Active Hydroxyl‐Mediated Preferential Cleavage of Carbon‐Carbon Bonds in Electrocatalytic Glycerol Oxidation

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 8, 2025

Electrocatalytic glycerol oxidation reaction (GOR) to produce high-value formic acid (FA) is hindered by high formation potential of active species and sluggish C-C bond cleavage kinetics. Herein, Ni single-atom (NiSA) Co (CoSA) dual sites anchored on nitrogen-doped carbon nanotubes embedded with Ni0.1Co0.9 alloy (Ni0.1Co0.9@NiSACoSA-NCNTs) are constructed for electrochemical GOR. Remarkably, it can reach 10 mA cm-2 at a low 1.15 V versus the reversible hydrogen electrode (vs. RHE) realize formate selectivity 93.27 % even conversion 98.81 1.45 vs. RHE. The GOR mechanism pathway systematically elucidated via experimental analyses theoretical calculations. It revealed that hydroxyl (*OH) be produced during NiSA, CoSA, synergistically optimizes electronic structure CoSA sites, reducing energy barriers *OH-mediated bonds dehydrogenation C1 intermediates. This decreases number intermediates steps GOR-to-FA, thus increasing production efficiency. After coupling evolution in membrane assembly cell, 14.26 g 23.10 L H2 100 108 h.

Language: Английский

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Hollow Mo/MoS_Vn Nanoreactors with Tunable Built‐in Electric Fields for Sustainable Hydrogen Production

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

Published: Dec. 8, 2024

Abstract Constructing built‐in electric field (BIEF) in heterojunction catalyst is an effective way to optimize adsorption/desorption of reaction intermediates, while its precise tailor achieve efficient bifunctional electrocatalysis remains great challenge. Herein, the hollow Mo/MoS Vn nanoreactors with tunable BIEFs are elaborately prepared simultaneously promote hydrogen evolution (HER) and urea oxidation (UOR) for sustainable production. The BIEF induced by sulfur vacancies can be modulated from 0.79 0.57 0.42 mV nm −1 , exhibits a parabola‐shaped relationship HER UOR activities, V1 nanoreactor moderate presents best activity. Theoretical calculations reveal that evidently facilitate breakage N─H bond UOR. electrolyzer assembled delivers cell voltage 1.49 V at 100 mA cm −2 which 437 lower than traditional water electrolysis, also excellent durability 200 h. Life cycle assessment indicates HER||UOR system possesses notable superiority across various environment impact energy consumption. This work provide theoretical experimental direction on rational design advanced materials energy‐saving eco‐friendly

Language: Английский

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Metal–organic frameworks (MOFs) for hybrid water electrolysis: structure–property–performance correlation

Chemical Communications, Journal Year: 2024, Volume and Issue: 60(62), P. 8020 - 8038

Published: Jan. 1, 2024

Structure–property–performance correlation of MOFs for various AORs in hybrid water electrolysis.

Language: Английский

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Interface engineering of hollow Janus-structured NiCoP/P-MoS2 heterojunction as self-supported electrode enables boosted alkaline hydrogen evolution reaction

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 684, P. 668 - 677

Published: Jan. 11, 2025

Language: Английский

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Aerophobic/Hydrophilic Nickel–Iron Sulfide Nanoarrays for Energy-Saving Hydrogen Production from Seawater Splitting Assisted by Sulfion Oxidation Reaction

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(38), P. 17662 - 17671

Published: Sept. 6, 2024

Electrolysis of infinite seawater is a promising and sustainable approach for clean hydrogen production. However, it remains big challenge to accomplish corrosion-resistant chlorine-free electrolysis at low power input. Herein, the bimetallic nickel-iron sulfide-based electrocatalytic nanoarrays are constructed by facile hydrothermal sulfidation redox-etched iron foam (IF), which manifests an effective reliable strategy sulfion oxidation reaction (SOR) assist alkaline achievement energy-saving production value-added upcycling. The resulting NiFeS

Language: Английский

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NiFe-Prussian blue analogs catalyst for glucose electrolytic hydrogen production and biomass valorization

International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 86, P. 511 - 518

Published: Aug. 31, 2024

Language: Английский

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Hierarchically Structured CuNiP/CuO_x‐V_P Nanoarrays Construction by Heteroatom Doping Boosting Glycerol Valorization at Industrial‐Level Current Density

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

Published: Oct. 13, 2024

Abstract Electrocatalytic valorization of glycerol to formate is considered be a promising sustainable approach; however, it holds great challenges increase catalyst activity and deliver market‐demanded chemicals with high Faradaic efficiency (FE) selectivity under industrial‐level current density. Herein, hierarchically structured phosphorus vacancy‐enriched nickel phosphide porous nanoarrays by copper doping, denoted as CuNiP/CuO x ‐V P , are constructed via facile glycol‐mediated solvothermal approach. The yields an industry‐level 1 A cm −2 at the ultralow potential 1.75 V, while showing notable FE (96.94%) (96.76%) over wide range potentials. Impressively, two‐electrode electrolyzer linked H 2 evolution possesses exceptional that merely requires cell voltage 1.45 V 40 mA exhibiting (97.53%) for production surpassing vast majority previously reported precious metal electrocatalysts. Microscopic electrochemical characterizations manifest composed NiP nanosheets attached aggregated CuO particles featuring superaerophobic‐hydrophilic morphology enables increased active sites, favorable electronic redistribution, thus boosted electrocatalytic performance. This study demonstrates effective electrode discovery, going from synthesis structure‐activity relationship subsequently developing more highly electrocatalysts energy‐saving coproduction valuable chemicals.

Language: Английский

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High-valence molybdenum doped Ni(OH)2 nanosheets enhancing hydrogen production and glycerol oxidation to formic acid

International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 1, 2024

Language: Английский

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Self-Powered Energy-Efficient Electrochemical Nitrite Reduction Coupled with Sulfion Oxidation for Ammonia Synthesis and Sulfur Recovery over Hierarchical Cobalt Sulfide Nanostructures

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: unknown, P. 124991 - 124991

Published: Dec. 1, 2024

Language: Английский

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Active Hydroxyl‐Mediated Preferential Cleavage of Carbon‐Carbon Bonds in Electrocatalytic Glycerol Oxidation

Angewandte Chemie, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 8, 2025

Abstract Electrocatalytic glycerol oxidation reaction (GOR) to produce high‐value formic acid (FA) is hindered by high formation potential of active species and sluggish C−C bond cleavage kinetics. Herein, Ni single‐atom (Ni SA ) Co (Co dual sites anchored on nitrogen‐doped carbon nanotubes embedded with 0.1 0.9 alloy @Ni ‐NCNTs) are constructed for electrochemical GOR. Remarkably, it can reach 10 mA cm −2 at a low 1.15 V versus the reversible hydrogen electrode (vs. RHE) realize formate selectivity 93.27 % even conversion 98.81 1.45 vs. RHE. The GOR mechanism pathway systematically elucidated via experimental analyses theoretical calculations. It revealed that hydroxyl (*OH) be produced during , synergistically optimizes electronic structure sites, reducing energy barriers *OH‐mediated bonds dehydrogenation C 1 intermediates. This decreases number intermediates steps GOR‐to‐FA, thus increasing production efficiency. After coupling evolution in membrane assembly cell, 14.26 g 23.10 L H 2 100 108 h.

Language: Английский

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