Engineering Atom‐Scale Cascade Catalysis via Multi‐Active Site Collaboration for Ampere‐Level CO₂ Electroreduction to C₂₊ Products

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

Published: Jan. 15, 2025

Electrochemical reduction of CO2 to value-added multicarbon (C2+) productions offers an attractive route for renewable energy storage and utilization, but it remains challenging achieve high C2+ selectivity at industrial-level current density. Herein, a Mo1Cu single-atom alloy (SAA) catalyst is reported that displays remarkable Faradaic efficiency 86.4% under 0.80 A cm-2. Furthermore, the partial density over reaches 1.33 cm-2 with surpasses 74.3%. The combination operando spectroscopy functional theory (DFT) indicates as-prepared SAA enables atom-scale cascade catalysis via multi-active site collaboration. introduced Mo sites promote H2O dissociation fabricate active *H, meanwhile, Cu (Cu0) far from atom are activation toward CO. Further, CO *H captured by adjacent (Cu&+) near atom, accelerating conversion C─C coupling process. Our findings benefit design tandem electrocatalysts atomic scale transforming products rate.

Language: Английский

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Creating Bridged‐H* Bond Structure for Boosting Electrocatalytic Hydrogen Evolution via Phosphorus‐Doped Iridium Nanosheets

Small, Journal Year: 2025, Volume and Issue: 21(11)

Published: Feb. 11, 2025

Abstract Iridium (Ir) is recognized to have extremely high catalytic activity in the hydrogen evolution reaction (HER). However, there are still technical challenges maximizing utilization of Ir atoms process through dimensional regulation strategies. Herein, an innovative strategy utilized fabricate porous phosphorus‐doped iridium (P‐Ir) with a 2D structure, specifically reduction 1T phase‐IrO 2 (1T‐IrO ) nanosheets using phosphine gas. The optimized P‐Ir achieves overpotential 17.2 mV (vs RHE without i R‐correction) 0.5 m H SO 4 during HER process, outperforming benchmark Pt/C (27.0 mV) and most reported Ir‐based electrocatalysts. During long‐term stability tests, maintains stable operation for more than 100 h at both −10 −100 mA cm −2 , respectively. Moreover, transient potential scanning results phosphides prove that doping P lattice promotes kinetic rate charge transport capacity evolution. Theoretical calculations reveal weakens adsorption energy intermediates (H*) by regulating d ‐band center sites. Simultaneously, desorption H* also facilitated forming special bridged‐H* bond eventually accelerating kinetics.

Language: Английский

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Promoting Efficient Ruthenium Sites With Lewis Acid Oxide for the Accelerated Hydrogen and Chlor‐Alkali Co‐Production

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

Published: Feb. 21, 2025

Abstract Ruthenium (Ru) –based catalysts have been considered a promising candidate for efficient sustainable hydrogen and chlor‐alkali co‐production. Theoretical calculations disclosed that the hollow sites on Ru surface strong adsorption energies of H Cl species, which inevitably leads to poor activity cathodic evolution reaction (HER) anodic chlorine (CER), respectively. Furthermore, it confirmed anchoring Lewis acid oxide nanoparticles such as MgO can induce formation onion‐like charge distribution atoms around nanoparticles, thereby exposing Ru‐bridge at interface excellent accelerate both HER CER. Under guidance theoretical calculations, novel dispersed (MgO x ‐Ru) electrocatalyst is successfully prepared. In strongly alkaline saline media, ‐Ru recorded CER electrocatalytic with very low overpotential 19 mV 74 current density 10 mA cm −2 , More stirringly, electrochemical test electrodes under simulated electrolysis conditions demonstrated superior performance industrial commercial 20 wt% Pt/C dimensionally stable anode (DSA).

Language: Английский

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MXene‐Supported Single‐Atom Electrocatalysts

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

Published: March 27, 2025

MXenes, a novel member of the 2D material family, shows promising potential in stabilizing isolated atoms and maximizing atom utilization efficiency for catalytic applications. This review focuses on role MXenes as support single-atom catalysts (SACs) various electrochemical reactions, namely hydrogen evolution reaction (HER), oxygen (OER), reduction (ORR), carbon dioxide (CO2RR), nitrogen (NRR). First, state-of-the-art characterization synthesis methods MXene-supported SACs are discussed, highlighting how unique structure tunable functional groups enhance performance pristine contribute to SAs. Then, recent studies different electrocatalytic areas examined, including experimental theoretical studies. Finally, this discusses challenges outlook field electrocatalysis.

Language: Английский

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Lamellar Nanoporous Intermetallic Cobalt-Titanium Multisite Electrocatalyst with Extraordinary Activity and Durability for the Hydrogen Evolution Reaction

Nano Letters, Journal Year: 2025, Volume and Issue: unknown

Published: April 1, 2025

Constructing well-defined multisites with high activity and durability is crucial for the development of highly efficient electrocatalysts toward multiple-intermediate reactions. Here we report negative mixing enthalpy caused intermetallic cobalt-titanium (Co3Ti) nanoprecipitates on a lamellar hierarchical nanoporous cobalt skeleton as high-performance nonprecious multisite electrocatalyst an alkaline hydrogen evolution reaction. The Co3Ti robust substantially boosts reaction kinetics water dissociation adsorption/combination by unisonous adsorptions hydroxyl intermediates proper binding energies. By virtue bicontinuous that enables sufficiently accessible facilitates electron transfer ion/molecule transportation, self-supported heterogeneous electrode exhibits extraordinary electrocatalytic in 1 M KOH. It reaches current density ∼3.31 A cm–2 at low overpotential 200 mV maintains exceptional stability ∼1.33 >1000 h.

Language: Английский

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Microwave quasi-solid-state-constructed low-content Pt on CeO₂ with strong electronic interactions for efficient electrocatalytic acidic overall water splitting

Inorganic Chemistry Frontiers, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Pt-loaded CeO 2 cubes were designed via a rapid and eco-friendly ultrafast microwave quasi-solid-state approach within 60 s, which exhibited low overpotential of 10 mV to reach mA cm −2 in 0.5 M H SO 4 with excellent long-term stability.

Language: Английский

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Noble Metal Nanoparticles Anchored on Transition Metal Phosphides for Effective pH‐Universal Hydrogen Evolution

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

Published: April 30, 2025

Constructing electrocatalysts with high activity and low precious metal content is essential for achieving efficient hydrogen production in pH-universal overall water splitting. Herein, five types of noble anchored transition phosphides are analyzed by theoretical derivation. Based on the calculation results, a suitable hybrid screened out Pt nanoparticles CoP nanowires (Pt─CoP) via robust Pt─P─Co bonds. This strong synergy between through interfacial bonds optimizes adsorption key intermediates evolution reaction (HER) wide pH range from 0 to 14. Furthermore, interaction accompanied delicate structure reduces charge transfer resistance, creates abundant active sites, enhances catalyst durability, while facilitating site exposure electron/mass during HER process. Accordingly, synthesized Pt─CoP exhibits overpotentials 79, 26, 18 mV at 10 mA cm-2 acidic, neutral, alkaline media HER, respectively, superior commercial Pt/C benchmarks most reported electrocatalysts. work paves new clue exploit low-Pt-loading HER.

Language: Английский

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Enhanced pH-universal hydrogen evolution reactions on the Rh/MoO3 electrocatalysts

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 163260 - 163260

Published: April 1, 2025

Language: Английский

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Synergistic Effect of Mo Doping and Oxygen Vacancies to Enhance the Her Catalytic Performance of Ruo2

Published: Jan. 1, 2025

Language: Английский

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Strain-induced water reorientation for enhanced alkaline hydrogen evolution reaction

International Journal of Hydrogen Energy, Journal Year: 2025, Volume and Issue: 111, P. 33 - 39

Published: Feb. 24, 2025

Language: Английский

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