Synergistic Cu/Cu2O/Co3O4 catalyst with crystalline-amorphous interfaces for efficient electrochemical nitrate reduction to ammonia

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: 507, P. 160393 - 160393

Published: Feb. 7, 2025

Language: Английский

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Recent advances and challenges of double-atom catalysts in diverse environmental applications: A state-of-the-art review

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 532, P. 216545 - 216545

Published: Feb. 19, 2025

Language: Английский

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Subnanometric Nickel Phosphide Heteroclusters with Highly Active Ni^δ+–P^δ− Pairs for Nitrate Reduction toward Ammonia

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: March 26, 2025

The development of efficient electrocatalysts for the neutral nitrate reduction reaction (NO3–RR) toward ammonia (NH3) is essential to address environmental issues caused by NO3– but remains considerably challenging owing sluggish kinetics NO3–RR in media. Herein, we report subnanometric heteroclusters with strongly coupled nickel–phosphorus (Ni–P) dual-active sites as boost NO3–RR. Experimental and theoretical results reveal that feature Ni–P promotes electron transfer from Ni P, generating Niδ+–Pδ− active pairs, which Niδ+ species are highly Pδ− tunes interfacial water hydrogen bonding network promote dissociation step accelerate proton during Consequently, NO3–RR, exhibit a large NH3 yield rate 0.61 mmol h–1 cm–2 at −0.8 V versus reversible electrode, 2.8- 3.3-fold larger than those on nanoparticles clusters, respectively, generated exists NH4+ electrolytes. This study offers an approach boosting electrocatalytic reactions multiple intermediates designing sites.

Language: Английский

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Metal-organic framework-derived diatomic catalysts for environmental remediation: Synthesis, applications and improvement strategies

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 526, P. 216357 - 216357

Published: Nov. 29, 2024

Language: Английский

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Balancing Electronic Spin State via Atomically-Dispersed Heteronuclear Fe–Co Pairs for High-Performance Sodium–Sulfur Batteries

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 27, 2025

Room-temperature sodium–sulfur (Na–S) batteries are emerging as a promising next-generation energy storage technology, offering high densities at low cost and utilizing abundant elements. However, their practical application is hindered by the shuttle effect of sodium-polysulfides sluggish kinetics sulfur redox reactions. In this study, we demonstrate heteronuclear diatomic catalyst featuring Fe Co bimetallic sites embedded in nitrogen-doped hollow carbon nanospheres (Fe–Co/NC) an effective host cathode Na–S batteries. Aberration-corrected high-angle annular dark field scanning transmission electron microscopy demonstrates presence isolated Fe–Co atomic pairs, while synchrotron radiation X-ray absorption fine structure analysis confirms (Fe–Co–N6) coordination structure. Density functional theory calculations show that introduction atoms induces delocalization Co(II), shifting electronic configuration from low-spin to higher-spin state. This shift enhances hybridization dz2 orbitals with antibonding π within sodium sulfide species accelerates catalytic conversion. As result, Fe–Co/NC-based cathodes exhibit excellent cycling stability (378 mAh g–1 after 2000 cycles) impressive rate performance (341.1 under 5 A g–1).

Language: Английский

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Tailoring asymmetric RuCu dual-atom electrocatalyst toward ammonia synthesis from nitrate

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: March 4, 2025

Atomically dispersed Ru-Cu dual-atom catalysts (DACs) with asymmetric coordination are critical for sustainable ammonia production via electrochemical nitrate reduction (NO3RR), but their rational synthesis remains challenging. Here, we report a pulsed discharge strategy that injects microsecond pulse current into ruthenium (Ru) and copper (Cu) precursors supported by nitrogen-doped graphene aerogels (NGA). The atomically Ru Cu dual atoms anchor onto nanopore defects of NGA (RuCu DAs/NGA) through explosive decomposition the metal salt nanocrystals. catalyst achieves 95.7% Faraday efficiency 3.1 mg h-1 cm-2 NH3 yield at -0.4 V vs. RHE. In situ studies reveal an RuN2-CuN3 active-site dynamic evolution during NO3RR. Density functional theory calculations demonstrate RuN2CuN3/C structure synergistically optimizes intermediate adsorption reduces energy barriers key steps. enables ultrafast various DACs (e.g., PtCu, AgCu, PdCu, FeCu, CoCu, NiCu) tailored environments, offering general-purpose precise preparation catalysts, which traditionally challenging to synthesize.

Language: Английский

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Structural Regulation Strategies of Atomic Cobalt Catalysts for Oxygen Electrocatalysis

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 3, 2025

Abstract Oxygen electrocatalysis is a core reaction in renewable energy devices, greatly promoting the transformation and upgrading of structure. Nonetheless, performance conversion devices hindered by large overpotential slow kinetics oxygen electrocatalytic reactions. Recently, single‐atom catalysts (SACs) have emerged as promising contenders field because their exceptional metal atom utilization, distinctive coordination environment, adjustable electronic properties. This review presents latest advancements design Co‐based SACs for electrocatalysis. First, OER ORR mechanisms are introduced. Subsequently, strategies regulating structure summarized three aspects, including centers, support carriers. A particular emphasis given to relationship between properties catalysts. Afterward, applications explored. Ultimately, challenges prospects prospected.

Language: Английский

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Recent Breakthroughs in Electrocatalytic Reduction of Nitrogen-Oxyanions for Environmentally Benign Ammonia Synthesis

Nano Energy, Journal Year: 2025, Volume and Issue: unknown, P. 110683 - 110683

Published: Jan. 1, 2025

Language: Английский

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Alloy Catalysts for Electrochemical Nitrate Reduction to Ammonia

ChemElectroChem, Journal Year: 2025, Volume and Issue: 12(4)

Published: Jan. 31, 2025

Abstract Electrochemical nitrate reduction reaction (NO 3 − RR) represents a promising ammonia (NH ) production approach and has garnered significant attention in recent years. Owing to the highly tunable electronic structures physicochemical properties, alloy materials have emerged as efficient catalysts for electrochemical NO RR. This review systematically examines advancements including binary alloys multi‐metal RR, comprehensively analyzing their structure, catalytic activity, mechanisms In addition, relationship between catalysts′ composition, active sites, activity are described, aiming elucidate underlying principles high guide rational design of future catalysts. Finally, this addresses challenges proposes directions research development.

Language: Английский

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Maximizing Available Active Hydrogen on FeNi Substitutional Solid-Solution Alloy to Boost Electrosynthesis of Ammonia from Nitrate

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

Published: Feb. 20, 2025

Electrochemical nitrate reduction reaction (NO3RR) stands out as a promising route for sustainable ammonia synthesis, in which active hydrogen (*H) plays crucial role both the deoxygenation and hydrogenation steps. However, regulation of surface *H is still overlooked, without intervention, competing evolution kinetically more favored over NO3RR, leaving current system far from satisfactory. Herein, based on reverse utilization Sabatier principle, series FexNiy substitutional solid-solution alloys (SSAs) are synthesized to manipulate behavior enhanced NO3RR. Upon precise optimization alloy composition, d-band center HER-active Ni shifts toward Fermi level, endowing catalyst with strong interaction greatly prolonging its lifetime, enables abundant supply facilitate As expected, maximum NH3 yield rate 31.46 mmol h-1 mg-1 delivered optimized Fe3Ni1-SSA, considerably higher than most extensively reported works. Several situ characterizations combined gain in-depth insight. Especially, Fourier transform infrared spectroscopy internal reflection mode directly observes enrichment surface, while accompanied facilitation NO3RR process verified by external mode.

Language: Английский

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