work, Pt-Ni bonded Pt catalyst adjustable electronic states was successfully constructed a electrochemical reduction on coordination unsaturated amorphous Ni(OH)

Language: Английский

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Enhanced N₂ Adsorption and Activation by Combining Re Clusters and In Vacancies as Dual Sites for Efficient and Selective Electrochemical NH₃ Synthesis

Nano Letters, Journal Year: 2024, Volume and Issue: 24(2), P. 748 - 756

Published: Jan. 3, 2024

The electrochemical N2 reduction reaction (NRR) is a green and energy-saving sustainable technology for NH3 production. However, high activity selectivity can hardly be achieved in the same catalyst, which severely restricts development of NRR. In2Se3 with partially occupied p-orbitals suppress H2 evolution (HER), shows excellent presence VIn simultaneously provide active sites confine Re clusters through strong charge transfer. Additionally, well-isolated stabilized on by confinement effect result Re-VIn maximum availability. By combining as dual spontaneous adsorption activation, NRR performance enhanced significantly. As result, Re-In2Se3-VIn/CC catalyst delivers yield rate (26.63 μg h–1 cm–2) FEs (30.8%) at −0.5 V vs RHE.

Language: Английский

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MXene‐Bimetallic Hybrids via Mixed Molten Salts Etching for Kinetics‐Enhanced and Dendrite‐Free Lithium–Sulfur Batteries

Small, Journal Year: 2024, Volume and Issue: 20(34)

Published: April 9, 2024

Lithium-sulfur (Li-S) batteries with high theoretical energy density (2600 Wh kg

Language: Английский

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Lattice Strain and Mott–Schottky Effect of the Charge-Asymmetry Pd₁Fe Single-Atom Alloy Catalyst for Semi-Hydrogenation of Alkynes with High Efficiency

ACS Nano, Journal Year: 2024, Volume and Issue: 18(20), P. 13286 - 13297

Published: May 10, 2024

The ideal interface design between the metal and substrate is crucial in determining overall performance of alkyne semihydrogenation reaction. Single-atom alloys (SAAs) with isolated dispersed active centers are media for study reaction effects. Herein, a charge-asymmetry "armor" SAA (named Pd1Fe SAA@PC), which consists alloy core semiconducting P-doped C (PC) shell, rationally designed as an catalyst selective hydrogenation alkynes high efficiency. Multiple spectroscopic analyses density functional theory calculations have demonstrated that SAA@PC dual-regulated by lattice tensile Schottky effects, govern selectivity activity hydrogenation, respectively. (1) PC shell layer applied external traction force causing 1.2% strain inside to increase selectivity. (2) P doping into C-shell realized transition from p-type semiconductor n-type semiconductor, thereby forming unique junction advancing activity. dual regulation effect ensures excellent phenylethylene, achieving conversion rate 99.9% 98.9% at 4 min. These well-defined modulation strategies offer practical approach rational optimization catalysts.

Language: Английский

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Local Symmetry-Broken Single Pd Atoms Induced by Doping Ag Sites for Selective Electrocatalytic Semihydrogenation of Alkynes

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 8, 2025

Engineering the local coordination environment of single metal atoms is an effective strategy to improve their catalytic activity, selectivity, and stability. In this study, we develop asymmetric Pd–Ag diatomic site on surface g-C3N4 for selective electrocatalytic semihydrogenation alkynes. The Pd atom catalyst, which has a locally symmetric coordination, was inactive phenylacetylene in 1 M KOH 1,4-dioxane solution at applied potential −1.3 V (vs RHE). sharp contrast, doping Ag sites into catalyst form paired with substantially enhanced reaction, resulting high conversion (>98%) exceptional time-independent selectivity styrene under identical conditions. Characterization theoretical calculations reveal that introduction disrupts symmetry by forming bonds N2–Pd–Ag–N configuration, thereby modulating electronic geometric structures sites, turn benefits adsorption activation substrate lowers energy barrier rate-determining step semihydrogenation, ultimately enhancing reaction. This work provides facile powerful design advanced catalysts tuning catalysis.

Language: Английский

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Breaking symmetry for better catalysis: insights into single-atom catalyst design

Chemical Society Reviews, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

This review examines the strategies of symmetry breaking (charge/coordination/geometric) in single-atom catalysts to regulate active site electronic structures, greatly enhancing catalytic performance.

Language: Английский

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Recent advances in transition metal electrocatalysts for effective nitrogen reduction reaction under ambient conditions

EcoEnergy, Journal Year: 2024, Volume and Issue: 2(2), P. 229 - 257

Published: May 29, 2024

Abstract As one of the world's largest chemical products, ammonia (NH 3 ) plays a vital role in industry, agricultural production, and national defense. In modern NH is produced primarily through high‐temperature high‐pressure Haber–Bosch process, which consumes large amounts energy releases greenhouse gases. Electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions has been widely considered among many fixation methods, can be using renewable energy. However, main challenge to achieve both high yield Faraday efficiency, attributed strong N ≡ bond serious hydrogen evolution reaction. Based on key problems, this review discussed transition metal (TM) catalysts, including alloys, TM oxides, sulfides, carbides, strategies for tuning electronic structure, regulating morphology, bimetallic synergistic effect improving NRR performance. Moreover, also summarized detection methods reliable control experimental parameters process obtain accurate results. Finally, challenges future directions catalysts are considered, emphasizing available opportunities by following giving principles.

Language: Английский

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