Spin effect in dual-atom catalysts for electrocatalysis

Chemical Science, Год журнала: 2024, Номер 15(36), С. 14585 - 14607

Опубликована: Янв. 1, 2024

The development of high-efficiency atomic-level catalysts for energy-conversion and -storage technologies is crucial to address energy shortages. spin states diatomic (DACs) are closely tied their catalytic activity. Adjusting the DACs' active centers can directly modify occupancy d-orbitals, thereby influencing bonding strength between metal sites intermediates as well transfer during electro reactions. Herein, we discuss various techniques characterizing atomic strategies modulating center states. Next, outline recent progress in study effects DACs oxygen reduction reaction (ORR), evolution (OER), hydrogen (HER), electrocatalytic nitrogen/nitrate (eNRR/NO

Язык: Английский

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Promoting Electrocatalytic Oxygen Reactions Using Advanced Heterostructures for Rechargeable Zinc–Air Battery Applications

ACS Nano, Год журнала: 2024, Номер 18(33), С. 21651 - 21684

Опубликована: Авг. 12, 2024

In order to facilitate electrochemical oxygen reactions in electrically rechargeable zinc-air batteries (ZABs), there is a need develop innovative approaches for efficient electrocatalysts. Due their reliability, high energy density, material abundance, and ecofriendliness, ZABs hold promise as next-generation storage conversion devices. However, the large-scale application of currently hindered by slow kinetics reduction reaction (ORR) evolution (OER). development heterostructure-based electrocatalysts has potential surpass limitations imposed intrinsic properties single material. This Account begins with an explanation configurations fundamentals electrochemistry air electrode. Then, we summarize recent progress respect variety heterostructures that exploit bifunctional electrocatalytic overview impact on ZAB performance. The range heterointerfacial engineering strategies improving ORR/OER performance includes tailoring surface chemistry, dimensionality catalysts, interfacial charge transfer, mass transport, morphology. We highlight multicomponent design take these features into account create advanced highly active catalysts. Finally, discuss challenges future perspectives this important topic aim enhance activity batteries.

Язык: Английский

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A review of novel materials for nano-photocatalytic and optoelectronic applications: recent perspectives, water splitting and environmental remediation

Deleted Journal, Год журнала: 2024, Номер 1(4), С. 100018 - 100018

Опубликована: Сен. 11, 2024

Язык: Английский

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DFT-Driven Approaches to Optimizing Small Bandgap Doping Structures: A Brief Review

Journal of Inorganic and Organometallic Polymers and Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 20, 2025

Язык: Английский

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Enhancing Peroxidase‐Like Activity and Photothermal Property of Copper Single‐Atom Nanozyme via A Cascade Competition Strategy

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 16, 2025

Abstract Single‐atom nanozymes (SANs) are promising enzyme‐active catalysts due to their maximum atomic utilization. However, it is still a challenge precisely regulate the single‐atom structure, especially in multimetallic MOFs. Based on Cu‐N 4 structure of Zn Cu 1 , cascade competition strategy mediated by buffer (polydopamine) proposed for first time, which induces one‐step nonthermal reaction remove inactive site and adjust coordination environment. Experimental results theoretical calculations show that nanozyme with 2 O (Cu‐N/O) breaks strong steric restriction, exposed active can better adsorb H making have peroxidase‐like activity. Compared traditional bimetallic (Cu ) monometallic (Cu‐MoF) nanozymes, has stronger catalytic activity photothermal properties, as well good photocatalytic extremely stability. It successfully applied Lateral flow immunoassay achieve three‐mode ultrasensitive detection Escherichia coli O157:H7, test strips after subjected broad‐spectrum sterilization treatment.

Язык: Английский

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Understanding the Metal‐Center Mediated Adsorption and Redox Mechanisms in a FeMn(NbTa)₂O₆ Columbite Material for Anion Exchange Membrane Water Electrolyzers

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Апрель 15, 2025

Abstract The rising demand for sustainable green hydrogen production necessitates efficient and cost‐effective water‐splitting electrocatalysts. Inspired by the catalytic activities of columbite‐tantalite, this study combines a scalable cutting‐edge synthesis approach with atomic‐level structures metal‐center‐mediated mechanisms to unravel its operational performance stability. Using ad in situ X‐ray absorption fine structure combined Density Functional Theory (DFT), results reveal distinctive valence band peaks moderate charge transfer from Mn Fe sites, enabling stable adsorption reduced activation barriers. In contrast, high‐valence Nb Ta centers at B‐sites promote favorable d ‐band alignment, enhancing orbital overlap oxygen p‐ orbitals. This facilites electronic delocalization, lowers accumulation, reduces barriers intermediates species. A‐sites exhibit strong redox reactivity optimal OH* O*, supporting electron fransfers. Solvation effects modeled via VASPsol further stabilize key intermediates, especially reducing energy barrier water dissociation. Notably, FeMn(NbTa) 2 O 6 ‐columbite catalysts stand out cell voltage 1.81 V current density 700 mA cm −2 , compared 40% Pt/C‐RuO₂ (1.75 V) same anion exchange membrane electrolyzer (AEMWE). Also, exhibits long‐term stability 800 surpassing benchmark Pt Vulcan‐RuO after 200 h AEMWE. work significantly advances research establishes design rule selecting metal compositions development advanced electrocatalysts alkaline electrolyzers.

Язык: Английский

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Spin-related excited-state phenomena in photochemistry

National Science Review, Год журнала: 2024, Номер 11(9)

Опубликована: Июль 18, 2024

ABSTRACT The spin of electrons plays a vital role in chemical reactions and processes, the excited state generated by absorption photons shows abundant spin-related phenomena. However, importance electron photochemistry studies has been rarely mentioned or summarized. In this review, we briefly introduce concept based on multiplicity state, which leads to observation various photophysical properties photochemical reactivities. Then, focus recent advances terms light-induced magnetic properties, excited-state magneto-optical effects spin-dependent reactions. review aims provide comprehensive overview utilize manipulating above processes. Finally, discuss existing challenges emerging field future opportunities such as smart materials, optical information technology spin-enhanced photocatalysis.

Язык: Английский

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Manipulating Superexchange Interaction of Ru–O–Fe Sites for Enhanced Electrocatalytic Nitrate-to-Ammonia Selectivity

ACS Catalysis, Год журнала: 2024, Номер 14(16), С. 12152 - 12162

Опубликована: Июль 30, 2024

Fe-based catalysts are promising for electrochemical nitrate reduction, but their selectivity is limited by the multielectron/proton transfer reaction steps. Here, we propose optimizing eg-orbital electron occupancy regulating superexchange interaction of Fe site to improve NH3 production performance. Our experimental and theoretical prediction results confirmed that Ru–O–Fe sites in double perovskite iron oxides (LaFe0.9Ru0.1O3) have more significant interactions, mainly manifested O-anion-mediated from Ru cations. alters Fe's spin configuration through orbital hybridization, transitioning a high-spin (HS, eg ≈ 2) an intermediate-spin state (eg 1). This transition promotes NO3– adsorption lowers hydrogenation energy barrier *NO intermediate. Consequently, LaFe0.9Ru0.1O3 could efficiently convert NH3, achieving rates 0.75 mmol·h–1·cm–2 with Faraday efficiency 98.5%. Remarkably, was as high 90.7%, which represents almost best catalyst date.

Язык: Английский

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Spin polarization strategy regulates heterogeneous catalytic activity performance: from fundamental to application

Chemical Communications, Год журнала: 2024, Номер 60(58), С. 7397 - 7413

Опубликована: Янв. 1, 2024

In recent years, there has been significant attention towards the development of catalysts that exhibit superior performance and environmentally friendly attributes. This surge in interest is driven by growing demands for energy utilization storage as well environmental preservation. Spin polarization plays a crucial role catalyst design, comprehension catalytic mechanisms, reaction control, offering novel insights design highly efficient catalysts. However, are still some research gaps current study spin catalysis. Therefore, it urgent to understand how impacts reactions develop Herein, we present comprehensive summary application Firstly, summarize fundamental mechanism from two aspects kinetics thermodynamics. Additionally, review regulation various applications several approaches modulate polarization. Moreover, discuss future catalysis propose potential avenues further progress. We aim improve systems through implementing distinctive engineering strategy.

Язык: Английский

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Promoting electrocatalytic nitrogen reduction by introducing low-spin sites in ferromagnetic single-atom alloys

Journal of Materials Chemistry A, Год журнала: 2024, Номер 12(35), С. 23425 - 23435

Опубликована: Янв. 1, 2024

In ferromagnetic single-atom alloys, the average electron spin moment P of dopants, a new descriptor, has volcano relationships with e-NRR theoretical activity and selectivity.

Язык: Английский

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