Phosphorus–tungsten dual-doping boosts acidic overall seawater splitting performance over RuO_x nanocrystals

Journal of Materials Chemistry A, Год журнала: 2024, Номер 12(41), С. 28023 - 28031

Опубликована: Янв. 1, 2024

Dual-doped ruthenium-based nanocrystals were developed as efficient and stable electrocatalysts for acidic overall seawater splitting with superior activity durability.

Язык: Английский

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Progress and challenges in nitrous oxide decomposition and valorization

Chemical Society Reviews, Год журнала: 2024, Номер 53(16), С. 8379 - 8423

Опубликована: Янв. 1, 2024

Nitrous oxide (N

Язык: Английский

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Electrochemical Cycling of Liquid Organic Hydrogen Carriers as a Sustainable Approach for Hydrogen Storage and Transportation

ACS Sustainable Chemistry & Engineering, Год журнала: 2025, Номер unknown

Опубликована: Янв. 14, 2025

Hydrogen (H2), as a high-energy-density molecule, offers clean solution to carry energy. However, the high diffusivity and low volumetric density of H2 pose challenge for long-term storage transportation. Liquid organic hydrogen carriers (LOHCs) have been suggested strategic way store transport in stable molecules. More so, electrochemical LOHC cycling renders an opportunity utilize renewable energy transportation toward goal eliminating carbon emissions. In this Perspective, examples reactions molecules their suitability couples are examined. A comparative footprint assessment processes against thermochemical hybrid was performed. The process had lowest relative only when highly concentrated LOHCs were used feed or purification product not required. diluted primarily contributed by distillation separation process. sensitivity analysis showed concentration dependence during Moreover, electrolyte composition significantly affects cycling. Energy utilization, water usage, toxicity discussed provide overview better economic environmental practices. There significant opportunities if appropriate conditions such concentrations reactant, reversible redox ability, Faradaic efficiencies, catalyst stabilities achieved.

Язык: Английский

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Sustainable Adipic Acid Production via Paired Electrolysis of Lignin-Derived Phenolic Compounds with Water as Hydrogen and Oxygen Sources

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(22), С. 15275 - 15285

Опубликована: Май 24, 2024

Adipic acid (AA) is an important feedstock for nylon polymers and industrially produced from fossil-derived aromatics via thermocatalysis. However, this process consumes explosive H2 corrosive HNO3 as reductants oxidants, respectively. Here, we report the direct synthesis of AA lignin-derived phenolic compounds paired electrolysis using bimetallic cooperative catalysts. At cathode, phenol hydrogenated on PtAu catalysts to form ketone-alcohol (KA) oil with 92% yield 43% Faradaic efficiency (FE). anode, KA electrooxidized into CuCo2O4 catalysts, achieving a maximum 85% 84% FE. Experimental theoretical studies reveal that excellent catalytic activity can be ascribed enhanced absorption activation capability reactants A two-electrode flow electrolyzer realizes stable at 2.5 over 200 h well 38.5% 70.2% selectivity. This study offers green sustainable route lignin electrolysis.

Язык: Английский

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Alloying and confinement effects on hierarchically nanoporous CuAu for efficient electrocatalytic semi-hydrogenation of terminal alkynes

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Июль 17, 2024

Abstract Electrocatalytic alkynes semi-hydrogenation to produce alkenes with high yield and Faradaic efficiency remains technically challenging because of kinetically favorable hydrogen evolution reaction over-hydrogenation. Here, we propose a hierarchically nanoporous Cu 50 Au alloy improve electrocatalytic performance toward alkynes. Using Operando X-ray absorption spectroscopy density functional theory calculations, find that modulate the electronic structure Cu, which could intrinsically inhibit combination H* form H 2 weaken alkene adsorption, thus promoting alkyne hampering Finite element method simulations experimental results unveil catalysts induce local microenvironment abundant K + cations by enhancing electric field within nanopore, accelerating water electrolysis more H*, thereby conversion As result, electrocatalyst achieves highly efficient 94% conversion, 100% selectivity, 92% over wide potential window. This work provides general guidance rational design for high-performance transfer catalysts.

Язык: Английский

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Cluster-Level Heterostructure of PMo₁₂/Cu for Efficient and Selective Electrocatalytic Hydrogenation of High-Concentration 5-Hydroxymethylfurfural

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(36), С. 25125 - 25136

Опубликована: Авг. 7, 2024

Electrochemical hydrogenation of aldehyde molecules, exemplified by 5-hydroxymethylfurfural (HMF), offers a sustainable approach for synthesizing higher value-added alcohols. However, severe coupling side reactions impede its practical implementation at high concentrations. In this work, cluster-level heterostructure PMo

Язык: Английский

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Electrochemical Nickel‐Catalyzed Hydrogenation

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(22)

Опубликована: Март 20, 2024

Olefin hydrogenation is one of the most important transformations in organic synthesis. Electrochemical transition metal-catalyzed an attractive approach to replace dangerous hydrogen gas with electrons and protons. However, this reaction poses major challenges due rapid evolution (HER) metal-hydride species that outcompetes alkene step, facile deposition metal catalyst at electrode stalls reaction. Here we report economical efficient strategy achieve high selectivity for reactivity over well-established HER. Using inexpensive bench-stable nickel salt as catalyst, mild features outstanding substrate generality functional group compatibility, distinct chemoselectivity. In addition, hydrodebromination alkyl aryl bromides could be realized using same system a different ligand, chemoselectivity between achieved through ligand selection. The practicability our method has been demonstrated by success large-scale synthesis catalytic amount electrolyte minimal solvent. Cyclic voltammetry kinetic studies were performed, which support Ni

Язык: 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, Год журнала: 2024, Номер 34(44)

Опубликована: Май 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.

Язык: Английский

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Substrate Diffusion Electrodes allow for the electrochemical hydrogenation of concentrated alkynol substrate feeds

iScience, Год журнала: 2025, Номер 28(2), С. 111789 - 111789

Опубликована: Янв. 10, 2025

Electrosynthesis has the potential to revolutionize industrial organic synthesis sustainably and efficiently. However, high cell voltages low stability often arise due solubility issues with solvents, while protic electrolytes restrict substrate options. We present a three-layered electrode design that enables use of concentrated neat feeds. This separates from aqueous electrolyte using layers varying porosity hydrophilicity, ensuring precise reactant transport catalyst layer minimizing crossover. demonstrate its effectiveness by semi-hydrogenating three alkynols different hydrophobicities. For semi-hydrogenation 3-methyl-1-pentyn-3-ol in pure form, we achieved 65% faradaic efficiency at 80 mA cm-2. Additionally, 2-methyl-3-butyn-2-ol on palladium showed for 36%, was stable 22 h. could be pioneering electrochemical valorization substrates, reducing need extensive downstream processing.

Язык: Английский

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In Situ Li⁺ Intercalation into Nanosized Chevrel Phase Mo₆S₈ toward Efficient Electrochemical Nitroarene Reduction

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Март 11, 2025

Electrochemical nitroarene reduction enables the green production of anilines at ambient conditions thanks to manipulated transfer multiple electrons and protons via controlling potentials currents, but challenges remain in pH-neutral electrolysis using nonprecious catalysts. Here, Chevrel phase Mo6S8 with high conductivity insertable frameworks is proposed for first time as a cost-efficient candidate prominent performance and, more importantly, new platform unravel cation effects on electroreduction. Nanosized derived from polymer-confined sulfidation affords yield (∼95%) Faradaic efficiency (∼99%) reducing 4-nitrostyrene 4-aminostyrene −0.45 V (vs RHE) 0.1 M LiClO4, outperforming series counterparts metal sulfides even noble metals. The combination experimental theoretical analyses identifies an intercalation-correlated effect, expanding current knowledge limited outer Helmholtz plane electrodes. In situ Li+ intercalation into cavities during ameliorates electronic configurations thereby promotes adsorption nitro group low-coordinated Mo sites hydrogenation proton-coupled electron mechanism. Furthermore, efficient electrosynthesis aniline derivatives conserved groups wide range substrates highlights promise electrochemical refinery.

Язык: Английский

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