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1.
Nanoscale ; 2024 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-38629997

RESUMO

Precise monitoring and quantification of H2O2 is highly urgent and of great significance for biomedicine, food safety, environmental monitoring, etc. Herein, we proposed a facile near-infrared (NIR) excited fluorescent probe composed of upconversion nanoparticles (UCNPs) and non-metallic plasmonic WO3-x for ultrasensitive quantitative H2O2 detection. Plasmonic WO3-x with oxygen vacancy-induced LSPR achieved over 680-fold enhancement of upconversion fluorescence at 520 nm, and also acts as the sensitive recognition site for H2O2. H2O2 quenched the LSPR band of plasmonic WO3-x, further significantly influencing adjacent fluorescence signals depending on its concentration. The probe exhibits a good linear response to H2O2 with a low detection limit (10-9 M) and a wide concentration range (0-50 µM), and shows satisfactory application in the determination of H2O2 in blood and milk. This work may provide new ideas for the development of non-invasive fluorescent nanoprobes and plasmon-assisted biochemical detection methods.

2.
Adv Sci (Weinh) ; : e2308040, 2024 Apr 05.
Artigo em Inglês | MEDLINE | ID: mdl-38581142

RESUMO

The shortage and unevenness of fossil energy sources are affecting the development and progress of human civilization. The technology of efficiently converting material resources into energy for utilization and storage is attracting the attention of researchers. Environmentally friendly biomass materials are a treasure to drive the development of new-generation energy sources. Electrochemical theory is used to efficiently convert the chemical energy of chemical substances into electrical energy. In recent years, significant progress has been made in the development of green and economical electrocatalysts for oxygen reduction reaction (ORR). Although many reviews have been reported around the application of biomass-derived catalytically active carbon (CAC) catalysts in ORR, these reviews have only selected a single/partial topic (including synthesis and preparation of catalysts from different sources, structural optimization, or performance enhancement methods based on CAC catalysts, and application of biomass-derived CACs) for discussion. There is no review that systematically addresses the latest progress in the synthesis, performance enhancement, and applications related to biomass-derived CAC-based oxygen reduction electrocatalysts synchronously. This review fills the gap by providing a timely and comprehensive review and summary from the following sections: the exposition of the basic catalytic principles of ORR, the summary of the chemical composition and structural properties of various types of biomass, the analysis of traditional and the latest popular biomass-derived CAC synthesis methods and optimization strategies, and the summary of the practical applications of biomass-derived CAC-based oxidative reduction electrocatalysts. This review provides a comprehensive summary of the latest advances to provide research directions and design ideas for the development of catalyst synthesis/optimization and contributes to the industrialization of biomass-derived CAC electrocatalysis and electric energy storage.

3.
Nano Lett ; 2024 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-38602330

RESUMO

The miniaturization of biomedical microrobots is crucial for their in vivo applications. However, it is challenging to reduce their size while maintaining their biomedical functions. To resolve this contradiction, we propose a semiphysical design concept for developing miniaturized microrobots, in which invisible components such as light beams are utilized to replace most of the physical parts of a microrobot, thus minimizing its physical size without sacrificing its biomedical functions. According to this design, we have constructed a semiphysical microrobot (SPM) composed of main light beam, light-responsive microparticle, and auxiliary light beam, serving as the actuation system, recognition part, and surgical claws, respectively. Based on the functions of actuation, biosensing, and microsurgery, a SPM has been applied for a series of applications, including thrombus elimination at the branch vessel, stratified removal of multilayer thrombus, and biosensing-guided microsurgery. The proposed semiphysical design concept should bring new insight into the development of miniaturized biomedical microrobots.

4.
Angew Chem Int Ed Engl ; 63(16): e202319983, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38404154

RESUMO

Herein, an interfacial electron redistribution is proposed to boost the activity of carbon-supported spinel NiCo2O4 catalyst toward oxygen conversion via Fe, N-doping strategy. Fe-doping into octahedron induces a redistribution of electrons between Co and Ni atoms on NiCo1.8Fe0.2O4@N-carbon. The increased electron density of Co promotes the coordination of water to Co sites and further dissociation. The generation of proton from water improves the overall activity for the oxygen reduction reaction (ORR). The increased electron density of Ni facilitates the generation of oxygen vacancies. The Ni-VO-Fe structure accelerates the deprotonation of *OOH to improve the activity toward oxygen evolution reaction (OER). N-doping modulates the electron density of carbon to form active sites for the adsorption and protonation of oxygen species. Fir wood-derived carbon endows catalyst with an integral structure to enable outstanding electrocatalytic performance. The NiCo1.8Fe0.2O4@N-carbon express high half-wave potential up to 0.86 V in ORR and low overpotential of 270 mV at 10 mA cm-2 in OER. The zinc-air batteries (ZABs) assembled with the as-prepared catalyst achieve long-term cycle stability (over 2000 cycles) with peak power density (180 mWcm-2). Fe, N-doping strategy drives the catalysis of biomass-derived carbon-based catalysts to the highest level for the oxygen conversion in ZABs.

5.
ChemSusChem ; : e202301779, 2024 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-38416074

RESUMO

Given the growing environmental and energy problems, developing clean, renewable electrochemical energy storage devices is of great interest. Zn-air batteries (ZABs) have broad prospects in energy storage because of their high specific capacity and environmental friendliness. The unavailability of cheap air electrode materials and effective and stable oxygen electrocatalysts to catalyze air electrodes are main barriers to large-scale implementation of ZABs. Due to the abundant biomass resources, self-doped heteroatoms, and unique pore structure, biomass-derived catalytically active carbon materials (CACs) have great potential to prepare carbon-based catalysts and porous electrodes with excellent performance for ZABs. This paper reviews the research progress of biomass-derived CACs applied to ZABs air electrodes. Specifically, the principle of ZABs and the source and preparation method of biomass-derived CACs are introduced. To prepare efficient biomass-based oxygen electrocatalysts, heteroatom doping and metal modification were introduced to improve the efficiency and stability of carbon materials. Finally, the effects of electron transfer number and H2 O2 yield in ORR on the performance of ZABs were evaluated. This review aims to deepen the understanding of the advantages and challenges of biomass-derived CACs in the air electrodes of ZABs, promote more comprehensive research on biomass resources, and accelerate the commercial application of ZABs.

6.
iScience ; 27(3): 109064, 2024 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-38375219

RESUMO

Titanium silicate zeolite (TS-1) is widely used in the research on selective oxidations of organic substrates by H2O2. Compared with the chlorohydrin process and the hydroperoxidation process, the TS-1 catalyzed hydroperoxide epoxidation of propylene oxide (HPPO) has advantages in terms of by-products and environmental friendliness. This article reviews the latest progress in propylene epoxidation catalyzed by TS-1, including the HPPO process and gas phase epoxidation. The preparation and modification of TS-1 for green and sustainable production are summarized, including the use of low-cost feedstocks, the development of synthetic routes, strategies to enhance mass transfer in TS-1 crystal and the enhancement of catalytic performance after modification. In particular, this article summarizes the catalytic mechanisms and advanced characterization techniques for propylene epoxidation in recent years. Finally, the present situation, development prospect and challenge of propylene epoxidation catalyzed by TS-1 were prospected.

7.
J Colloid Interface Sci ; 660: 792-799, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38277836

RESUMO

Non-precious metals have shown attractive catalytic prospects in hydrogen production from ammonia borane hydrolysis. However, the sluggish reaction kinetics in the hydrolysis process remains a challenge. Herein, P-bridged Fe-X-Co coupled sites in hollow carbon spheres (Fe-CoP@C) has been synthesized through in situ template solvothermal and subsequent surface-phosphorization. Benefiting from the optimized electronic structure induced by Fe doping to enhance the specific activity of Co sites, bimetallic synergy and hollow structure, the as-prepared Fe-CoP@C exhibits superior performances with a turnover frequency (TOF) of 183.5 min-1, and stability of over 5 cycles for ammonia borane hydrolysis, comparable to noble metal catalysts. Theoretical calculations reveal that the P-bridged Fe-X-Co coupled sites on the Fe-CoP@C catalyst surfaces is beneficial to adsorb reactant molecules and reduce their reaction barrier. This strategy of constructing hollow P-bridged bimetallic coupled sites may open new avenues for non-precious metal catalysis.

8.
Angew Chem Int Ed Engl ; 63(4): e202316550, 2024 Jan 22.
Artigo em Inglês | MEDLINE | ID: mdl-38038407

RESUMO

Single-atom alloys (SAAs), combining the advantages of single-atom and nanoparticles (NPs), play an extremely significant role in the field of heterogeneous catalysis. Nevertheless, understanding the catalytic mechanism of SAAs in catalysis reactions remains a challenge compared with single atoms and NPs. Herein, ruthenium-nickel SAAs (RuNiSAAs ) synthesized by embedding atomically dispersed Ru in Ni NPs are anchored on two-dimensional Ti3 C2 Tx MXene. The RuNiSAA-3 -Ti3 C2 Tx catalysts exhibit unprecedented activity for hydrogen evolution from ammonia borane (AB, NH3 BH3 ) hydrolysis with a mass-specific activity (rmass ) value of 333 L min-1 gRu -1 . Theoretical calculations reveal that the anchoring of SAAs on Ti3 C2 Tx optimizes the dissociation of AB and H2 O as well as the binding ability of H* intermediates during AB hydrolysis due to the d-band structural modulation caused by the alloying effect and metal-supports interactions (MSI) compared with single atoms and NPs. This work provides useful design principles for developing and optimizing efficient hydrogen-related catalysts and demonstrates the advantages of SAAs over NPs and single atoms in energy catalysis.

9.
Nano Lett ; 24(2): 566-575, 2024 Jan 17.
Artigo em Inglês | MEDLINE | ID: mdl-37962055

RESUMO

Optical biosensors based on micro/nanofibers are highly valuable for probing and monitoring liquid environments and bioactivity. Most current optical biosensors, however, are still based on glass, semiconductors, or metallic materials, which might not be fully suitable for biologically relevant environments. Here, we introduce biocompatible and flexible microfibers from lotus silk as microenvironmental monitors that exhibit waveguiding of intrinsic fluorescence as well as of coupled light. These features make single-filament monitors excellent building blocks for a variety of sensing functions, including pH probing and detection of bacterial activity. These results pave the way for the development of new and entirely eco-friendly, potentially multiplexed biosensing platforms.


Assuntos
Técnicas Biossensoriais , Nanofibras , Técnicas Biossensoriais/métodos , Seda , Semicondutores , Bactérias
10.
Small Methods ; 8(1): e2301112, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37880897

RESUMO

The active delivery of nanodrugs has been a bottleneck problem in nanomedicine. While modification of nanodrugs with targeting agents can enhance their retention at the lesion location, the transportation of nanodrugs in the circulation system is still a passive process. The navigation of nanodrugs with external forces such as magnetic field has been shown to be effective for active delivery, but the existing techniques are limited to specific materials like magnetic nanoparticles. In this study, an alternative actuation method is proposed based on optical manipulation for remote navigation of nanodrugs in vivo, which is compatible with most of the common drug carriers and exhibits significantly higher manipulation precision. By the programmable scanning of the laser beam, the motion trajectory and velocity of the nanodrugs can be precisely controlled in real time, making it possible for intelligent drug delivery, such as inverse-flow transportation, selective entry into specific vascular branch, and dynamic circumvention across obstacles. In addition, the controlled mass delivery of nanodrugs can be realized through indirect actuation by the microflow field. The developed optical manipulation method provides a new solution for the active delivery of nanodrugs, with promising potential for the treatment of blood diseases such as leukemia and thrombosis.


Assuntos
Portadores de Fármacos , Nanopartículas , Sistemas de Liberação de Medicamentos , Nanomedicina/métodos , Luz
11.
J Comput Assist Tomogr ; 48(1): 137-142, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-37531643

RESUMO

OBJECTIVE: To investigate the utility of texture analysis in detecting osseous changes associated with hyperparathyroidism on neck CT examinations compared with control patients and to explore the best regions in the head and neck to evaluate changes in the trabecular architecture secondary to hyperparathyroidism. METHODS: Patients with hyperparathyroidism who underwent a 4D CT of the neck with contrast were included in this study. Age-matched control patients with no history of hyperparathyroidism who underwent a contrast-enhanced neck CT were also included. Mandibular condyles, bilateral mandibular bodies, the body of the C4 vertebra, the manubrium of the sternum, and bilateral clavicular heads were selected for analysis, and oval-shaped regions of interest were manually placed. These segmented areas were imported into an in-house developed texture analysis program, and 41 texture analysis features were extracted. A mixed linear regression model was used to compare differences in the texture analysis features contoured at each of the osseous structures between patients with hyperparathyroidism and age-matched control patients. RESULTS: A total of 30 patients with hyperparathyroidism and 30 age-matched control patients were included in this study. Statistically significant differences in texture features between patients with hyperparathyroidism and control patients in all 8 investigated osseous regions. The sternum showed the greatest number of texture features with statistically significant differences between these groups. CONCLUSIONS: Some CT texture features demonstrated statistically significant differences between patients with hyperparathyroidism and control patients. The results suggest that texture features may discriminate changes in the osseous architecture of the head and neck in patients with hyperparathyroidism.


Assuntos
Hiperparatireoidismo Primário , Humanos , Hiperparatireoidismo Primário/diagnóstico por imagem , Estudos Retrospectivos , Tomografia Computadorizada Quadridimensional
12.
Small ; 20(4): e2305782, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37718497

RESUMO

Due to their unique electronic and structural properties, single-atom catalytic materials (SACMs) hold great promise for the oxygen reduction reaction (ORR). Coordinating environmental and engineering strategies is the key to improving the ORR performance of SACMs. This review summarizes the latest research progress and breakthroughs of SACMs in the field of ORR catalysis. First, the research progress on the catalytic mechanism of SACMs acting on ORR is reviewed, including the latest research results on the origin of SACMs activity and the analysis of pre-adsorption mechanism. The study of the pre-adsorption mechanism is an important breakthrough direction to explore the origin of the high activity of SACMs and the practical and theoretical understanding of the catalytic process. Precise coordination environment modification, including in-plane, axial, and adjacent site modifications, can enhance the intrinsic catalytic activity of SACMs and promote the ORR process. Additionally, several engineering strategies are discussed, including multiple SACMs, high loading, and atomic site confinement. Multiple SACMs synergistically enhance catalytic activity and selectivity, while high loading can provide more active sites for catalytic reactions. Overall, this review provides important insights into the design of advanced catalysts for ORR.

13.
Small Methods ; 8(1): e2301105, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37818749

RESUMO

Optical manipulation has emerged as a pivotal tool in soft matter research, offering superior applicability, spatiotemporal precision, and manipulation capabilities compared to conventional methods. Here, an overview of the optical mechanisms governing the interaction between light and soft matter materials during manipulation is provided. The distinct characteristics exhibited by various soft matter materials, including liquid crystals, polymers, colloids, amphiphiles, thin liquid films, and biological soft materials are highlighted, and elucidate their fundamental response characteristics to optical manipulation techniques. This knowledge serves as a foundation for designing effective strategies for soft matter manipulation. Moreover, the diverse range of applications and future prospects that arise from the synergistic collaboration between optical manipulation and soft matter materials in emerging fields are explored.

14.
J Colloid Interface Sci ; 658: 22-31, 2024 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-38091795

RESUMO

Designing non-precious catalysts to synergistically achieve a facilitated exposure of abundant active sites is highly desired but remains a significant challenge. Herein, a hetero-structured catalyst CoP-Co supported on porous g-C3N4 nanosheets (CoP-Co/CN-I) was prepared by pyrolysis and P-inducing strategy. The optimal catalyst achieves a turnover frequency (TOF) of 26 min-1 at room temperature and the apparent activation energy (Ea) is 35.5 kJ·mol-1. The catalytic activity is ranked top among the non-precious metal phosphides or the other supports. Meanwhile, the catalytic activity has no significant decrease even after 5 cycles. The CoP/Co interfaces provide richly exposed active sites, optimize hydrogen/water absorption free energy via electronic coupling, and thus improve the catalytic activity. The experimental results reveal that the CoP/Co heterojunction improves the catalytic activity due to the construction of dual-active sites. This research facilitates the innovative construction of non-noble metal catalysts to meet industrial demand for heterogeneous catalysis.

15.
Small ; : e2306369, 2023 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-38054776

RESUMO

Cobalt sulfide is deemed a promising anode material, owing to its high theoretical capacity (630 mAh g-1 ). Due to its low conductivity, fast energy decay, and the huge volume change during the lithiation process limits its practical application. In this work, a simple and large-scale method are developed to prepare Co1-x S nanoparticles embedding in N-doped carbon/graphene (CSCG). At a current density of 0.2 C, the reversible discharge capacity of CSCG maintains 937 mAh g-1 after 200 cycles. The discharge capacity of CSCG maintains at 596 mAh g-1 after 500 cycles at the high current density of 2.0 C. The excellent performance of CSCG is due to its unique structural features. The addition of rGO buffered volume changes while preventing Co1-x S from crushing/aggregating during the cycle, resulting in multiplier charge-discharge and long cycle life. The N-doped carbon provides a simple and easy way to achieve excellent performance in practical applications. Combined with density functional theory calculation, the presence of Co-vacancies(Co1-x ) increases more active site. Moreover, N-doping carbon is beneficial to the improve adsorption energy. This work presents a simple and effective structural engineering strategy and also provides a new idea to improve the performance of Li-ion batteries.

16.
Small ; : e2307662, 2023 Dec 10.
Artigo em Inglês | MEDLINE | ID: mdl-38072770

RESUMO

The problem in d-band center modulation of transition metal-based catalysts for the rate-determining steps of oxygen conversion is an obstacle to boost the electrocatalytic activity by accelerating proton coupling. Herein, the Co doping to FeP is adopted to modify the d-band center of Fe. Optimized Fe sites accelerate the proton coupling of oxygen reduction reaction (ORR) on N-doped wood-derived carbon through promoting water dissociation. In situ generated Fe sites optimize the adsorption of oxygen-related intermediates of oxygen evolution reaction (OER) on CoFeP NPs. Superior catalytic activity toward ORR (half-wave potential of 0.88 V) and OER (overpotential of 300 mV at 10 mA cm-2 ) express an unprecedented level in carbon-based transition metal-phosphide catalysts. The liquid zinc-air battery presents an outstanding cycling stability of 800 h (2400 cycles). This research offers a newfangled perception on designing highly efficient carbon-based bifunctional catalysts for ORR and OER.

17.
Small ; : e2305405, 2023 Dec 10.
Artigo em Inglês | MEDLINE | ID: mdl-38072804

RESUMO

As the cleanest energy source, hydrogen has been followed with interest by researchers around the world. However, due to the internal low density of hydrogen, it cannot be stored and used efficiently which limits the hydrogen application on a huge scale. Chemical hydrogen storage is considered as a useful method for efficient handling and storage. Due to its excellent safety, formic acid stands out. It is worth noting that the matter and energy conversion is established based on formic acid, which is not referred to in the previous documentation. In this review, the latest development of research on heterogeneous catalysis via production and application of formic acid for energy application is reported. The matter and energy conversion based on formic acid are both discussed systematically. More importantly, with formic acid as the node, biomass energy shows potential to be in a dominant position in the energy conversion process. In addition, the catalytic mechanism is also mentioned. This review can provide the current state in this field and the new inspirations for developing superior catalytic systems.

18.
Stud Health Technol Inform ; 308: 696-704, 2023 Nov 23.
Artigo em Inglês | MEDLINE | ID: mdl-38007801

RESUMO

Chronic obstructive pulmonary disease (COPD) is a common respiratory disease with high incidence in the world. Its main feature is that the lungs are affected by airflow obstruction. The disease can lead to impaired lung function in adults and cannot be completely cured. This paper expounds the pathogenesis of COPD, which can be alleviated by chemical methods and TCM methods. TCM treatment of COPD has the advantage of overall regulation, which can improve airway remodeling and alleviate the development of the disease. According to their structure, TCM therapeutic drugs can be divided into flavonoids, terpenoids, phenylpropanoids and alkaloids. On this basis, the article summarizes the advantages and disadvantages of common Chinese medicine administration methods, aiming to provide some reference and help when alleviating the disease.


Assuntos
Medicamentos de Ervas Chinesas , Doença Pulmonar Obstrutiva Crônica , Adulto , Humanos , Medicina Tradicional Chinesa , Doença Pulmonar Obstrutiva Crônica/tratamento farmacológico , Pulmão , Medicamentos de Ervas Chinesas/uso terapêutico
19.
Front Radiol ; 3: 1187449, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37810756

RESUMO

Purpose: The purpose of this study is to utilize a two-material decomposition to quantify bone marrow edema on a dual-energy computed tomography (DECT) scanner at the cervical, thoracic, and lumbar spine acute fractures in correlation with short tau inversion recovery (STIR) hyperintensity on magnetic resonance imaging (MRI) in comparison with the normal bone marrow. Materials and methods: This retrospective institutional review board-approved study gathered patients over 18 years old who had acute cervical, thoracic, or lumbar spinal fractures scanned on a DECT scanner. Those who had a spinal MRI done with bone marrow STIR hyperintensity within 3 weeks of the DECT were included. The water (calcium) and fat (calcium) density (mg/cm3) measurements of the region of interest of the bone marrow were obtained at a normal anatomic equivalent site and at the fracture site where STIR hyperintensity was noted on MRI. A statistical analysis was performed using the paired t-test and Wilcoxon signed rank test (p > 0.05). Results: A total of 20 patients met the inclusion criteria (males n = 17 males, females n = 3). A total of 32 fractures were analyzed: 19 cervical and 13 thoracolumbar. There were statistically significant differences in the water (43 ± 24 mg/cm3) and fat (36 ± 31 mg/cm3) density (mg/cm3) at the acute thoracic and lumbar spine fractures in correlation with edema on STIR images (both paired t-test <0.001, both Wilcoxon signed ranked test p < 0.01). There were no significant differences in the water (-10 ± 46 mg/cm3) or fat (+7 ± 50 mg/cm3) density (mg/cm3) at the cervical spine fractures. Conclusion: The DECT two-material decomposition using water (calcium) and fat (calcium) analyses has the ability to quantify a bone marrow edema at the acute fracture site in the thoracic and lumbar spine.

20.
Adv Sci (Weinh) ; 10(32): e2304103, 2023 11.
Artigo em Inglês | MEDLINE | ID: mdl-37749869

RESUMO

With high reconfigurability and swarming intelligence, programmable medical micromachines (PMMs) represent a revolution in microrobots for executing complex coordinated tasks, especially for dynamic routing of various targets along their respective routes. However, it is difficult to achieve a biocompatible implantation into the body due to their exogenous building blocks. Herein, a living microrouter based on an organic integration of endogenous red blood cells (RBCs), programmable scanning optical tweezers and flexible optofluidic strategy is reported. By harvesting energy from a designed optical force landscape, five RBCs are optically rotated in a controlled velocity and direction, under which, a specific actuation flow is achieved to exert the well-defined hydrodynamic forces on various biological targets, thus enabling a selective routing by integrating three successive functions, i.e., dynamic input, inner processing, and controlled output. Benefited from the optofluidic manipulation, various blood cells, such as the platelets and white blood cells, are transported toward the damaged vessel and cell debris for the dynamic hemostasis and targeted clearance, respectively. Moreover, the microrouter enables a precise transport of nanodrugs for active and targeted delivery in a large quantity. The proposed RBC microrouter might provide a biocompatible medical platform for cell separation, drug delivery, and immunotherapy.


Assuntos
Eritrócitos , Pinças Ópticas , Plaquetas , Sistemas de Liberação de Medicamentos
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