Efficient Hydrogen Generation from Ammonia Borane Hydrolysis on a Tandem Ruthenium–Platinum–Titanium Catalyst

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(33)

Опубликована: Май 28, 2024

Hydrolysis of ammonia borane (NH

Язык: Английский

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Destabilization of Single‐Atom Catalysts: Characterization, Mechanisms, and Regeneration Strategies

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 19, 2025

Abstract Numerous in situ characterization studies have focused on revealing the catalytic mechanisms of single‐atom catalysts (SACs), providing a theoretical basis for their rational design. Although research is relatively limited, stability SACs under long‐term operating conditions equally important and prerequisite real‐world energy applications, such as fuel cells water electrolyzers. Recently, there has been rise destabilization regeneration SACs; however, timely comprehensive summaries that provide catalysis community with valuable insights directions are still lacking. This review summarizes recent advances strategies SACs, specifically highlighting various state‐of‐the‐art techniques employed studies. The factors induce identified by discussing failure active sites, coordination environments, supports, reaction scenarios. Next, primary introduced, including redispersion, surface poison desorption, exposure subsurface sites. Additionally, advantages limitations both ex discussed. Finally, future proposed, aimed at constructing structure–stability relationships guiding design more stable SACs.

Язык: Английский

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Fluorescent Fingerprint Identification of Protein Structural Changes and Disease-Specific Amyloid Beta Aggregates Based on a Single-Nanozyme Sensor Array

Analytical Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Фев. 25, 2025

The misfolding of amyloid β (Aβ) peptides into an aggregation state is a central hallmark the onset Alzheimer's disease (AD). However, conventional methods are mainly focused on detecting specific Aβ peptide, which makes it difficult to recognize multiple analytes with different topological features and unfolded states at same time. Here, we propose simple universal sensing strategy construct fluorescence sensor array by using single-nanozyme probe combined three fluorescent substrates as recognition units protein structural changes identify between assemblies. In this system, fingerprint-like patterns produced from nonspecific interactions proteins units. As result, can accurately 13 kinds their mixtures ratios. Moreover, discriminate against diverse conformational forms. Most importantly, successfully distinguishes species, even in artificial cerebrospinal fluid samples human serum samples. This work provides attractive reliable for predicting pathologically relevant clinical diagnosis AD.

Язык: Английский

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High‐Throughput Screening and General Synthesis Strategy of Single‐Atom Nanozymes for Oral Squamous Cell Carcinoma Therapy

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 5, 2025

Abstract Single‐atom nanozymes (SAzymes), with their superior enzyme‐like catalytic activity, have emerged as promising candidates for oncology therapeutics. The well‐defined structures of SAzymes make them well predictable by experiences and theoretical calculation. However, the effects metal center species coordination environments on activity are variable, screening artificial experiments is challenging. High‐throughput can rapidly select optimal thus better application in tumor therapy highly desirable. Herein, a “high‐throughput screening‐SAzymes structures” system established efficient drug preparation density functional theory oxidase‐like processes screened differences brought about different metals environments. Through this process, transition (Mn, Fe, Co, Ni) active centers synthesized then tested multi‐enzyme activities. It found that SAzyme Co exhibited best further showed good anti‐oral squamous cell carcinoma properties both vitro vivo. This study opens up new avenue rational design oral cancer combining computational experimental validation.

Язык: Английский

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Unleashing the Potential of Single-Atom Nanozymes: Catalysts for the Future

ACS Sensors, Год журнала: 2024, Номер 9(8), С. 3840 - 3847

Опубликована: Июль 31, 2024

Single-atom nanozymes (SANs) have become a breakthrough in atomically precise catalysis, which relies on the catalytic active site formed by single-atom itself. From this angle, SANs and their advantages compared to natural enzymes as well spaces for application are emphasized. The outstanding control over activities; is with bulk materials enzymes. structure of has very promising potential next generation biosensing biomedical devices environmental remediation. Although capabilities high, difficulties still arise. specificity, scalability, biosafety, catalysis mechanisms raise additional issues that require further research. We build up vision perspectives better implementation SANs, designed diagnostic purposes, improving industrial technologies, creating new sustainable technologies food processing industry. AI machine learning systems may clarify structure–performance relationship improved material process selectivity. future promising, addressing these challenges leveraging advancements artificial intelligence science, powerful tools future.

Язык: Английский

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Recent progress in noble metal-based single-atom nanozymes for biomedical applications

Microchemical Journal, Год журнала: 2024, Номер unknown, С. 111731 - 111731

Опубликована: Сен. 1, 2024

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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Engineering the Lewis Acidity of Fe Single-Atom Sites via Atomic-Level Tuning of Spatial Coordination Configuration for Enhanced Oxygen Reduction

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Фев. 16, 2025

Nitrogen-doped carbon-supported Fe catalysts (Fe-N-C) with Fe-N4 active sites hold great promise for the oxygen reduction reaction (ORR). However, fine-tuning structure of to enhance their performance remains a grand challenge. Herein, we report an innovative design strategy promote ORR activity and kinetics by engineering Lewis acidity, which is achieved tuning spatial coordination geometry. Theoretical calculations indicated that Fe1-N4SO2 (with axial –SO2 group bonded Fe) offered favorable acidity ORR, leading optimized adsorption energies key intermediates. To implement this strategy, developed molecular-cage-encapsulated synthesize single-atom site catalyst (SAC) sites. In agreement theory, Fe1-N4SO2/NC demonstrated outstanding in both alkaline (E1/2 = 0.910 V 0.1 M KOH) acidic media 0.772 HClO4), surpassing commercial Pt/C traditional SACs Fe1-N4 or planar S-coordinated Fe1-N4-S Moreover, newly showed application potential quasi-solid-state Zn–air batteries, delivering superior across wide temperature range.

Язык: Английский

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Coordination Engineering in Fe‐Mn Dual‐Atom Nanozyme: Yielding ROS Storm to Efficiently Promote Wound Healing

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 19, 2025

Abstract Multidrug‐resistant bacterial infections have become a global public health issue. To solve this dilemma, single‐atom nanozymes been used as versatile antibiotics. However, the efficacy of individual nanozyme is hindered by their limited catalytic activity and antibacterial effect. Herein, novel N 3 ‐Fe 1 ‐Mn ‐N 2 S (Fe/Mn‐SNC), with neighboring Mn Fe dual pairs decorated on yolk‐shell‐like carbon skeleton, constructed through partial modulation Fe‐Mn site coordination sulfur atoms. The developed Fe/Mn‐SNC possesses superior multienzyme‐like cascade activities (oxidase‐, superoxide‐, peroxidase‐like activities). It catalyzes conversion O into ·− its oxidase‐like activity, which then decomposed H superoxide‐like enzyme properties. Ultimately, ·OH generated under influence activity. This process effectively kills bacteria without addition , contributing to overcoming resistance issues. Density functional theory calculations indicate that direct coordinated atom enhances dual‐atomic provides an additional active for enhancement superoxidase‐ activities. Fe/Mn‐SNC, high effect biosafety, showing wide potential applications in medical technology consumer care. work opens new avenue designing multifunctional applications.

Язык: Английский

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Boosting Peroxidase-Mimetic Activity of FeMn-NC_e Dual-Atom Radiosensitizing Nanozymes for Augmented Radiodynamic Immunotherapy

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Март 7, 2025

Dual-atom nanozymes (DAzymes) have garnered considerable attention as catalysts for reactive oxygen species (ROS)-based therapies, effectively leveraging ROS generation within the tumor microenvironment (TME). Herein, we introduce FeMn-NCe DAzymes, which are meticulously engineered enhanced peroxidase (POD)-mimetic activity and potent radiosensitization to advance radioimmunotherapy. Density functional theory (DFT) calculations reveal that DAzymes lower energy barrier increase substrate affinity, enabling highly efficient catalytic performance. Within TME, these efficiently convert overexpressed hydrogen peroxide (H2O2) into hydroxyl radicals (•OH), potentially activating cGAS-STING immune pathway. This POD-mimetic catalysis is further accelerated under X-ray irradiation, significantly enhancing radiosensitization. Additionally, a uniform coating of ultrasmall gold nanoparticles on enhances absorption cancer cells. The incorporation STING agonist diABZI onto induces long-term antitumor immunity, reprograms immunosuppressive suppresses growth metastasis following single low-dose treatment. work highlights valuable strategy designing radiodynamic immunotherapy.

Язык: Английский

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