Heteroatom‐Doping of Non‐Noble Metal‐Based Catalysts for Electrocatalytic Hydrogen Evolution: An Electronic Structure Tuning Strategy

Small Methods, Год журнала: 2021, Номер 5(4)

Опубликована: Янв. 25, 2021

Abstract Electrocatalytic water splitting for hydrogen production is an appealing way to reduce carbon emissions and generate renewable fuels. This promising process, however, limited by its sluggish reaction kinetics high‐cost catalysts. Construction of low‐cost high‐performance non‐noble metal‐based catalysts have been one the most effective approaches address these grand challenges. Notably, electronic structure tuning strategy, which could subtly tailor states, band structures, adsorption ability catalysts, has become a pivotal further enhance electrochemical reactions based on Particularly, heteroatom‐doping plays role in regulating optimizing intrinsic activity Nevertheless, kinetics, particular, functional mechanisms hetero‐dopants yet remains ambiguous. Herein, recent progress comprehensively reviewed heteroatom doped electrocatalysts evolution reaction, particularly focus effect corresponding synthetic pathway, catalytic performance, origin. review also attempts establish correlation between localized structures properties, so as provide good reference developing advanced

Язык: Английский

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Intrinsic Activity of Metal Centers in Metal–Nitrogen–Carbon Single-Atom Catalysts for Hydrogen Peroxide Synthesis

Journal of the American Chemical Society, Год журнала: 2020, Номер 142(52), С. 21861 - 21871

Опубликована: Дек. 17, 2020

Metal–nitrogen–carbon (M–N–C) single-atom catalysts (SACs) show high catalytic activity for many important chemical reactions. However, an understanding of their intrinsic remains ambiguous because the lack well-defined atomic structure control in current M–N–C SACs. Here, we use covalent organic framework SACs with identical metal coordination environment as model to elucidate various centers A pH-universal trend is discovered among six 3d transition metals hydrogen peroxide (H2O2) synthesis, Co having highest activity. Using density functional calculations access a total 18 species, demonstrate that difference binding energy O2* and HOOH* intermediates (EO2* – EHOOH*) on single reliable thermodynamic descriptor predict centers. The predicted Ir from further validated experimentally. This work suggests class structurally defined clear mechanistic principles H2O2 which may be extendable other

Язык: Английский

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Single-atom catalysts boost signal amplification for biosensing

Chemical Society Reviews, Год журнала: 2020, Номер 50(2), С. 750 - 765

Опубликована: Дек. 11, 2020

This tutorial review highlights the signal amplification of single-atom catalysts in colorimetric, electrochemical, chemiluminescence, electrochemiluminescence, and photoelectrochemical biosensing applications.

Язык: Английский

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Atomically Dispersed Transition Metal-Nitrogen-Carbon Bifunctional Oxygen Electrocatalysts for Zinc-Air Batteries: Recent Advances and Future Perspectives

Nano-Micro Letters, Год журнала: 2021, Номер 14(1)

Опубликована: Дек. 16, 2021

Abstract Rechargeable zinc-air batteries (ZABs) are currently receiving extensive attention because of their extremely high theoretical specific energy density, low manufacturing costs, and environmental friendliness. Exploring bifunctional catalysts with activity stability to overcome sluggish kinetics oxygen reduction reaction evolution is critical for the development rechargeable ZABs. Atomically dispersed metal-nitrogen-carbon (M-N-C) possessing prominent advantages metal atom utilization electrocatalytic promising candidates promote electrocatalysis. In this work, general principles designing atomically M-N-C reviewed. Then, strategies aiming at enhancing catalytic presented. Finally, challenges perspectives ZABs outlined. It expected that review will provide insights into targeted optimization in

Язык: Английский

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Oxo dicopper anchored on carbon nitride for selective oxidation of methane

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Март 16, 2022

Selective conversion of methane (CH4) into value-added chemicals represents a grand challenge for the efficient utilization rising hydrocarbon sources. We report here dimeric copper centers supported on graphitic carbon nitride (denoted as Cu2@C3N4) advanced catalysts CH4 partial oxidation. The copper-dimer demonstrate high selectivity oxidation under both thermo- and photocatalytic reaction conditions, with hydrogen peroxide (H2O2) oxygen (O2) being used oxidizer, respectively. In particular, O2 achieves >10% conversion, >98% toward methyl oxygenates mass-specific activity 1399.3 mmol g Cu-1h-1. Mechanistic studies reveal that reactivity Cu2@C3N4 can be ascribed to symphonic mechanisms among bridging oxygen, two sites semiconducting C3N4 substrate, which do not only facilitate heterolytic scission C-H bond, but also promotes H2O2 activation in photocatalysis,

Язык: Английский

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Two-Dimensional Cobalt-Doped Ti₃C₂ MXene Nanozyme-Mediated Homogeneous Electrochemical Strategy for Pesticides Assay Based on In Situ Generation of Electroactive Substances

Analytical Chemistry, Год журнала: 2022, Номер 94(8), С. 3669 - 3676

Опубликована: Фев. 15, 2022

Common homogeneous electrochemical (HEC) sensors usually suffer from the drawbacks of high background signal, low signal-to-noise ratio, and even false positive results due to preaddition electroactive substances. Thus, it is necessary develop novel HEC based on in situ generation substances overcome these shortcomings, which, however, underexplored. In this work, two-dimensional (2D) nanozymes, i.e., cobalt-doped 2D Ti3C2 MXene nanosheets (CMNSs), with excellent peroxidase-like properties were utilized for organophosphate pesticides (OPs) detection. The CMNSs synthesized via a template-directed wet chemical approach displayed outstanding features hydrophilia water dispersibility, which could catalyze oxidation o-phenylenediamine (OPD) generate significantly increased reduction current. Interestingly, exhibited unique response thiol compounds thus employed as highly efficient catalysts OPs hydrolysis acetylthiocholine (ATCh) form thiocholine catalyzed by acetylcholinesterase (AChE) inhibition AChE activity OPs. recovery analysis pakchoi extract solutions ranged 97.4% 103.3%. as-proposed sensor will provide new way development high-performance demonstrate potential applicability determination pesticide residues real samples.

Язык: Английский

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Stabilizing Fe–N–C Catalysts as Model for Oxygen Reduction Reaction

Advanced Science, Год журнала: 2021, Номер 8(23)

Опубликована: Окт. 23, 2021

Abstract The highly efficient energy conversion of the polymer‐electrolyte‐membrane fuel cell (PEMFC) is extremely limited by sluggish oxygen reduction reaction (ORR) kinetics and poor electrochemical stability catalysts. Hitherto, to replace costly Pt‐based catalysts, non‐noble‐metal ORR catalysts are developed, among which transition metal–heteroatoms–carbon (TM–H–C) materials present great potential for industrial applications due their outstanding catalytic activity low expense. However, during testing in a two‐electrode system high complexity have become big barrier commercial applications. Thus, herein, simplify research, typical Fe–N–C material with relatively simple constitution structure, selected as model catalyst TM–H–C explore improve such kind Then, different types active sites (centers) coordination systematically summarized discussed, possible attenuation mechanism strategies analyzed. Finally, some challenges faced prospects proposed shed light on future development trend advanced catalysis.

Язык: Английский

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MgH2 confinement in MOF-derived N-doped porous carbon nanofibers for enhanced hydrogen storage

Chemical Engineering Journal, Год журнала: 2022, Номер 434, С. 134701 - 134701

Опубликована: Янв. 15, 2022

Язык: Английский

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Carbon-based bifunctional electrocatalysts for oxygen reduction and oxygen evolution reactions: Optimization strategies and mechanistic analysis

Journal of Energy Chemistry, Год журнала: 2022, Номер 71, С. 234 - 265

Опубликована: Март 25, 2022

Язык: Английский

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Regulating the FeN₄ Moiety by Constructing Fe–Mo Dual-Metal Atom Sites for Efficient Electrochemical Oxygen Reduction

Nano Letters, Год журнала: 2022, Номер 22(23), С. 9507 - 9515

Опубликована: Ноя. 15, 2022

An Fe–N–C catalyst with an FeN4 active moiety has gained ever-increasing attention for the oxygen reduction reaction (ORR); however, catalytic performance is sluggish in acidic solutions and regulation still a challenge. Herein, Fe–Mo dual-metal sites were constructed to tune ORR activity of mononuclear Fe site embedded porous nitrogen-doped carbon. The cracking O–O bonds much more facile on atomic pair due preferred bridge-cis adsorption model molecules. downshift d band center when Mo atom introduced FeNx configuration optimizes absorption–desorption behavior intermediates FeMoN6 moiety, thus boosting performance. construction regulate catalytically paves way electrocatalytic other similar non-precious-metal catalysts.

Язык: Английский

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