Reversed Spillover Effect Activated by Pt Atom Dimers Boosts Alkaline Hydrogen Evolution Reaction

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(45)

Published: Aug. 30, 2023

Abstract The hydrogen spillover effect has garnered considerable attention as a promising avenue to enhance the activity of evolution reaction (HER) in metal‐support compound materials. Herein, Pt atom dimers on NiOOH support are successfully synthesized with reversed effect, demonstrating much better alkaline HER than single atoms and clusters. Atomic electronic structure characterizations unequivocally verify anchoring through Pt─O bonds, thus obtaining enhanced effect. Theoretical experimental results indicate that exhibits pronounced water dissociation capability, while dimers, comparison clusters, demonstrate superior desorption ability. leads remarkable solutions, evidenced by an ultra‐small overpotential 13 mV at 10 mA cm −2 . These findings not only provide insights into potential use for HER, but also shed light designing high‐performance catalysts.

Language: Английский

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Cost‐Effective High Entropy Core–Shell Fiber for Stable Oxygen Evolution Reaction at 2 A cm⁻²

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(50)

Published: Aug. 1, 2023

Abstract Exploring highly efficient oxygen evolution reaction (OER) electrocatalysts is important for industrial water electrolysis, especially under high current densities (>1 A cm −2 ). High‐entropy alloy (HEA) with surface OER activity and excellent electrical conductivity of the core an ideal route to improve catalytic activity. Herein, a combined theoretical experimental approach establish core–shell FeCoNiMoAl‐based HEA as promising electrocatalyst presented. Theoretical calculations structure analyses indicate crystalline–amorphous ( c–a ) heterostructure shell reduces electron transfer resistance generates more active sites, furthermore crystalline improves self‐supporting ability. electrodes demonstrate superior performance overpotential η 470 mV at 2 no apparent degradation even after 330 h continuous testing, notably, overall splitting stability than 120 2.06 V. The special achieves win–win strategy stability. These findings shed light on structural design present achieve electrolysis relevant energy conversion processes.

Language: Английский

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Atomically dispersed Cu coordinated Rh metallene arrays for simultaneously electrochemical aniline synthesis and biomass upgrading

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Sept. 14, 2023

Organic electrocatalytic conversion is an essential pathway for the green of low-cost organic compounds to high-value chemicals, which urgently demands development efficient electrocatalysts. Here, we report a Cu single-atom dispersed Rh metallene arrays on foam cathodic nitrobenzene electroreduction reaction and anodic methanol oxidation reaction. In coupled system, Cusingle-atom-Rh requires only low voltages 1.18 V reach current densities 100 mA cm-2 generating aniline formate, with up ~100% conversion/ selectivity over ~90% formate Faraday efficiency, achieving synthesis chemicals. Density functional theory calculations reveal electron effect between host catalytic mechanism. The synergistic H*-spillover can improve process reduce energy barrier process, thus enhancing activity target product selectivity.

Language: Английский

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In Situ Electrochemical Oxyanion Steering of Water Oxidation Electrocatalysts for Optimized Activity and Stability

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(24)

Published: May 4, 2023

Abstract Compared to traditional modulation by metal cations doping, oxyanions offer a higher possibility of mediating the performance electrocatalysts toward oxygen evolution reaction (OER) due their special polyanion configurations and large electronegativity. However, mechanism rules mediation remain poorly understood. Herein, an in situ electrochemical oxyanion (NO 3 − , PO 4 3− SO 2− or SeO ) steering strategy study variation OER for transition‐metal (TM = Ni, Fe, Co) hydroxide is reported. Electrocatalytic experiments indicate both activity stability oxyanion‐modified TM hydroxides follow order > NO . Electrochemical incorporation improves hydroxides. Conversely, doping significantly accelerates leaching thus impairs performance. Theoretical calculations reveal that simultaneously modulates TM‐O covalency TM‐3 d band centers, correlating with This research constructs oxyanion‐mediated rule designing high‐performance energy transformation.

Language: Английский

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Next-Generation Green Hydrogen: Progress and Perspective from Electricity, Catalyst to Electrolyte in Electrocatalytic Water Splitting

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

Published: July 5, 2024

Green hydrogen from electrolysis of water has attracted widespread attention as a renewable power source. Among several production methods, it become the most promising technology. However, there is no large-scale system currently that can compete with conventional fossil fuel production. Renewable energy electrocatalytic splitting an ideal technology environmental cleanliness protection and good purity, which meet requirements future development. This review summarizes introduces current status by three aspects: electricity, catalyst electrolyte. In particular, present situation latest progress key sources power, catalytic materials electrolyzers for are introduced. Finally, problems generation electrolytic directions next-generation green in discussed outlooked. It expected this will have important impact on field water.

Language: Английский

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Tailoring Nanocrystalline/Amorphous Interfaces to Enhance Oxygen Evolution Reaction Performance for FeNi‐Based Alloy Fibers

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 6, 2024

Abstract Efficient oxygen evolution reaction (OER) electrocatalysts play a pivotal role in water electrolysis, notably for industrial high current densities (>1000 mA cm −2 ). Crystalline/amorphous heterostructure interfaces have proven to be advantageous enhancing the OER activities of electrocatalytic materials. However, constructing and tailoring crystalline/amorphous still remain great challenge due destruction active substrates by intricate post‐treatment. Here, strategy tailor nanocrystalline/amorphous (N/A) interface optimize performance as‐cast N/A alloys adjusting size nanocrystals is proposed. The alloy fibers obtained based on this exhibit superior with an overpotential 227 mV (@10 ), maintaining stability over 1000, 600, 240 h under 500, 1800 , respectively. Theoretical calculations material characterizations reveal that interfaces, facilitated appropriately sized possessing loose atomic arrangement, favorable surface electronic structure, local coordination, optimal O‐contained intermediate adsorption, can yield abundant sites without compromising stability. This study not only provides deeper understanding mechanism but also offers new design perspective development cost‐effective, industrial‐grade electrocatalysts.

Language: Английский

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Ruthenium‐Based Electrocatalysts for Hydrogen Evolution Reaction: from Nanoparticles to Single Atoms

Small, Journal Year: 2024, Volume and Issue: 20(45)

Published: July 27, 2024

Abstract Benefiting from similar hydrogen bonding energy to Pt and much lower price compare with Pt, Ru based catalysts are promising candidates for electrocatalytic evolution reaction (HER). The catalytic activity of nanoparticles can be enhanced through improving their dispersion by using different supports, the strong metal supports interaction further regulate performance. In addition, single‐atom (SACs) almost 100% atomic utilization attract great attention coordinative atmosphere single atoms adjusted supports. Moreover, syngenetic effects improve performance catalysts. this review, progress HER electrocatalysts summarized according existing forms, including (NPs), (SAs) combination both NPs SAs. common such as carbon materials, oxides, phosphides sulfides classified clarify active centers. Especially, possible mechanisms reasons improved discussed experimental results theoretical calculations. Finally, some challenges opportunities prospected facilitate development HER.

Language: Английский

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Experimental Demonstration of Topological Catalysis for CO₂ Electroreduction

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(10), P. 6536 - 6543

Published: Feb. 27, 2024

The past decade has witnessed substantial progress in understanding nontrivial band topology and discovering exotic topological materials condensed-matter physics. Recently, physics been further extended to the chemistry discipline, leading emergence of catalysis. In principle, effect is detectable catalytic reactions, but no conclusive evidence reported yet. Herein, by precisely manipulating surface state (TSS) Bi2Se3 nanosheets through thickness control application a magnetic field, we provide direct experimental illustrate catalysis for CO2 electroreduction. With without cooperation TSS, mainly reduced into liquid fuels (HCOOH H2C2O4) CO, exhibiting high (up 90% at −1.1 V versus reversible hydrogen electrode) low Faradaic efficiency (FE), respectively. Theoretically, product FE difference can be attributed TSS-regulated adsorption key intermediates barrier potential-determining step. Our work demonstrates inherent correlation between electrocatalysis, paving new avenue designing high-performance catalysts.

Language: Английский

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Catalytic Mechanism of Nanocrystalline and Amorphous Matrix in Fe‐Based Microwires for Advanced Oxidation

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

Published: Feb. 24, 2025

Abstract The sustainable management of water resources is a critical global challenge, with advanced oxidation processes emerging as promising solution for addressing environmental pollution. However, the clear trade‐off between catalytic activity and stability in existing catalysts hinders their broader application. In this study, nanocrystalline/amorphous (N/A) microwire catalyst developed, featuring design that regulates nanocrystal size while preserving pure amorphous matrix. Unlike brittle annealed N/A microwires subjected to structural relaxation, as‐cast demonstrate outstanding performance oxidation. They can completely degrade pollutants within 60 s maintain up 40 reuse cycles. Theoretical calculations material characterizations reveal exceptional properties arise from combined effects residual stresses stored matrix synergistic effect nanocrystals phases. Moreover, optimally sized nanocrystalline phase optimizes atomic arrangement induces an structure low coordination number, providing abundant active sites. This also enhances adsorption characteristics persulfate accelerates electron transfer. These findings offer novel framework developing efficient stable wastewater treatment.

Language: Английский

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Nanoalloys Composed of Platinum Group Metals and p‐Block Elements for Innovative Catalysis

Advanced Energy and Sustainability Research, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 14, 2025

Alloy nanoparticles based on platinum group metals (PGMs) have been intensively investigated in various fields, especially catalysis. Recently, the scope of alloying has expanded to include not only d‐block transition but also p‐block elements, which a wide range properties that are very different from those metals. By PGMs with electronic structure and surface catalysts can be tuned, enhancing their catalytic performance. The focus this review is PGM–p‐block element nanoalloys, synthesis methods, characterization techniques, properties. In addition typical binary crystalline alloys, such as solid‐solution intermetallic highlights potential multielement, amorphous, or liquid recently garnered much attention. aims provide valuable perspectives for development PGM‐based sustainable innovative catalysis, while addressing current challenges future directions field.

Language: Английский

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