Current Advances on the Single‐Atom Nanozyme and Its Bioapplications

Advanced Materials, Год журнала: 2023, Номер 36(10)

Опубликована: Фев. 11, 2023

Nanozymes, a class of nanomaterials mimicking the function enzymes, have aroused much attention as candidate in diverse fields with arbitrarily tunable features owing to diversity crystalline nanostructures, composition, and surface configurations. However, uncertainty their active sites lower intrinsic deficiencies nanomaterial-initiated catalysis compared natural enzymes promote pursuing alternatives by imitating biological centers. Single-atom nanozymes (SAzymes) maximize atom utilization well-defined structure, providing an important bridge investigate mechanism relationship between structure catalytic activity. They risen new burgeoning alternative enzyme from vitro bioanalytical tool vivo therapy flexible atomic engineering structure. Here, focus is mainly on three parts. First, detailed overview single-atom catalyst synthesis strategies including bottom-up top-down approaches given. Then, according structural feature nanocatalysts, influence factors such central metal atom, coordination number, heteroatom doping, metal-support interaction are discussed representative applications (including antibacterial/antiviral performance, cancer therapy, biosensing) highlighted. In end, future perspective challenge facing demonstrated.

Язык: Английский

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Review of Carbon Support Coordination Environments for Single Metal Atom Electrocatalysts (SACS)

Advanced Materials, Год журнала: 2023, Номер 36(1)

Опубликована: Апрель 20, 2023

This topical review focuses on the distinct role of carbon support coordination environment single-atom catalysts (SACs) for electrocatalysis. The article begins with an overview atomic configurations in SACs, including a discussion advanced characterization techniques and simulation used understanding active sites. A summary key electrocatalysis applications is then provided. These processes are oxygen reduction reaction (ORR), evolution (OER), hydrogen (HER), nitrogen (NRR), dioxide (CO

Язык: Английский

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A sodium-ion-conducted asymmetric electrolyzer to lower the operation voltage for direct seawater electrolysis

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Июль 4, 2023

Hydrogen produced from neutral seawater electrolysis faces many challenges including high energy consumption, the corrosion/side reactions caused by Cl-, and blockage of active sites Ca2+/Mg2+ precipitates. Herein, we design a pH-asymmetric electrolyzer with Na+ exchange membrane for direct electrolysis, which can simultaneously prevent Cl- corrosion precipitation harvest chemical potentials between different electrolytes to reduce required voltage. In-situ Raman spectroscopy density functional theory calculations reveal that water dissociation be promoted catalyst based on atomically dispersed Pt anchored Ni-Fe-P nanowires reduced barrier (by 0.26 eV), thus accelerating hydrogen evolution kinetics in seawater. Consequently, asymmetric exhibits current densities 10 mA cm-2 100 at voltages 1.31 V 1.46 V, respectively. It also reach 400 low voltage 1.66 80 °C, corresponding electricity cost US$1.36 per kg H2 ($0.031/kW h bill), lower than United States Department Energy 2025 target (US$1.4 H2).

Язык: Английский

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Terbium-induced cobalt valence-band narrowing boosts electrocatalytic oxygen reduction

Energy & Environmental Science, Год журнала: 2023, Номер 16(11), С. 5500 - 5512

Опубликована: Янв. 1, 2023

Tb 2 O 3 endows Co 3d with a narrow band and appropriate location via 3d–O 2p–Tb 4f gradient orbital coupling to efficiently enhance the oxygen reduction reaction.

Язык: Английский

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Elucidating Electrocatalytic Oxygen Reduction Kinetics via Intermediates by Time‐Dependent Electrochemiluminescence

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(12)

Опубликована: Янв. 2, 2023

Facile evaluation of oxygen reduction reaction (ORR) kinetics for electrocatalysts is critical sustainable fuel-cell development and industrial H2 O2 production. Despite great success in ORR studies using mainstream strategies, such as the membrane electrode assembly, rotation electrodes, advanced surface-sensitive spectroscopy, time spatial distribution reactive species (ROS) intermediates diffusion layer remain unknown. Using time-dependent electrochemiluminescence (Td-ECL), we report an intermediate-oriented method analysis. Owing to multiple ultrasensitive stoichiometric reactions between ROS ECL emitter, except electron transfer numbers rate constants, potential-dependent were successfully obtained first time. Such exclusively uncovered information would guide fuel cells production with maximized activity durability.

Язык: Английский

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Recent advances and challenges in developing electrochemiluminescence biosensors for health analysis

Chemical Communications, Год журнала: 2023, Номер 59(24), С. 3507 - 3522

Опубликована: Янв. 1, 2023

Recent advances and challenges in developing electrochemiluminescence biosensors for health analysis are reviewed.

Язык: Английский

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On the Road from Single-Atom Materials to Highly Sensitive Electrochemical Sensing and Biosensing

Analytical Chemistry, Год журнала: 2023, Номер 95(1), С. 433 - 443

Опубликована: Янв. 10, 2023

ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTOn the Road from Single-Atom Materials to Highly Sensitive Electrochemical Sensing and BiosensingLei JiaoLei JiaoKey Laboratory of Pesticide Chemical Biology Ministry Education, International Joint Research Center for Intelligent Biosensing Technology Health, College Chemistry, Central China Normal University, Wuhan, Hubei 430079, P. R. ChinaInstitute Molecular Metrology, Chemistry Engineering, Qingdao 266071, ChinaMore by Lei JiaoView Biography, Weiqing XuWeiqing XuKey XuView Yu WuYu WuKey WuView Hengjia WangHengjia WangKey WangView Liuyong HuLiuyong HuHubei Engineering Optoelectronic New Energy Materials, Key Plasma Advanced School Science Wuhan Institute Technology, 430205, HuView Wenling GuWenling GuKey GuView Chengzhou Zhu*Chengzhou ZhuKey China*[email protected]More ZhuView Biographyhttps://orcid.org/0000-0003-0679-7965Cite this: Anal. Chem. 2023, 95, 1, 433–443Publication Date (Web):January 10, 2023Publication History Received19 April 2022Published online10 January 2023Published inissue 10 2023https://pubs.acs.org/doi/10.1021/acs.analchem.2c01722https://doi.org/10.1021/acs.analchem.2c01722review-articleACS PublicationsCopyright © 2023 American SocietyRequest reuse permissionsArticle Views2478Altmetric-Citations4LEARN ABOUT THESE METRICSArticle Views are COUNTER-compliant sum full text article downloads since November 2008 (both PDF HTML) across all institutions individuals. These metrics regularly updated reflect usage leading up last few days.Citations number other articles citing this article, calculated Crossref daily. Find more information about citation counts.The Altmetric Attention Score is a quantitative measure attention that research has received online. Clicking on donut icon will load page at altmetric.com with additional details score social media presence given article. how calculated. Share Add toView InAdd Full Text ReferenceAdd Description ExportRISCitationCitation abstractCitation referencesMore Options onFacebookTwitterWechatLinked InRedditEmail Other access optionsGet e-Alertsclose SUBJECTS:Biotechnology,Electrochemical detection,Metals,Platinum,Sensors Get e-Alerts

Язык: Английский

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Regulating Reactive Oxygen Species over M–N–C Single-Atom Catalysts for Potential-Resolved Electrochemiluminescence

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(17), С. 12197 - 12205

Опубликована: Апрель 17, 2024

The development of potential-resolved electrochemiluminescence (ECL) systems with dual emitting signals holds great promise for accurate and reliable determination in complex samples. However, the practical application such is hindered by inevitable mutual interaction mismatch between different luminophores or coreactants. In this work, first time, precisely tuning oxygen reduction performance M–N–C single-atom catalysts (SACs), we present a luminol ECL system employing endogenous dissolved O2 as coreactant. Using advanced situ monitoring theoretical calculations, elucidate intricate mechanism involving selective efficient activation through central metal species modulation. This modulation leads to controlled generation hydroxyl radical (·OH) superoxide (O2·–), which subsequently trigger cathodic anodic emission, respectively. well-designed Cu–N–C SACs, their moderate oxophilicity, enable simultaneous ·OH O2·–, thereby facilitating ECL. As proof concept, employed principal component analysis statistical method differentiate antibiotics based on output dual-potential signals. work establishes new avenue constructing platform single luminophore coreactant precise regulation active intermediates.

Язык: Английский

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Precise coordination of high-loading Fe single atoms with sulfur boosts selective generation of nonradicals

Proceedings of the National Academy of Sciences, Год журнала: 2024, Номер 121(4)

Опубликована: Янв. 17, 2024

Nonradicals are effective in selectively degrading electron-rich organic contaminants, which unfortunately suffer from unsatisfactory yield and uncontrollable composition due to the competitive generation of radicals. Herein, we precisely construct a local microenvironment carbon nitride–supported high-loading (~9 wt.%) Fe single-atom catalyst (Fe SAC) with sulfur via facile supermolecular self-assembly strategy. Short-distance S coordination boosts peroxymonosulfate (PMS) activation generates high-valent iron–oxo species IV =O) along singlet oxygen ( 1 O 2 ), significantly increasing yield, PMS utilization, p -chlorophenol reactivity by 6.0, 3.0, 8.4 times, respectively. The nonradicals is controllable simply changing content. In contrast, long-distance both radicals nonradicals, could not promote reactivity. Experimental theoretical analyses suggest that short-distance upshifts d -band center atom, i.e., being close Fermi level, changes binding mode between atom site generate =O high yield. S-coordinated SAC exhibits excellent application potential various water matrices. These findings can guide rational design robust SACs toward selective utilization.

Язык: Английский

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Electroless Deposition of Palladium Nanoparticles on Graphdiyne Boosts Electrochemiluminescence

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(6), С. 3836 - 3843

Опубликована: Фев. 2, 2024

Modulating the electronic structure of metal nanoparticles via metal–support interaction has attracted intense interest in field catalytic science. However, roles supporting substrates regulating properties electrochemiluminescence (ECL) remain elusive. Here, we find that use graphdiyne (GDY) as substrate for electroless deposition Pd (Pd/GDY) produces most pronounced anodic signal enhancement luminol–dissolved oxygen (O2) ECL system co-reactant accelerator over other carbon-based composite nanomaterials. Pd/GDY exhibits electrocatalytic activity reduction O2 through a four-electron pathway at approximately −0.059 V (vs Ag/AgCl) neutral solution forming reactive species (ROS) intermediates. The study shows and GDY increases amount stability ROS on electrode surface promotes reaction luminol anion radical to generate excited luminol, which significantly boosts emission. Based quenching consumption by antioxidants, develop platform detection intracellular antioxidants. This provides an avenue development efficient systems media expands biological application systems.

Язык: Английский

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