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

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 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.

Язык: Английский

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Construction of Ru Single-Atom and Cluster/np-Mo synergistic active sites with hydrogen spillover for efficient hydrogen evolution reaction

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 161683 - 161683

Опубликована: Март 1, 2025

Язык: Английский

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MXene‐Supported Single‐Atom Electrocatalysts

Advanced Science, Год журнала: 2025, Номер unknown

Опубликована: Март 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.

Язык: Английский

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Constructing RuNi‐MoO₂ Heterojunction with Optimal Built‐In Electrical Field for Efficient Hydrogen Production in Anion Exchange Membrane Water Electrolyzer

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Дек. 15, 2024

Abstract Water electrolysis in alkaline media, demonstrating robust facility and cheap electrolyzer construction, are regarded as a promising strategy for industrial green hydrogen generation. Exploring effective evolution electrocatalysts is remained an obstacle to date, which requires additional effort obtain active by water dissociation promote the following unfavorable coupling further H 2 release. Herein, MoO supported RuNi nanoparticle (RuNi‐MoO ) constructed efficient electrocatalyst evolution. Experimental theoretical analysis demonstrate that optimized built‐in electric field at interface between alloy simultaneously accelerates kinetics spillover. It attains current densities of 10 100 mA cm −2 ultralow potential −0.019 −0.086 V versus RHE, respectively, along with rapid cleavage kinetics, even surpasses commercial Pt/C. The constructing anion exchange membrane adopting RuNi‐MoO cathode density 1 A low voltage 1.71 steadily operates over 1000 h large .

Язык: Английский

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

Опубликована: Янв. 1, 2025

Язык: Английский

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

Small, Год журнала: 2025, Номер 21(11)

Опубликована: Фев. 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.

Язык: Английский

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

Small, Год журнала: 2025, Номер unknown

Опубликована: Фев. 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).

Язык: Английский

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Strain-induced water reorientation for enhanced alkaline hydrogen evolution reaction

International Journal of Hydrogen Energy, Год журнала: 2025, Номер 111, С. 33 - 39

Опубликована: Фев. 24, 2025

Язык: Английский

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

Nano Letters, Год журнала: 2025, Номер unknown

Опубликована: Апрель 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.

Язык: Английский

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Electron Rearrangement at the Crystalline-Amorphous Heterogeneous Interface Boosts Alkaline Hydrogen Production

Chemical Science, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Modifying the platinum (Pt) local reaction microenvironment is a critical and complex challenge in enhancing electrochemical performance. Herein, amorphous Co(OH)2 crystalline Pt (labeled as ac-Pt@Co(OH)2) featuring abundant crystalline-amorphous (c-a) interfaces are designed to boost hydrogen evolution (HER). The engineered structure creates an advantageous chemical environment at level, adsorption efficiency resulting exceptional HER ac-Pt@Co(OH)2 achieves low Tafel slope of 28.5 mV dec-1 requires merely 95 overpotential reach 200 mA cm-2 alkaline electrolyte (1 M KOH), surpassing those conventional Pt/C catalysts (39.4 dec-1, 256 mV). In situ advanced characterization investigations reveal dynamic electron rearrangement c-a interface, where Co species initially accept electrons from optimize *H then donate for accelerating reduction kinetics. Theoretical calculations that promotes dissociation water molecules produce active *H, interface downshifts d-band center, thereby optimizing strength activity. ac-Pt@Co(OH)2-based anion-exchange membrane electrolyzer (AEMWE) maintains current density 500 over h.

Язык: Английский

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