Promoting Oxygen Reduction Reaction on Atomically Dispersed Fe Sites via Establishing Hydrogen Bonding with the Neighboring P Atoms

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 13(5)

Published: Dec. 16, 2022

Abstract Single atom catalysts (SACs) comprised of nitrogen‐coordinated transition metal (TM–N–C) moieties show encouraging performance towards the oxygen reduction reaction (ORR). Nevertheless, for reactions involving multiple intermediates, single‐atom sites fail to satisfactorily optimize adsorption all intermediates. Here, a facile strategy is reported construct Fe, P dual‐atom in multimodal porous carbon (Fe,P‐DAS@MPC), and its superiority synergistically boosting ORR demonstrated. Fe,P‐DAS@MPC exhibits excellent with substantially positive onset potential ( E = 1.02 V) half‐wave 1/2 0.92 V). Theoretical analysis unveils cooperative effect composed adjacent Fe atoms, aiding hydrogen bonding interaction can promote adsorption/desorption Additionally, Zn–air battery based on shows high peak power density exceptional cycling stability. These findings provide novel avenue design electrocatalysts practical energy conversion applications.

Language: Английский

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Research on cobalt-doping sites in g-C3N4 framework and photocatalytic reduction CO2 mechanism insights

Journal of Alloys and Compounds, Journal Year: 2023, Volume and Issue: 954, P. 170044 - 170044

Published: April 12, 2023

Language: Английский

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Interlayer Spacing Regulation by Single‐Atom Indium^δ+–N₄ on Carbon Nitride for Boosting CO₂/CO Photo‐Conversion

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(35)

Published: May 17, 2023

Abstract Simultaneous optimization on bulk photogenerated‐carrier separation and surface atomic arrangement of catalyst is crucial for reactivity CO 2 photo‐reduction. Rare studies capture the detail that, better than in‐plane regulation, interlayer‐spacing regulation may significantly influence carrier transport bulk‐catalyst thereby affecting its photo‐reduction in g ‐C 3 N 4 . Herein, through a single atom‐assisted thermal‐polymerization process, single‐atom In‐bonded N‐atom (In δ + –N ) (002) crystal planes originally constructed. This In reduces interplanar spacing by electrostatic adsorption, which enhances carriers greatly promotes photoreduction. The photo‐conversion performance this resulted modified superior to other atom loaded carbon nitride catalysts. Moreover, adsorption , *COOH formation energy, optimizes reaction path. It achieves remarkable 398.87 µmol −1 h yield rate, 0.21% apparent quantum efficiency, nearly 100% selectivity without any cocatalyst or sacrificial agent. Through d modulation atom, study provides ground‐breaking insight enhancement from double‐gain view structural control ‐reduction photocatalysts.

Language: Английский

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Visible-light-driven selective cleavage of C C bonds in lignin model substrates using carbon nitride-supported ruthenium single-atom catalyst

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 462, P. 142282 - 142282

Published: March 4, 2023

Language: Английский

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Atomic Distance Engineering in Metal Catalysts to Regulate Catalytic Performance

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(3)

Published: Oct. 2, 2023

Abstract It is very important to understand the structure–performance relationship of metal catalysts by adjusting microstructure at atomic scale. The distance has an essential influence on composition environment active atom, which a key factor for design targeted with desired function. In this review, we discuss and summarize strategies changing from three aspects relate their effects reactivity catalysts. First, regulating bond length between coordination atom one single‐atom site catalytic performance are introduced. lengths affected strain effect support high‐shell doping can evolve during reaction. Next, sites discussed. Due space matching adsorption electron transport, be adjusted shortening distance. addition, arrangement spacing surface atoms nanocatalysts studied. Finally, comprehensive summary outlook given.

Language: Английский

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Competitive Trapping of Single Atoms onto a Metal Carbide Surface

ACS Nano, Journal Year: 2023, Volume and Issue: 17(7), P. 6955 - 6965

Published: March 27, 2023

Controlling atomic adjustment of single-atom catalysts (SACs) can directly change its local configuration, regulate the energy barrier intermediates, and further optimize reaction pathways. Herein, we report an atom manipulating process to synthesize Ni atoms stabilized on vanadium carbide (NiSA-VC) through a nanofiber-medium thermodynamically driven migration strategy. Experimental theoretical results systematically reveal tunable pathway from nanoparticles neighboring N-doped carbon (NC) finally metal that was obtained by regulating competitive adsorption energies between VC NC for capturing atoms. For CO2-to-CO electroreduction, NiSA-VC exhibits industrial current density -180 mA cm-2 at -1.0 V vs reversible hydrogen electrode highest Faradaic efficiency CO production (FECO) 96.8% -0.4 RHE in flow cell. Significant electron transfers occurring structures contribute activation CO2, facilitate free energy, *CO desorption as rate-determining step, promote activity selectivity. This study provides understanding how design powerful SACs electrocatalysis.

Language: Английский

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Noble‐Metal‐Free Single‐ and Dual‐Atom Catalysts for Artificial Photosynthesis

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(22)

Published: May 13, 2023

Abstract Artificial photosynthesis enables direct solar‐to‐chemical energy conversion aimed at mitigating environmental pollution and producing solar fuels chemicals in a green sustainable approach, efficient, robust, low‐cost photocatalysts are the heart of artificial systems. As an emerging new class cocatalytic materials, single‐atom catalysts (SACs) dual‐atom (DACs) have received great deal current attention due to their maximal atom utilization unique photocatalytic properties, whereas noble‐metal‐free ones impart abundance, availability, cost‐effectiveness allowing for scalable implementation. This review outlines fundamental principles synthetic methods SACs DACs summarizes most recent advances (Co, Fe, Cu, Ni, Bi, Al, Sn, Er, La, Ba, etc.) (CuNi, FeCo, InCu, KNa, CoCo, CuCu, based on non‐noble metals, confined arsenal organic or inorganic substrates (polymeric carbon nitride, metal oxides, sulfides, metal–organic frameworks, carbon, acting as versatile scaffolds solar‐light‐driven reactions, including hydrogen evolution, dioxide reduction, methane conversion, synthesis, nitrogen fixation, peroxide production, remediation. The concludes with challenges, opportunities, future prospects photosynthesis.

Language: Английский

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Constructing FeNiPt@C Trifunctional Catalyst by High Spin‐Induced Water Oxidation Activity for Zn‐Air Battery and Anion Exchange Membrane Water Electrolyzer

Advanced Science, Journal Year: 2024, Volume and Issue: 11(19)

Published: March 14, 2024

Abstract Developing cost‐efficient trifunctional catalysts capable of facilitating hydrogen evolution reaction (HER), oxygen (OER), and reduction (ORR) activity is essential for the progression energy devices. Engineering these to optimize their active sites integrate them into a cohesive system presents significant challenge. This study introduces nanoflower (NFs)‐like carbon‐encapsulated FeNiPt nanoalloy catalyst (FeNiPt@C NFs), synthesized by substituting Co 2+ ions with high‐spin Fe in Hofmann‐type metal‐organic framework, followed carbonization pickling processes. The FeNiPt@C NFs catalyst, characterized its nitrogen‐doped metal alloy structure phase‐segregated slight surface oxidization, exhibits excellent catalytic performance. evidenced activities HER (−25 mV at 10 mA cm −2 ), ORR (half‐wave potential 0.93 V), OER (294 enhanced water oxidation attributed state element. Consequently, Zn‐air battery anion exchange membrane electrolyzer assembled demonstrate remarkable power density (168 mW ) industrial‐scale current (698 1.85 respectively. innovative integration multifunctional paves way advancement sustainable systems.

Language: Английский

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Precise Regulation of the Coordination Environment of Single Co(II) Sites in a Metal–Organic Framework for Boosting CO₂ Photoreduction

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(13), P. 8760 - 8769

Published: June 16, 2023

While the coordination environment around catalytic metal sites plays a crucial role in catalysis, its precise design and modulation still remain challenge. Herein, coordinated N atom number single Co installed on UiO-type metal–organic framework has been modulated to afford UiO-Co-Nx (x = 2, 3, 4) for photocatalytic CO2 reduction. Significantly, performance is affected by site, which UiO-Co-N3 exhibits superior activity other counterparts. Photo-/electrochemical results support fastest charge transfer kinetics between photosensitizer UiO-Co-N3. Theoretical calculations, together with acquired from situ diffuse reflectance infrared Fourier transform spectra, manifest lowest energy barriers of rate-determining step desorption CO* over among all samples.

Language: Английский

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Band engineering of non-metal modified polymeric carbon nitride with broad spectral response for enhancing photocatalytic CO2 reduction

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 461, P. 141841 - 141841

Published: Feb. 10, 2023

Language: Английский

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