Co-catalytic metal–support interactions in single-atom electrocatalysts

Nature Reviews Materials, Journal Year: 2024, Volume and Issue: 9(3), P. 173 - 189

Published: Jan. 10, 2024

Language: Английский

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Precise Tuning of the D-Band Center of Dual-Atomic Enzymes for Catalytic Therapy

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(14), P. 10023 - 10031

Published: March 30, 2024

Single-atom nanozyme-based catalytic therapy is of great interest in the field tumor therapy; however, their development suffers from low affinity nanozymes to substrates (H2O2 or O2), leading deficient activity microenvironment. Herein, we report a new strategy for precisely tuning d-band center dual-atomic sites enhance metal atomic and on class edge-rich N-doped porous carbon Fe–Mn (Fe1Mn1–NCe) greatly boosting multiple-enzyme-like activities. The as-made Fe1Mn1–NCe achieved much higher efficiency (Kcat/Km = 4.01 × 105 S–1·M–1) than Fe1–NCe 2.41 104 with an outstanding stability over 90% retention after 1 year, which best among reported dual-atom nanozymes. Theoretical calculations reveal that synergetic effect Mn upshifts Fe −1.113 −0.564 eV enhances adsorption capacity substrate, thus accelerating dissociation H2O2 weakening O–O bond O2. We further demonstrated superior enzyme-like combined photothermal could effectively inhibit growth vivo, inhibition rate up 95.74%, highest value artificial enzyme therapies so far.

Language: Английский

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Bimetallic Single-Atom Nanozyme-Based Electrochemical-Photothermal Dual-Function Portable Immunoassay with Smartphone Imaging

Analytical Chemistry, Journal Year: 2024, Volume and Issue: 96(33), P. 13663 - 13671

Published: Aug. 10, 2024

Rapid and accurate detection of human epidermal growth factor receptor 2 (HER2) is crucial for the early diagnosis prognosis breast cancer. In this study, we reported an iron-manganese ion N-doped carbon single-atom catalyst (FeMn-NC

Language: Английский

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Glutathione Induced In situ Synthesis of Cu Single‐Atom Nanozymes with Anaerobic Glycolysis Metabolism Interference for Boosting Cuproptosis

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(18)

Published: Feb. 23, 2024

Abstract Single‐atom nanozyme (SAzyme) has sparked increasing interest for catalytic antitumor treatment due to their more tunable and diverse active sites than natural metalloenzymes in complex physiological conditions. However, it is usually a hard task precisely conduct catalysis at tumor after intravenous injection of those SAzyme with high reactivity. Moreover, the explorations SAzymes anticancer application are still its infancy need be developed. Herein, an situ synthesis strategy Cu was constructed convert adsorbed copper ions into isolated atoms anchored by oxygen (Cu−O 2 /Cu−O 4 ) via GSH‐responsive deformability supports. Our results suggest that activation process could further facilitate dissociation consumption glutathione, thereby leading deposition cytoplasm triggering cuproptosis. peroxidase‐like activity enabled intracellular reactive species production, resulting specifically disturbance metabolism pathway. Meanwhile, exposed glucose transporter (GLUT) inhibitor phloretin (Ph) can block glycose uptake boost cuproptosis efficacy. Overall, this effectively diminished off‐target effects SACs‐induced therapies introduced promising paradigm advancing cuproptosis‐associated therapies.

Language: Английский

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High-Volumetric Density Atomic Cobalt on Multishell Zn_xCd_1–xS Boosts Photocatalytic CO₂ Reduction

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(14), P. 9721 - 9727

Published: April 1, 2024

The volumetric density of the metal atomic site is decisive to operating efficiency photosynthetic nanoreactor, yet its rational design and synthesis remain a grand challenge. Herein, we report shell-regulating approach enhance Co sites onto/into multishell ZnxCd1–xS for greatly improving CO2 photoreduction activity. We first establish quantitative relation between number shell layers, specific surface areas, on conclude positive performance layers. triple-shell ZnxCd1–xS–Co1 achieves highest CO yield rate 7629.7 μmol g–1 h–1, superior those double-shell (5882.2 h–1) single-shell (4724.2 h–1). Density functional theory calculations suggest that high-density can promote mobility photogenerated electrons adsorption Co(bpy)32+ increase activation (CO2 → CO2* COOH* CO* CO) via S–Co-bpy interaction, thereby enhancing photocatalytic reduction.

Language: Английский

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Tailored Metal‐Organic Framework‐Based Nanozymes for Enhanced Enzyme‐Like Catalysis

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 19, 2024

Abstract The global crisis of bacterial infections is exacerbated by the escalating threat microbial antibiotic resistance. Nanozymes promise to provide ingenious solutions. Here, we reported a homogeneous catalytic structure Pt nanoclusters with finely tuned metal–organic framework (ZIF‐8) channel structures for treatment infected wounds. Catalytic site normalization showed that active aggregates fine‐tuned pore modifications had capacity 14.903×10 5 min −1 , which was 18.7 times higher than particles in monodisperse state ZIF‐8 (0.793×10 ). In situ tests revealed change from homocleavage heterocleavage hydrogen peroxide at interface nanozyme one key reasons improvement activity. Density‐functional theory and kinetic simulations reaction jointly determine role center substrate together. Metabolomics analysis developed nanozyme, working conjunction reactive oxygen species, could effectively block energy metabolic pathways within bacteria, leading spontaneous apoptosis rupture. This pioneering study elucidates new ideas regulation artificial enzyme activity provides perspectives development efficient substitutes.

Language: Английский

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Dual-Atom Nanozyme Eye Drops Attenuate Inflammation and Break the Vicious Cycle in Dry Eye Disease

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 16(1)

Published: Feb. 19, 2024

Dry eye disease (DED) is a major ocular pathology worldwide, causing serious discomfort and even visual impairment. The incidence of DED gradually increasing with the high-frequency use electronic products. Although inflammation core cause vicious cycle, reactive oxygen species (ROS) play pivotal role in cycle by regulating from upstream. Therefore, current therapies merely targeting show failure treatment. Here, novel dual-atom nanozymes (DAN)-based drops are developed. antioxidative DAN successfully prepared embedding Fe Mn bimetallic single-atoms N-doped carbon material modifying it hydrophilic polymer. vitro vivo results demonstrate endowed superior biological activity scavenging excessive ROS, inhibiting NLRP3 inflammasome activation, decreasing proinflammatory cytokines expression, suppressing cell apoptosis. Consequently, effectively alleviate inflammation, promote corneal epithelial repair, recover goblet density tear secretion, thus breaking cycle. Our findings open an avenue to make as intervention form ROS-mediated inflammatory diseases.

Language: Английский

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Mechanism Exploration of the Photoelectrochemical Immunoassay for the Integration of Radical Generation with Self-Quenching

Analytical Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 10, 2024

Photoelectrochemical (PEC) sensing mechanisms based on enzyme-catalyzed strategies primarily achieve the quantitative analysis of biomolecules through enhancement or attenuation photocurrent signals. However, there are still no reports that delve into principles signaling conversion in reaction between photoactive materials and biomolecules. In this work, we demonstrated indium oxysulfide InOS-0.5 heterojunction has excellent peroxidase activity to catalyze H

Language: Английский

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Materials Containing Single‐, Di‐, Tri‐, and Multi‐Metal Atoms Bonded to C, N, S, P, B, and O Species as Advanced Catalysts for Energy, Sensor, and Biomedical Applications

Advanced Science, Journal Year: 2024, Volume and Issue: 11(33)

Published: July 1, 2024

Abstract Modifying the coordination or local environments of single‐, di‐, tri‐, and multi‐metal atom (SMA/DMA/TMA/MMA)‐based materials is one best strategies for increasing catalytic activities, selectivity, long‐term durability these materials. Advanced sheet supported by metal atom‐based have become a critical topic in fields renewable energy conversion systems, storage devices, sensors, biomedicine owing to maximum utilization efficiency, precisely located centers, specific electron configurations, unique reactivity, precise chemical tunability. Several offer excellent support are attractive applications energy, medical research, such as oxygen reduction, production, hydrogen generation, fuel selective detection, enzymatic reactions. The strong metal–metal metal–carbon with metal–heteroatom (i.e., N, S, P, B, O) bonds stabilize optimize electronic structures atoms due interfacial interactions, yielding activities. These provide models understanding fundamental problems multistep This review summarizes substrate structure‐activity relationship different active sites based on experimental theoretical data. Additionally, new synthesis procedures, physicochemical characterizations, biomedical discussed. Finally, remaining challenges developing efficient SMA/DMA/TMA/MMA‐based presented.

Language: Английский

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p–d Orbital Hybridization-Engineered PdSn Nanozymes for a Sensitive Immunoassay

Nano Letters, Journal Year: 2024, Volume and Issue: 24(9), P. 2912 - 2920

Published: Feb. 23, 2024

Nanozymes with peroxidase-like activity have been extensively studied for colorimetric biosensing. However, their catalytic and specificity still lag far behind those of natural enzymes, which significantly affects the accuracy sensitivity To address this issue, we design PdSn nanozymes selectively enhanced activity, improves a immunoassay. The is higher than that Pd nanozymes. Theoretical calculations reveal p–d orbital hybridization Sn not only results in an upward shift d-band center to enhance hydrogen peroxide (H2O2) adsorption but also regulates O–O bonding strength H2O2 achieve selective activation. Ultimately, nanozyme-linked immunosorbent assay has successfully developed sensitively accurately detect prostate-specific antigen (PSA), achieving low detection limit 1.696 pg mL–1. This work demonstrates promising approach detecting PSA clinical diagnosis.

Language: Английский

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