Precisely Constructing Orbital‐Coupled Fe─Co Dual‐atom Sites for High‐Energy‐Efficiency Zn–Air/Iodide Hybrid Batteries

Advanced Materials, Год журнала: 2024, Номер 36(32)

Опубликована: Май 30, 2024

Abstract Rechargeable Zn–air batteries (ZABs) are promising for energy storage and conversion. However, the high charging voltage low efficiency hinder their commercialization. Herein, these challenges addressed by employing precisely constructed multifunctional Fe–Co diatomic site catalysts (FeCo‐DACs) integrating iodide/iodate redox into ZABs to create Zinc–air/iodide hybrid (ZAIHBs) with highly efficient catalyst. The strong coupling between 3d orbitals of Fe Co weakens excessively binding strength active sites intermediates, enhancing catalytic activities oxygen reduction/evolution reaction redox. Consequently, FeCo‐DACs exhibit outstanding bifunctional activity a small potential gap (Δ E = 0.66 V) stability. Moreover, an performance toward is obtained. Therefore, FeCo‐DAC‐based ZAIHBs up 75% at 10 mA cm −2 excellent cycling stability (72% after 500 h). This research offers critical insights rational design DACs paves way high‐energy devices.

Язык: Английский

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Shear‐Strained Pd Single‐Atom Electrocatalysts for Nitrate Reduction to Ammonia

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Июль 16, 2024

Electrochemical nitrate reduction method (NitRR) is a low-carbon, environmentally friendly, and efficient for synthesizing ammonia, which has received widespread attention in recent years. Copper-based catalysts have leading edge due to their good adsorption of *NO

Язык: Английский

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Rational design of local microenvironment for electrocatalytic water splitting

Inorganic Chemistry Frontiers, Год журнала: 2024, Номер 11(14), С. 4080 - 4106

Опубликована: Янв. 1, 2024

This summary describes the effects of wettability, local pH, interfacial water structure, and electrolyte composition on interface reactant compositions, key intermediate adsorption, reaction kinetics.

Язык: Английский

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Interfacial Water Regulation for Nitrate Electroreduction to Ammonia at Ultralow Overpotentials

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 8, 2025

Abstract Nitrate electroreduction is promising for achieving effluent waste‐water treatment and ammonia production with respect to the global nitrogen balance. However, due impeded hydrogenation process, high overpotentials need be surmounted during nitrate electroreduction, causing intensive energy consumption. Herein, a hydroxide regulation strategy developed optimize interfacial H 2 O behavior accelerating conversion of at ultralow overpotentials. The well‐designed Ru─Ni(OH) electrocatalyst shows remarkable efficiency 44.6% +0.1 V versus RHE nearly 100% Faradaic NH 3 synthesis 0 RHE. In situ characterizations theoretical calculations indicate that Ni(OH) can regulate structure promoted dissociation process contribute spontaneous hydrogen spillover boosting NO − Ru sites. Furthermore, assembled rechargeable Zn‐NO /ethanol battery system exhibits an outstanding long‐term cycling stability charge–discharge tests high‐value‐added ammonium acetate, showing great potential simultaneously removal, conversion, chemical synthesis. This work not only provide guidance in extensive reactions but also inspire design novel hybrid flow multiple functions.

Язык: Английский

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Enhancing Electrocatalytic Activity Through Targeted Local Electrolyte Micro‐Environment

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 10, 2025

Abstract The local electrolyte micro‐environment surrounding the catalyst reaction center, including critical factors such as pH, reactant concentration, and electric field, plays a decisive role in electrocatalytic reactions water splitting. Recently, this topic has garnered significant attention due to its potential significantly enhance catalytic performance. While various strategies optimize processes have been explored, deliberate control over fundamental principles guiding these adjustments remain their early stages of development. This review provides comprehensive examination key efforts aimed at designing tailoring localized micro‐environments improve It discusses advances micro‐environmental design, methodologies for evaluating shifts, mechanistic insights driving developments. Additionally, highlights existing challenges prospective industrial applications strategies. By offering detailed analysis recent developments, aims equip researchers with practical knowledge on controlling micro‐environments, thereby accelerating progress toward real‐world processes.

Язык: Английский

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Unlocking Efficient Alkaline Hydrogen Evolution Through Ru–Sn Dual Metal Sites and a Novel Hydroxyl Spillover Effect

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 28, 2024

Abstract Alkaline hydrogen evolution reaction (HER) has great potential in practical production but is still limited by the lack of active and stable electrocatalysts. Herein, efficient water dissociation process, fast transfer adsorbed hydroxyl optimized adsorption are first achieved on a cooperative electrocatalyst, named as Ru–Sn/SnO 2 NS, which Ru–Sn dual metal sites SnO heterojunction constructed based porous Ru nanosheet. The density functional theory (DFT) calculations situ infrared spectra suggest that can optimize process adsorption, while existence induce unique spillover effect, accelerating avoiding poison sites. As results, NS display remarkable alkaline HER performance with an extremely low overpotential (12 mV at 10 mA cm −2 ) robust stability (650 h), much superior to those (27 90 h stability) (16 120 stability). work sheds new light designing electrocatalyst.

Язык: Английский

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Harvesting energy from marine: Seawater electrolysis for hydrogen production

Fuel, Год журнала: 2024, Номер 377, С. 132782 - 132782

Опубликована: Авг. 14, 2024

Язык: Английский

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Shear‐strained Pd Single‐atom Electrocatalysts for Nitrate Reduction to Ammonia

Angewandte Chemie, Год журнала: 2024, Номер 136(43)

Опубликована: Июль 16, 2024

Abstract Electrochemical nitrate reduction method (NitRR) is a low‐carbon, environmentally friendly, and efficient for synthesizing ammonia, which has received widespread attention in recent years. Copper‐based catalysts have leading edge due to their good adsorption of *NO 3 . However, the formation active hydrogen (*H) on Cu surfaces difficult insufficient, resulting large amount by‐product NO 2 − In this work, Pd single atoms suspended interlayer unsaturated bonds CuO formed dislocations (Pd−CuO) were prepared by low temperature treatment, located subjected shear stress dynamic effect support promote conversion into ammonia. The catalysis had an ammonia yield 4.2 mol. g cat −1 h , Faraday efficiency 90 % production at −0.5 V vs. RHE. situ characterization theoretical calculations indicate that effects carriers under obviously hydrogen, reduce reaction energy barrier decision‐making step further generation.

Язык: Английский

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Strong d‐p Orbital Hybridization of Os‐P via Ultrafast Microwave Plasma Assistance for Anion Exchange Membrane Electrolysis

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Авг. 2, 2024

Abstract Orbital hybridization is a promising approach to modulating the electronic structure of designed electrocatalysts boost reaction kinetics. In contrast d‐d hybridization, p‐d orbital between p‐block elements and d‐block metals can provide new opportunities modulate properties thus promote catalytic performance. Herein, phosphorus‐doped osmium (P‐Os) catalyst through ultrafast (20 s) microwave plasma engineering. Theoretical calculations verify d‐p P Os, leading modulation d‐band center Os active site. Specifically, neighboring exhibit highest activity, facilitating crucial processes such as H 2 O/H* adsorption dissociation. The overpotential P‐Os in alkaline seawater only 152 mV at 1 A cm −2 , which superior reported electrocatalysts. Moreover, synthesized catalysts are integrated into an anion exchange membrane (AEM) electrolyzer, demonstrating remarkable AEM electrolyzer requires 1.86/2.02 V achieve 500/1000 mA current densities. Then, achieved have great potential for practical electrocatalytic water‐splitting applications.

Язык: Английский

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Origin of Enhanced Oxygen Evolution in Restructured Metal‐Organic Frameworks for Anion Exchange Membrane Water Electrolysis

Angewandte Chemie International Edition, Год журнала: 2024, Номер 64(1)

Опубликована: Сен. 14, 2024

Metal-Organic Frameworks (MOFs), praised for structural flexibility and tunability, are prominent catalyst prototypes exploring oxygen evolution reaction (OER). Yet, their intricate transformations under OER, especially in industrial high-current environments, pose significant challenges accurately elucidating structure-activity correlation. Here, we harnessed an electrooxidation process controllable MOF reconstruction, discovering that Fe doping expedites Ni(Fe) evolution, accompanied by the elongation of Ni-O bonds, monitored situ Raman UV/Visible spectroscopy. Theoretical modeling further reveals defect-induced tensile strain NiO

Язык: Английский

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