Sub-nm RuO_x Clusters on Pd Metallene for Synergistically Enhanced Nitrate Electroreduction to Ammonia

ACS Nano, Journal Year: 2023, Volume and Issue: 17(2), P. 1081 - 1090

Published: Jan. 11, 2023

The electrochemical nitrate reduction to ammonia reaction (NO3RR) has emerged as an appealing route for achieving both wastewater treatment and production. Herein, sub-nm RuOx clusters anchored on a Pd metallene (RuOx/Pd) are reported highly effective NO3RR catalyst, delivering maximum NH3-Faradaic efficiency of 98.6% with corresponding NH3 yield rate 23.5 mg h–1 cm–2 partial current density 296.3 mA at −0.5 V vs RHE. Operando spectroscopic characterizations combined theoretical computations unveil the synergy enhance energetics through mechanism hydrogen spillover hydrogen-bond interactions. In detail, activates NO3– form intermediates, while dissociates H2O generate *H, which spontaneously migrates RuOx/Pd interface via process. Further interactions between spillovered *H intermediates makes desorb from participate in intermediate hydrogenation, contributing enhanced activity NO3–-to-NH3 conversion.

Language: Английский

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Modulating the d‐Band Center Enables Ultrafine Pt₃Fe Alloy Nanoparticles for pH‐Universal Hydrogen Evolution Reaction

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(41)

Published: July 1, 2023

By providing dual active sites to synergistically accelerate H2 O dissociation and H+ reduction, ordered intermetallic alloys usually show extraordinary performance for pH-universal hydrogen evolution reaction (HER). Herein, activated N-doped mesoporous carbon spheres supported Pt3 Fe (Pt3 Fe/NMCS-A), as a highly-efficient electrocatalyst HER, are reported. The Fe/NMCS-A exhibits low overpotentials (η10 ) of 13, 29, 48 mV deliver 10 mA cm-2 in 0.5 m SO4 , 1.0 KOH, phosphate buffered solution (PBS), respectively, well robust stability maintain the overall catalytic performances. Theoretical studies reveal that strong Pt 5d-Fe 3d orbital electronic interactions negatively shift d-band center (εd 5d orbital, resulting reduced H* adsorption energy enhanced acidic HER activity. With acting co-adsorption *OH intermediates, barrier is required dissociate afford which greatly promotes formation alkaline neutral conditions. synthetic strategy further extended synthesis Co Ni with excellent activity electrolytes, demonstrating great potential these Pt-based practical applications.

Language: Английский

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Recent advances in interface engineering strategy for highly‐efficient electrocatalytic water splitting

InfoMat, Journal Year: 2022, Volume and Issue: 5(1)

Published: Oct. 13, 2022

Abstract The hydrogen energy generated by the electrocatalytic water splitting reaction has been established as a renewable and clean carrier with ultra‐high density, which can well make up for shortcomings of conventional sources, such geographical limitations, climatic dependence, wastage. Notably, introduction electrocatalysts enhance efficiency process to generate hydrogen. Particularly, heterostructure constructed coupling multiple components (or phases) have emerged most promising option due well‐known electronic synergistic effects. existing reviews on interface engineering electrocatalyst design mostly focus relationship between heterostructures specific reactions. However, comprehensive overview integration model building, directional synthesis, mechanism rarely reported. To this end, in review, development catalysts is systematically introduced from perspective classification, growth regulation performance based interfacial microenvironment (bonding, configuration, lattice strain, etc.), thereby offering useful insights construction models. Besides, combined current applications strategies, challenges future are discussed relevant solutions proposed. Overall, review serve theoretical reference mechanism, further promote production technologies low consumption high yield. image

Language: Английский

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Constructing regulable supports via non-stoichiometric engineering to stabilize ruthenium nanoparticles for enhanced pH-universal water splitting

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: March 29, 2024

Abstract Establishing appropriate metal-support interactions is imperative for acquiring efficient and corrosion-resistant catalysts water splitting. Herein, the interaction mechanism between Ru nanoparticles a series of titanium oxides, including TiO, Ti 4 O 7 TiO 2, designed via facile non-stoichiometric engineering systematically studied. 7, with unique band structure, high conductivity chemical stability, endows ingenious through interfacial Ti–O–Ru units, which stabilizes species during OER triggers hydrogen spillover to accelerate HER kinetics. As expected, Ru/Ti displays ultralow overpotentials 8 mV 150 long operation 500 h at 10 mA cm −2 in acidic media, expanded pH-universal environments. Benefitting from excellent bifunctional performance, proton exchange membrane anion electrolyzer assembled achieves superior performance robust operation. The work paves way energy conversion devices.

Language: Английский

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Interfacial built-in electric-field for boosting energy conversion electrocatalysis

Nanoscale Horizons, Journal Year: 2023, Volume and Issue: 8(4), P. 441 - 452

Published: Jan. 1, 2023

A critical review of built-in electric fields for the applications in electrocatalytic reactions is organized by focusing on fundamental concepts, modification strategies, and positive influences promotion catalytic performance.

Language: Английский

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Reactive template‐derived interfacial engineering of CoP/CoO heterostructured porous nanotubes towards superior electrocatalytic hydrogen evolution

Carbon Energy, Journal Year: 2022, Volume and Issue: 5(1)

Published: Oct. 14, 2022

Abstract The development of economical, efficient, and robust electrocatalysts toward the hydrogen evolution reaction (HER) is highly imperative for rapid advancement renewable H 2 energy‐associated technologies. Extensive utilization heterointerface effect can endow catalysts with remarkably boosted electrocatalytic performance due to modified electronic state active sites. Herein, we demonstrate deliberate crafting CoP/CoO heterojunction porous nanotubes (abbreviated as PNTs hereafter) using a self‐sacrificial template‐engaged strategy. Precise control over Kirkendall diffusion process presynthesized cobalt–aspartic acid complex nanowires indispensable formation heterostructures. topochemical transformation strategy reactive templates enables uniform maximized construction heterojunctions throughout all nanotubes. establishment could considerably modify configuration sites also improve electric conductivity, which endows resultant enhanced intrinsic activity. Simultaneously, hollow nanotube architectures allow sufficient accessibility exterior/interior surfaces molecular permeability, drastically promoting kinetics. Consequently, when used HER electrocatalysts, well‐designed show Pt‐like activity, an overpotential only 61 mV at 10 mA cm −2 excellent stability in 1.0 M KOH medium, exceeding those vast majority previously reported nonprecious candidates. Density functional theory calculations further substantiate that optimization Gibbs free energies water adsorption adsorption, resulting present study may provide in‐depth insights into fundamental mechanisms heterojunction‐induced regulation, pave way rational design advanced Earth‐abundant future.

Language: Английский

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Recent Progress on Ruthenium-Based Electrocatalysts towards the Hydrogen Evolution Reaction

Catalysts, Journal Year: 2023, Volume and Issue: 13(12), P. 1497 - 1497

Published: Dec. 7, 2023

Hydrogen has emerged as an important candidate for clean energy, owing to its environmentally friendly advantages. Electrolytic hydrogen production stands out the most promising technology production. Therefore, design of highly efficient electrocatalysts is significant drive application technologies. Platinum (Pt)-based catalysts are famous their outstanding performance in evolution reaction (HER). However, expensive cost limits wide application. Ruthenium (Ru)-based have received extensive attention due relatively lower and HER similar that Pt. Nevertheless, Ru-based still unable meet industrial demands. improving through modification remains significant. In this review, mechanism analyzed latest research progress summarized. From perspective, addressing adsorption intermediates on electrocatalyst surface, adsorption–activation interface water molecules, behavior molecules proposing solutions enhance main findings, ultimately contributing promoting field electrocatalysis.

Language: Английский

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Hydrogen spillover as a promising strategy for boosting heterogeneous catalysis and hydrogen storage

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 471, P. 144691 - 144691

Published: July 8, 2023

Language: Английский

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Intensifying the Supported Ruthenium Metallic Bond to Boost the Interfacial Hydrogen Spillover Toward pH‐Universal Hydrogen Evolution Catalysis

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(28)

Published: March 29, 2024

Abstract The effectuation of pH‐universal electrocatalysis is highly attractive but still challenging for the hydrogen evolution reaction (HER). It appeals not only facilitated electron transport also kinetical proton mass transfer. In this study, a via‐hole Ru/MoO 2 confined heterostructure profiled as metal‐support platform electron/mass transfer‐boosted HER studies. indicated that as‐formed Ru─O─Mo bridge can modulate electronic at interface, and adsorption transfer are kinetically derived by intensified metallic Ru─Ru bond. Resultantly, stably attains Pt‐beyond activity with an ultralow overpotential 9.2 mV 10 mA cm −2 in 1 m KOH, achieves competitive stability acidic/neutral electrolytes. Both experimental computational results reveal accelerated kinetics attributable to intensive through interfacial Ru→MoO spillover effect. This work opens up opportunities rationalize advanced electrocatalysts effect bond engineering.

Language: Английский

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Accelerated Transfer and Spillover of Carbon Monoxide through Tandem Catalysis for Kinetics‐boosted Ethylene Electrosynthesis

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(10)

Published: Jan. 3, 2023

Cu-based catalysts have been widely applied in electroreduction of carbon dioxide (CO2 ER) to produce multicarbon (C2+ ) feedstocks (e.g., C2 H4 ). However, the high energy barriers for CO2 activation on Cu surface is a challenge catalytic efficiency and product selectivity. Herein, we developed an situ *CO generation spillover strategy by engineering single Ni atoms pyridinic N-enriched support with sodalite (SOD) topology (Ni-SOD/NC) that acted as donor feed adjacent nanoparticles (NPs) intermediate. As result, selectivity 62.5 % industrial-level current density 160 mA cm-2 at low potential -0.72 V were achieved. Our studies revealed isolated NiN3 active sites N species facilitated desorption massive intermediate released from Ni-SOD/NC then overflowed NPs enrich coverage improving ER .

Language: Английский

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