Hydrogen spillover effect tuning the rate-determining step of hydrogen evolution over Pd/Ir hetero-metallene for industry-level current density

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 352, P. 124047 - 124047

Published: April 21, 2024

Language: Английский

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Electric Field Redistribution Triggered Surface Adsorption and Mass Transfer to Boost Electrocatalytic Glycerol Upgrading Coupled with Hydrogen Evolution

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(29)

Published: May 5, 2024

Abstract Electrocatalytic glycerol oxidation reaction (GOR) stands out as an economical and prospective technology to replace oxygen evolution for co‐producing high‐valued chemicals hydrogen (H 2 ). Regulating the adsorption of (GLY) hydroxyl (OH) species is great significance improving GOR performance. Herein, a hierarchical p–n heterojunction by combining Co‐metal organic framework (MOF) nanosheets with CuO nanorod arrays (CuO@Co‐MOF) developed realize optimization on GOR. Specifically, CuO@Co‐MOF electrode exhibits superior performance conversion 98.4%, formic acid (FA) selectivity 87.3%, Faradaic efficiency (FE) 98.9%. The flow‐cell system bifunctional pairing (HER) reveals better energy efficiency. Experimental results theoretical calculations unravel redistributed electric field introducing Co‐containing that contribute improved performance, which not only enhances OH but also modulates excessive GLY CuO, thus reducing barriers FA desorption. Simultaneously, finite element analysis novelty structure can increase concentration − facilitate mass transfer in solution.

Language: Английский

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Defect-rich AuCu@Ag nanowires with exclusive strain effect accelerate nitrate reduction to ammonia

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 350, P. 123919 - 123919

Published: April 24, 2024

Language: Английский

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Superlattices in Ru Metallene Nanobelts for Robust Hydrogen Evolution

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

Published: Jan. 22, 2025

Abstract 2D materials, especially superlattices with tailored geometries, represent an emerging class of promising electrocatalysts for sustainable energy conversion. However, the development has been largely confined to self‐assembled layered structures, and it remains a great challenge rationally design distances between neighboring metal sites at atomic level match adsorption configurations key species in target reaction pathways. In this work, general strategy is reported synthesizing Ru metallene nanobelts (Ru‐ene) in‐plane using molten salts as space‐confined growth templates. The fabricated Ru‐ene consist atom pairs separated by atomic‐level distance periodicity 0.32 nm high density active sites. Both experiments DFT calculations show that structure enhances H 2 O accelerates desorption H*. exhibits excellent hydrogen evolution (HER) performance small overpotential ( η 10 = 50 mV), low Tafel slope (42.38 mV dec −1 ), well good long‐term stability. This work not only provides new method constructing but also establishes intrinsic mechanistic correlation distance, Δ G H* H‐adsorption, HER performance.

Language: Английский

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One‐Pot Synthesis Inorganic–Organic Hybrid PdNi Bimetallenes for PET Electrocatalytic Value‐Added Transformation

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

Published: Feb. 27, 2024

Abstract Progress is made in the advancement of efficient and durable electrocatalysts for ethylene glycol oxidation reaction (EGOR), which a critical breakthrough conversion waste plastic into high‐value‐added chemicals. Here, an organic ligand‐modified PdNi bimetallenes (PdNi O‐BMs) catalyst designed constructed through one‐pot method. Benefiting from frizzy porous surface structure inorganic–organic hybrid interface modification, O‐BMs undergo electrocatalytic reforming (EG) derived polyethylene terephthalate (PET) to form formic acid. The unique structural advantages result high EGOR performance. Meanwhile, influence Ni ligand on performance confirmed density functional theory calculations. This study reveals advanced strategy synthesis bimetallenes, providing green sustainable new approach PET value‐added transformation.

Language: Английский

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Electrocatalytic upcycling of plastic waste: Progress, challenges, and future

Electron, Journal Year: 2024, Volume and Issue: 2(3)

Published: Aug. 1, 2024

Abstract The escalating accumulation of plastic waste has been developed into a formidable global environmental challenge. Traditional disposal methods such as landfilling and incineration not only exacerbate degradation by releasing harmful chemicals greenhouse gases, but also squander finite resources that could otherwise be recycled or repurposed. Upcycling is kind recycling technology converts high‐value helps to avoid resource pollution. Electrocatalytic upcycling emerges novel distinguished its mild operational conditions, high transformation efficiency product selectivity. This review commences with an overview the employed in management respective advantages inherent limitations are delineated. different types upcycled electrocatalytic strategy then discussed process examined together mechanisms underlying upcycling. Furthermore, structure‐activity relationships between electrocatalysts performance elucidated. aims furnish readers comprehensive understanding techniques for provide guidance design towards efficient transformation.

Language: Английский

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High‐Density Rare‐Earth Single‐Atom‐Triggered Unconventional Transition of Adsorption Configuration on La₁Pd Monatomic Alloy Metallene for Sustainable Electrocatalytic Alkynol Semi‐Hydrogenation

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(44)

Published: May 17, 2024

Abstract Electrocatalytic alkynol semi‐hydrogenation for the high‐value chemicals alkenol with mild conditions and carbon‐free emission is a potentially green sustainable alternative to conventional thermocatalytic routes, which generally involves design of electrocatalysts high activity selectivity. Here, rare‐earth single‐atom (Ln = La, Nd, Pr) coordinated Pd metallene 1 Pdene) reported electrocatalytic 2‐methyl‐3‐butyn‐2‐ol (MBY) reaction (MBY ESHR) synthesis 2‐methyl‐3‐buten‐2‐ol (MBE). Typically, in alkaline medium containing 0.1 m MBY, MBY conversion MBE selectivity La Pdene are as ≈97% ≈95%, respectively, excellent stability. Meanwhile, situ infrared spectra reveal during dynamic process. Theoretical calculations that interaction between host triggers an unconventional transformation intermediate MBE* adsorption configuration hydrogenation, achieving optimal desorption energy target product optimizing barriers inhibit over‐hydrogenation MBE. Moreover, active site hydrogen supplier H 2 O effectively reduces competition reactants O, rendering synergistic co‐catalytic sites promote reaction.

Language: Английский

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Evaluating the impact of anodic oxidation reactions on water splitting using Prussian blue analog-derived metal-(oxy)hydroxides

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(30), P. 19321 - 19330

Published: Jan. 1, 2024

Prussian blue analog (PBA)-derived Fe–Co(O)OH showed improved anodic oxidation of a series organic and inorganic compounds without the interference from oxygen evolution reaction.

Language: Английский

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Amorphous Ni(OH)₂ Coated Cu Dendrites with Superaerophobic Interface for Bipolar Hydrogen Production Assisted with Formaldehyde Oxidation

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 13, 2025

Abstract Since formaldehyde oxidation reaction (FOR) can release H 2 , it is attractive to construct a bipolar hydrogen production system consisting of FOR and evolution (HER). Although copper‐based catalysts have attracted much attention due their low cost high activity, the performance enhancement mechanism lacks in‐depth investigation. Here, an amorphous‐crystalline catalyst amorphous nickel hydroxide‐coated copper dendrites on foam (Cu@Ni(OH) /CF) prepared. The modification Ni(OH) resulted in hydrophilic aerophobic states Cu@Ni(OH) /CF surface, facilitating transport liquid‐phase species electrode surface accelerating . Open circuit potential (OCP) density functional theory (DFT) calculations indicate that this core–shell structure facilitates adsorption HCHO OH − In addition, catalytic pathway are investigated through situ FTIR DFT calculations, results showed lowered energy barrier for C─H bond breaking H─H formation. HER//FOR system, Pt/C//Cu@Ni(OH) provide current 0.5 A cm −2 at 0.36 V achieve efficient stable production. This work offers new ideas designing electrocatalysts assisted with oxidation.

Language: Английский

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Self‐assembled Gap‐Rich PdMn Nanofibers with High Mass/Electron Transport Highways for Electrocatalytic Reforming of Waste Plastics

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

Published: Jan. 28, 2025

Abstract Innovating nanocatalysts with both high intrinsic catalytic activity and selectivity is crucial for multi‐electron reactions, however, their low mass/electron transport at industrial‐level currents often overlooked, which usually leads to comprehensive performance the device level. Herein, a Cl − /O 2 etching‐assisted self‐assembly strategy reported synthesizing self‐assembled gap‐rich PdMn nanofibers highway greatly enhancing electrocatalytic reforming of waste plastics currents. The nanofiber shows excellent in upcycling into glycolic acid, current density 223 mA cm −2 @0.75 V ( vs RHE), (95.6%), Faraday efficiency (94.3%) acid flow electrolyzer. Density functional theory calculation, X‐ray absorption spectroscopy combined situ electrochemical Fourier transform infrared reveals that introduction highly oxophilic Mn induces downshift d ‐band center Pd, optimizes adsorption energy reaction intermediates on surface, thereby facilitating desorption as high‐value product. Computational fluid dynamics simulations confirm structure conducive mass transfer deliver an current.

Language: Английский

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