Pd–PdO Nanodomains on Amorphous Ru Metallene Oxide for High‐Performance Multifunctional Electrocatalysis

Advanced Materials, Год журнала: 2023, Номер 35(12)

Опубликована: Янв. 4, 2023

Developing highly efficient multifunctional electrocatalysts is crucial for future sustainable energy pursuits, but remains a great challenge. Herein, facile synthetic strategy used to confine atomically thin Pd-PdO nanodomains amorphous Ru metallene oxide (RuO2 ). The as-synthesized electrocatalyst (Pd2 RuOx-0.5 h) exhibits excellent catalytic activity toward the pH-universal hydrogen evolution reaction (η10 = 14 mV in 1 m KOH, η10 12 0.5 H2 SO4 , and 22 PBS), alkaline oxygen 225 mV), overall water splitting (E10 1.49 V) with high mass operational stability. Further reduction endows material RuOx-2 promising activity, evidenced by halfway potential, four-electron selectivity, poison tolerance. enhanced attributed rational integration of favorable nanostructures, including 1) nanosheet morphology, 2) coexisting defective crystalline phases, 3) multi-component heterostructural features. These structural factors effectively regulate material's electronic configuration adsorption intermediates at active sites energetics.

Язык: Английский

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Heterointerface and Tensile Strain Effects Synergistically Enhances Overall Water‐Splitting in Ru/RuO₂ Aerogels

Small, Год журнала: 2023, Номер 19(10)

Опубликована: Янв. 15, 2023

Designing robust electrocatalysts for water-splitting is essential sustainable hydrogen generation, yet difficult to accomplish. In this study, a fast and facile two-step technique synthesize Ru/RuO2 aerogels catalyzing overall under alkaline conditions reported. Benefiting from the synergistic combination of high porosity, heterointerface, tensile strain effects, aerogel exhibits low overpotential oxygen evolution reaction (189 mV) (34 at 10 mA cm-2 , surpassing RuO2 (338 Pt/C (53 mV), respectively. Notably, when are applied anode cathode, resultant cell reflected potential 1.47 V exceeding commercial Pt/C||RuO2 standard (1.63 V). X-ray adsorption spectroscopy theoretical studies demonstrate that heterointerface optimizes charge redistribution, which reduces energy barriers intermediates, thereby enhancing kinetics.

Язык: Английский

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Activating Amorphous Ru Metallenes Through Co Integration for Enhanced Water Electrolysis

Advanced Energy Materials, Год журнала: 2023, Номер 13(28)

Опубликована: Июнь 11, 2023

Abstract Designing efficient bifunctional electrocatalysts with excellent activity and robust stability presents a central challenge for the large‐scale commercialization of water electrolysis. Herein, facile approach is reported construct atomically thin amorphous RuM (MCo, Fe, or Ni) bimetallenes as high‐performance toward both electrochemical hydrogen evolution reaction (HER) oxygen (OER). The RuCo bimetallene manifests characterized by low required overpotentials, superior price activity, durability well cell potential splitting performance, outperforming Pt/C RuO 2 benchmark catalysts. Combined operando X‐ray absorption spectroscopy investigation theoretical simulations reveal synergism taking place between binary constituents, in which Co serves promotive role along HER/OER pathway, contributing via optimal binding to *OH dissociation modulating Ru electronic structure favorably, hence rendering high catalytic centers alkaline HER OER.

Язык: Английский

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High‐Density Atomic Fe–N₄/C in Tubular, Biomass‐Derived, Nitrogen‐Rich Porous Carbon as Air‐Electrodes for Flexible Zn–Air Batteries

Advanced Functional Materials, Год журнала: 2023, Номер 33(20)

Опубликована: Фев. 22, 2023

Abstract Developing low‐cost single‐atom catalysts (SACs) with high‐density active sites for oxygen reduction/evolution reactions (ORR/OER) are desirable to promote the performance and application of metal–air batteries. Herein, Fe nanoparticles precisely regulated single atoms supported on waste biomass corn silk (CS) based porous carbon ORR OER. The distinct hierarchical structure hollow tube morphology critical boosting ORR/OER through exposing more accessible sites, providing facile electron conductivity, facilitating mass transfer reactant. Moreover, enhanced intrinsic activity is mainly ascribed high (4.3 wt.%) loading content in as‐synthesized catalyst.Moreover, ultra‐high N doping (10 can compensate insufficient OER conventional FeNC catalysts. When as‐prepared assembled as air‐electrodes flexible Zn–air batteries, they perform a peak power density 101 mW cm −2 , stable discharge–charge voltage gap 0.73 V >44 h, which shows great potential Zinc–air battery. This work provides an avenue transform renewable materials into bifunctional electrocatalysts structure.

Язык: Английский

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Spin polarized Fe1−Ti pairs for highly efficient electroreduction nitrate to ammonia

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

Опубликована: Янв. 2, 2024

Abstract Electrochemical nitrate reduction to ammonia offers an attractive solution environmental sustainability and clean energy production but suffers from the sluggish *NO hydrogenation with spin–state transitions. Herein, we report that manipulation of oxygen vacancies can contrive spin−polarized Fe 1 −Ti pairs on monolithic titanium electrode exhibits NH 3 yield rate 272,000 μg h −1 mg a high Faradic efficiency 95.2% at −0.4 V vs. RHE, far superior counterpart spin−depressed (51000 –1 ) mostly reported electrocatalysts. The unpaired spin electrons Ti atoms effectively interact key intermediates, facilitating hydrogenation. Coupling flow−through electrolyzer membrane-based recovery unit, simultaneous was realized. This work pioneering strategy for manipulating polarization electrocatalysts within pair sites wastewater treatment.

Язык: Английский

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Revealing Spin Magnetic Effect of Iron-Group Layered Double Hydroxides with Enhanced Oxygen Catalysis

ACS Catalysis, Год журнала: 2023, Номер 13(2), С. 1431 - 1440

Опубликована: Янв. 9, 2023

The oxygen evolution reaction (OER) is the bottleneck limiting process of water splitting. OER involves recombination from diamagnetic singlet state OH or H2O to paramagnetic triplet O2. spin conservation for oxygenated intermediates must play an important role in OER. However, dynamic mechanism magnetic field-induced polarization still its infancy. Herein, based on spin-coupling interaction iron group elements, three typical layered double hydroxides (LDHs) were constructed study relationship among field, polarization, and activity. Combining experimental theoretical studies, we revealed spin-magnetic effect LDHs enhancing process. There a positive correlation between saturation magnetization performance under different fields. NiCoFe-LDHs (NCFL) endows strongest activity (η10 = 230 mV) (Ms 44 emu mg–1) compared with that CoFe-LDHs (CFL, η10 372 mV, Ms 21 NiFe-LDHs (NFL, 246 29 mg–1). density functional theory calculations show Fe sites NCFL endow stronger OH, Raman spectroscopy further proves promotion formation O–O bond NCFL. Applying external due LDHs, enhancement amplitude also positively correlated magnetism catalyst. has about −34.8 mV T–1 NFL (−27.0 T–1) CFL (−16.7 T–1). overpotential only 206 condition 700 mT field. In conclusion, demonstrate underlying influence provide insights into catalysts intermediates. These would help understand design at spintronic level.

Язык: Английский

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Oxygen-Bridged Stabilization of Single Atomic W on Rh Metallenes for Robust and Efficient pH-Universal Hydrogen Evolution

ACS Nano, Год журнала: 2023, Номер 17(11), С. 10733 - 10747

Опубликована: Май 17, 2023

Highly efficient and durable electrocatalysts are of the utmost importance for sustainable generation clean hydrogen by water electrolysis. Here, we present a report an atomically thin rhodium metallene incorporated with oxygen-bridged single atomic tungsten (Rh-O-W) as high-performance electrocatalyst pH-universal evolution reaction. The Rh-O-W delivers ascendant electrocatalytic HER performance, characterized exceptionally low overpotentials, ultrahigh mass activities, excellent turnover frequencies, robust stability negligible deactivation, in electrolytes, outperforming that benchmark Pt/C, Rh/C numerous other reported precious-metal catalysts. Interestingly, promoting feature -O-W sites is understood via operando X-ray absorption spectroscopy characterization theoretical calculations. On account electron transfer equilibration processes take place between binary components metallenes, fine-tuning density states localization at Rh active attained, hence near-optimal adsorption.

Язык: Английский

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Selective activation of peroxymonosulfate govern by B-site metal in delafossite for efficient pollutants degradation: Pivotal role of d orbital electronic configuration

Water Research, Год журнала: 2023, Номер 236, С. 119957 - 119957

Опубликована: Апрель 8, 2023

Язык: Английский

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An ultrathin 2D NiCo-LDH nanosheet decorated NH₂-UiO-66 MOF-nanocomposite with exceptional chemical stability for electrocatalytic water splitting

Journal of Materials Chemistry A, Год журнала: 2023, Номер 11(19), С. 10309 - 10318

Опубликована: Янв. 1, 2023

Utilization of bifunctional high-efficiency non-precious electrocatalysts for stable and effective water splitting is crucial to the growth clean energy industry.

Язык: Английский

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Manipulation of Electron Spins with Oxygen Vacancy on Amorphous/Crystalline Composite-Type Catalyst

ACS Nano, Год журнала: 2023, Номер 18(1), С. 1214 - 1225

Опубликована: Дек. 27, 2023

By substituting the oxygen evolution reaction (OER) with anodic urea oxidation (UOR), it not only reduces energy consumption for green hydrogen generation but also allows purification of urea-rich wastewater. Spin engineering d orbital and oxygen-containing adsorbates has been recognized as an effective pathway enhancing performance electrocatalysts. In this work, we report fabrication a bifunctional electrocatalyst composed amorphous RuO2-coated NiO ultrathin nanosheets (a-RuO2/NiO) abundant amorphous/crystalline interfaces (HER) UOR. Impressively, 1.372 V voltage is required to attain current density 10 mA cm–2 over electrolyzer. The increased vacancies in a-RuO2/NiO by incorporation RuO2 enhance total magnetization entail numerous spin-polarized electrons during reaction, which speeds up UOR kinetics. functional theory study reveals that promote charge-carrier transfer, tailored d-band center endows optimized adsorption oxygen-generated intermediates. This kind vacancy induced toward boosting HER kinetics provides reliable reference exploration advanced

Язык: Английский

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