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1.
Nat Immunol ; 23(3): 423-430, 2022 03.
Artigo em Inglês | MEDLINE | ID: mdl-35228696

RESUMO

The global severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) pandemic requires effective therapies against coronavirus disease 2019 (COVID-19), and neutralizing antibodies are a promising therapy. A noncompeting pair of human neutralizing antibodies (B38 and H4) blocking SARS-CoV-2 binding to its receptor, ACE2, have been described previously. Here, we develop bsAb15, a bispecific monoclonal antibody (bsAb) based on B38 and H4. bsAb15 has greater neutralizing efficiency than these parental antibodies, results in less selective pressure and retains neutralizing ability to most SARS-CoV-2 variants of concern (with more potent neutralizing activity against the Delta variant). We also selected for escape mutants of the two parental mAbs, a mAb cocktail and bsAb15, demonstrating that bsAb15 can efficiently neutralize all single-mAb escape mutants. Furthermore, prophylactic and therapeutic application of bsAb15 reduced the viral titer in infected nonhuman primates and human ACE2 transgenic mice. Therefore, this bsAb is a feasible and effective strategy to treat and prevent severe COVID-19.


Assuntos
Anticorpos Biespecíficos/imunologia , Anticorpos Monoclonais/imunologia , Anticorpos Antivirais/imunologia , SARS-CoV-2/imunologia , Animais , Anticorpos Biespecíficos/química , Anticorpos Biespecíficos/genética , Anticorpos Monoclonais/química , Anticorpos Monoclonais/genética , Anticorpos Neutralizantes/genética , Anticorpos Neutralizantes/imunologia , Anticorpos Antivirais/química , Anticorpos Antivirais/genética , COVID-19/imunologia , COVID-19/patologia , COVID-19/prevenção & controle , COVID-19/virologia , Clonagem Molecular , Modelos Animais de Doenças , Relação Dose-Resposta Imunológica , Epitopos , Humanos , Macaca mulatta , Camundongos , Testes de Neutralização , Engenharia de Proteínas/métodos , Relação Estrutura-Atividade
2.
Nature ; 610(7933): 661-666, 2022 10.
Artigo em Inglês | MEDLINE | ID: mdl-36198794

RESUMO

Networks of optical clocks find applications in precise navigation1,2, in efforts to redefine the fundamental unit of the 'second'3-6 and in gravitational tests7. As the frequency instability for state-of-the-art optical clocks has reached the 10-19 level8,9, the vision of a global-scale optical network that achieves comparable performances requires the dissemination of time and frequency over a long-distance free-space link with a similar instability of 10-19. However, previous attempts at free-space dissemination of time and frequency at high precision did not extend beyond dozens of kilometres10,11. Here we report time-frequency dissemination with an offset of 6.3 × 10-20 ± 3.4 × 10-19 and an instability of less than 4 × 10-19 at 10,000 s through a free-space link of 113 km. Key technologies essential to this achievement include the deployment of high-power frequency combs, high-stability and high-efficiency optical transceiver systems and efficient linear optical sampling. We observe that the stability we have reached is retained for channel losses up to 89 dB. The technique we report can not only be directly used in ground-based applications, but could also lay the groundwork for future satellite time-frequency dissemination.

3.
Proc Natl Acad Sci U S A ; 120(52): e2314193120, 2023 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-38109549

RESUMO

Currently, monoclonal antibodies (MAbs) targeting the SARS-CoV-2 receptor binding domain (RBD) of spike (S) protein are classified into seven classes based on their binding epitopes. However, most of these antibodies are seriously impaired by SARS-CoV-2 Omicron and its subvariants, especially the recent BQ.1.1, XBB and its derivatives. Identification of broadly neutralizing MAbs against currently circulating variants is imperative. In this study, we identified a "breathing" cryptic epitope in the S protein, named as RBD-8. Two human MAbs, BIOLS56 and IMCAS74, were isolated recognizing this epitope with broad neutralization abilities against tested sarbecoviruses, including SARS-CoV, pangolin-origin coronaviruses, and all the SARS-CoV-2 variants tested (Omicron BA.4/BA.5, BQ.1.1, and XBB subvariants). Searching through the literature, some more RBD-8 MAbs were defined. More importantly, BIOLS56 rescues the immune-evaded antibody, RBD-5 MAb IMCAS-L4.65, by making a bispecific MAb, to neutralize BQ.1 and BQ.1.1, thereby producing an MAb to cover all the currently circulating Omicron subvariants. Structural analysis reveals that the neutralization effect of RBD-8 antibodies depends on the extent of epitope exposure, which is affected by the angle of antibody binding and the number of up-RBDs induced by angiotensin-converting enzyme 2 binding. This cryptic epitope which recognizes non- receptor binding motif (non-RBM) provides guidance for the development of universal therapeutic antibodies and vaccines against COVID-19.


Assuntos
COVID-19 , SARS-CoV-2 , Humanos , Vacinas contra COVID-19 , Anticorpos Monoclonais , Epitopos , Anticorpos Neutralizantes , Anticorpos Antivirais , Glicoproteína da Espícula de Coronavírus
4.
Chem Soc Rev ; 53(6): 3002-3035, 2024 Mar 18.
Artigo em Inglês | MEDLINE | ID: mdl-38353930

RESUMO

Heterojunctions combining two photocatalysts of staggered conduction and valence band energy levels can increase the photocatalytic efficiency compared to their individual components. This activity enhancement is due to the minimization of undesirable charge recombination by the occurrence of carrier migration through the heterojunction interface with separated electrons and holes on the reducing and oxidizing junction component, respectively. Metal-organic frameworks (MOFs) are currently among the most researched photocatalysts due to their tunable light absorption, facile charge separation, large surface area and porosity. The present review summarizes the current state-of-the-art in MOF-based heterojunctions, providing critical comments on the construction of these heterostructures. Besides including examples showing the better performance of MOF heterojunctions for three important photocatalytic processes, such as hydrogen evolution reaction, CO2 photoreduction and dye decolorization, the focus of this review is on describing synthetic procedures to form heterojunctions with MOFs and on discussing the experimental techniques that provide evidence for the operation of charge migration between the MOF and the other component. Special attention has been paid to the design of rational MOF heterojunctions with small particle size and controlled morphology for an appropriate interfacial contact. The final section summarizes the achievements of the field and provides our views on future developments.

5.
Nano Lett ; 2024 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-38856112

RESUMO

Electrical manipulation of magnetic states in two-dimensional ferromagnetic systems is crucial in information storage and low-dimensional spintronics. Spin-orbit torque presents a rapid and energy-efficient method for electrical control of the magnetization. In this letter, we demonstrate a wafer-scale spin-orbit torque switching of two-dimensional ferromagnetic states. Using molecular beam epitaxy, we fabricate two-dimensional heterostructures composed of low crystal-symmetry WTe2 and ferromagnet CrTe2 with perpendicular anisotropy. By utilizing out-of-plane spins generated from WTe2, we achieve field-free switching of the CrTe2 perpendicular magnetization. The threshold switching current density in CrTe2/WTe2 is 1.2 × 106 A/cm2, 20 times smaller than that of the CrTe2/Pt control sample even with an external magnetic field. In addition, the switching behavior can be modulated by external magnetic fields and crystal symmetry. Our findings demonstrate a controllable and all-electric manipulation of perpendicular magnetization in a two-dimensional ferromagnet, representing a significant advancement toward the practical implementation of low-dimensional spintronic devices.

6.
Anal Chem ; 96(4): 1733-1741, 2024 01 30.
Artigo em Inglês | MEDLINE | ID: mdl-38227423

RESUMO

Exosomal miRNAs are considered promising biomarkers for cancer diagnosis, but their accuracy is severely compromised by the low content of miRNAs and the large amount of exosomal miRNAs released from normal cells. Here, we presented a dual-specific miRNA's logical recognition triggered by an entropy-driven catalysis (EDC)-enhanced system in exosomes for accurate detection of liver cancer-cell-derived exosomal miR-21 and miR-122. Taking advantage of the accurate analytical performance of the logic device, the excellent membrane penetration of gold nanoparticles, and the outstanding amplification ability of the EDC reaction, this method exhibits high sensitivity and selectivity for the detection of tumor-derived exosomal miRNAs in situ. Moreover, due to its excellent performance, this logic device can effectively distinguish liver cancer patients from healthy donors by determining the amount of cancer-cell-derived exosomal miRNAs. Overall, this strategy has great potential for analyzing various types of exosomes and provides a viable tool to improve the accuracy of cancer diagnosis.


Assuntos
Exossomos , Neoplasias Hepáticas , Nanopartículas Metálicas , MicroRNAs , Humanos , MicroRNAs/genética , Ouro , Entropia , Exossomos/genética , DNA , Neoplasias Hepáticas/diagnóstico , Lógica
7.
Small ; 20(25): e2311240, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38299719

RESUMO

Shape memory hydrogels provide a worldwide scope for functional soft materials. However, most shape memory hydrogels exhibit poor mechanical properties, leading to low actuation strength, which severely limits their applications in smart biomimetic devices. Herein, a strategy for muscle-inspired shape memory-oriented polyvinyl alcohol (PVA)-natural rubber latex (NRL) hydrogel (OPNH) with multiscale oriented structure is demonstrated. The shape memory function comes from the stretch-induced crystallization of natural rubber (NR), while PVA forms strong hydrogen bonding interactions with proteins and phospholipids on the surface of NRL particles. Meanwhile, the reconfigurable interactions of PVA and NR produce a multiscale-oriented structure during stretch-drying, improving the mechanical and shape memory properties. The resultant OPNH shows excellent interfacial compatibility, exhibiting outstanding mechanical performance (3.2 MPa), high shape fixity (≈80%) and shape recovery ratio (≈92%), high actuation strength (206 kPa), working capacity (105 kJ m- 3), extremely short response time (≈2 s), low response temperature (28 °C) and smart thermal responsiveness. It can even maintain muscle-like working capacity when lifting a load equivalent to 372 times its weight, providing a new class shape memory material for the application in smart biomimetic muscles and multistimulus responsive devices.

8.
Opt Express ; 32(6): 9128-9138, 2024 Mar 11.
Artigo em Inglês | MEDLINE | ID: mdl-38571153

RESUMO

High-speed optical polarization characterization is highly desirable for a wide range of applications, including remote sensing, telecommunication, and medical diagnosis. The utilization of the Mueller matrix provides a superior systematic and comprehensive approach to represent polarization attributes when matter interacts with optical beams. However, the current measurement speed of Mueller matrix is limited to only seconds or milliseconds. In this study, we present an ultrafast Mueller matrix polarimetry (MMP) technique based on optical time-stretch and spectral encoding that enables us to achieve an impressive temporal resolution of 4.83 nanoseconds for accurate Mueller matrix measurements. The unique feature of optical time-stretch technology enables continuous, ultrafast single-shot spectroscopy, resulting in a remarkable speed of up to 207 MHz for spectral encoding Mueller matrix measurement. We have employed an effective Mueller linear reconstruction algorithm based on the measured modulation matrix, accounting for all potential non-ideal effects of polarization components like retardance error and azimuth error. To ensure high precision, prior to the actual measurement, high-order dispersion induced by time-stretch requires adjustment through proper modulation matrix design. Upon such correction, both the results of static and rapid dynamic samples measurements exhibit exceptional accuracy with root-mean-square error (RMSE) approximately equal to 0.04 and 0.07 respectively. This presented ultrafast MMP provides a significant advance over preceding endeavors, enabling superior accuracy and increased speed concurrently.

9.
Opt Lett ; 49(5): 1221-1224, 2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38426978

RESUMO

This paper reports an optical strain sensor that integrates a self-powered mechanoluminescent (ML) elastic fiber with a flexible circuit. The inclusion of an alumina nanoparticle as the additive results in seven-fold enhancement of ML intensity while maintaining flexibility of 120% strain. The sensor facilitates the detection of strain and stretching speed. It attains a sensitivity of 0.0022 lx/(1% strain) and a resolution of 0.2% strain, respectively. We have successfully applied it to detect bending motions of the finger, wrist, and elbow. This wearable strain sensor holds promise for diverse applications in wearable technology.

10.
Opt Lett ; 49(11): 3082-3085, 2024 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-38824333

RESUMO

In this Letter, we experimentally investigate a non-line-of-sight (NLOS) optical wireless communication (OWC) system that utilizes wavefront shaping techniques to realize simultaneous data transmission for multiple users. Wavefront shaping techniques are employed to address the issue of low intensity of diffusely reflected light at the receiver in NLOS scenarios for indoor high-speed access. To achieve communication path planning and tracing for two different users in free-space optical communication, the pixels of the spatial light modulator (SLM) are divided into two halves to separately manipulate the wavefront of two independent data carriers centered at different wavelengths. The maximum received optical power can be effectively improved by more than 15 dB with the wavefront shaping technique. To avoid power enhancement of non-target wavelength, the wavelength difference of two different users is experimentally studied. The difference in power enhancement ratio (DPER) is increased with the wavelength difference, and 14.95 dB DPER is obtained with a 10 nm wavelength difference. Under the aforementioned wavelength planning strategy, successful transmission and reception of 2 × 160 Gbit/s 16-QAM signals for two users with coherent detection is achieved using wavelengths of 1550 and 1560 nm in an indoor access scenario.

11.
J Magn Reson Imaging ; 2024 Mar 27.
Artigo em Inglês | MEDLINE | ID: mdl-38544434

RESUMO

BACKGROUND: The fasting-postprandial state remains an underrecognized confounding factor for quantifying cerebral blood flow (CBF) in the cognitive assessment and differential diagnosis of Alzheimer's disease (AD). PURPOSE: To investigate the effects of fasting-postprandial state on arterial spin labeling (ASL)-based CBF in AD patients. STUDY TYPE: Prospective. SUBJECTS: Ninety-two subjects (mean age = 62.5 ± 6.4 years; females 29.3%), including 30 with AD, 32 with mild cognitive impairment (MCI), and 30 healthy controls (HCs). Differential diagnostic models were developed with a 4:1 training to testing set ratio. FIELD STRENGTH/SEQUENCE: 3-T, T1-weighted imaging using gradient echo and pseudocontinuous ASL imaging using turbo spin echo. ASSESSMENT: Two ASL scans were acquired to quantify fasting state and postprandial state regional CBFs based on an automated anatomical labeling atlas. Two-way ANOVA was used to assess the effects of fasting/postprandial state and disease state (AD, MCI, and HC) on regional CBF. Pearson's correlation analysis was conducted between regional CBF and cognitive scores (Mini-Mental State Examination [MMSE] and Montreal Cognitive Assessment [MoCA]). The diagnostic performances of the fasting state, postprandial state, and mixed state (random mixing of the fasting and postprandial state CBF) in differential diagnosis of AD were conducted using support vector machine and logistic regression models. STATISTICAL TESTS: Two-way ANOVA, Pearson's correlation, and area under the curve (AUC) of diagnostic model were performed. P values <0.05 indicated statistical significance. RESULTS: Fasting-state CBF was correlated with cognitive scores in more brain regions (17 vs. 4 [MMSE] and 15 vs. 9 [MoCA]) and had higher absolute correlation coefficients than postprandial-state CBF. In the differential diagnosis of AD patients from MCI patients and HCs, fasting-state CBF outperformed mixed-state CBF, which itself outperformed postprandial-state CBF. DATA CONCLUSION: Compared with postprandial CBF, fasting-state CBF performed better in terms of cognitive score correlations and in differentiating AD patients from MCI patients and HCs. EVIDENCE LEVEL: 2 TECHNICAL EFFICACY: Stage 3.

12.
Graefes Arch Clin Exp Ophthalmol ; 262(7): 2171-2179, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38329529

RESUMO

PURPOSE: To investigate the capacity of critical flicker frequency (CFF) in discriminating cataract eyes with or without macula disease using trichromatic flickers, and to develop a model to predict postoperative best corrected visual acuity (BCVA). METHODS: Patients were divided into two groups based on the presence or absence of macular disease. CFF threshold measurements of red (R-CFF), green (G-CFF), and yellow (Y-CFF) flickers were conducted both preoperatively and postoperatively. A generalized estimating equations model (GEE) was employed to examine the relationship between CFF threshold and 3-month postoperative BCVA. RESULTS: A total of 115 eyes were enrolled, with 59 eyes in the cataract alone group and 56 eyes in the cataract with macular disease group completing the follow-up. R-CFF was found to be consistent before and after cataract removal (P = 0.06), even in cases where OCT was not performed successfully (P > 0.05). Y-CFF showed the highest AUC (0.798) for differentiating ocular comorbidities. According to the GEE model, in patients with a CFF threshold below 26 Hz, the odds ratios for achieving a postoperative VA of 20/40 or better were 34.8% for R-CFF, 26.0% for G-CFF, and 24.5% for Y-CFF. CONCLUSION: CFF emerges as a promising tool for predicting postoperative BCVA, providing valuable supplementary insights when fundus examination is obstructed. R-CFF demonstrates the best resistance to cataracts, while Y-CFF exhibits the highest sensitivity both in identifying macular diseases and predicting postoperative BCVA of 20/40 or better.


Assuntos
Catarata , Acuidade Visual , Humanos , Feminino , Masculino , Catarata/fisiopatologia , Catarata/complicações , Catarata/diagnóstico , Acuidade Visual/fisiologia , Idoso , Pessoa de Meia-Idade , Macula Lutea/fisiopatologia , Macula Lutea/diagnóstico por imagem , Macula Lutea/patologia , Seguimentos , Doenças Retinianas/fisiopatologia , Doenças Retinianas/diagnóstico , Tomografia de Coerência Óptica/métodos , Curva ROC , Estudos Prospectivos , Testes Visuais/métodos
13.
BMC Womens Health ; 24(1): 240, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38622605

RESUMO

BACKGROUND: Human papillomavirus (HPV) infection is an important factor leading to cervical cell abnormalities. 90% of cervical cancers are closely associated with persistent infection of high-risk HPV, with the highest correlation with HPV16 and 18. Currently available vaccines and antivirals have limited effectiveness and coverage. Guanylate binding protein 1 (GBP1) was induced by interferon gamma and involved in many important cellular processes such as clearance of various microbial pathogens. However, whether GBP1 can inhibit human papillomavirus infection is unclear. RESULTS: In this study, we found that GBP1 can effectively degrade HPV18 E6, possibly through its GTPase activity or other pathways, and E6 protein degrades GBP1 through the ubiquitin-proteasome pathway to achieve immune escape. CONCLUSION: Therefore, GBP1 is an effector of IFN-γ anti-HPV activity. Our findings provided new insights into the treatment of HPV 18 infections.


Assuntos
Infecções por Papillomavirus , Neoplasias do Colo do Útero , Feminino , Humanos , Proteínas de Ligação ao GTP , Papillomavirus Humano 18 , Interferon gama/farmacologia
14.
Eur Spine J ; 33(6): 2420-2429, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38705902

RESUMO

PURPOSE: This study aimed to use MRI histogram analysis to routine MRI sequences to evaluate lumbar disc degeneration (LDD), illustrate the correlation between this novel method and the traditional Pfirrmann classification method, and more importantly, perform comprehensive agreement analysis of MRI histogram analysis in various situations to evaluate its objectivity and stability. METHODS: Lumbar MRI images from 133 subjects were included in this study. LDD was classified into grades by Pfirrmann classification and was measured as peak separation value by MRI histogram analysis. Correlation analysis between the two methods was performed and cutoff values were determined. In addition, the agreement analysis of peak separation value was performed by intraclass correlation coefficient (ICC) in four scenarios, including inter-resolution, inter-observer, inter-regions of interest (ROI) and inter-slice. RESULTS: Peak separation values were strongly correlated with Pfirrmann grades (r = - 0.847). The inter-resolution agreements of peak separation value between original image resolution of 2304 × 2304 and compressed image resolutions (1152 × 1152, 576 × 576, 288 × 288) were good to excellent (ICCs were 0.916, 0.876 and 0.822), except 144 × 144 was moderate (ICC = 533). The agreements of inter-observer (ICC = 0.982) and inter-ROI (ICC = 0.915) were excellent. Compared with the mid-sagittal slice, the inter-slice agreements were good for the first adjacent slices (ICCs were 0.826 and 0.844), and moderate to good for the second adjacent slices (ICC = 0.733 and 0.753). CONCLUSION: MRI histogram analysis, used in routine MRI sequences, demonstrated a strong correlation with Pfirrmann classification and good agreements in various scenarios, expanding the range of application and providing an effective, objective and quantitative tool to evaluate LDD.


Assuntos
Degeneração do Disco Intervertebral , Vértebras Lombares , Imageamento por Ressonância Magnética , Humanos , Degeneração do Disco Intervertebral/diagnóstico por imagem , Imageamento por Ressonância Magnética/métodos , Masculino , Vértebras Lombares/diagnóstico por imagem , Feminino , Pessoa de Meia-Idade , Adulto , Idoso , Adulto Jovem
15.
Nano Lett ; 23(10): 4487-4494, 2023 May 24.
Artigo em Inglês | MEDLINE | ID: mdl-37171136

RESUMO

Chalcogenide glasses (ChGs) have recently emerged as enabling materials for building reconfigurable nanophotonic devices by employing their refractive index changes associated with photosensitive effects. In particular, the availability of low-loss thin-film ChGs and the realization of high-Q microresonators provide exciting opportunities for integrated photonics. So far, the ChG photonic devices are predominately operated in the classical optics regime. In this work, we present the realization on-chip bright photon-pair quantum light sources via spontaneous four-wave mixing in a high-Q microring resonator fabricated on the newly developed ChG Ge25Sb10S65 platform. The emission wavelength of the photon-pair source can be continuously tuned across a double-free spectral range in a reconfigurable manner. Our work serves as a starting point to fully unleash the potential of exploiting ChGs for developing reconfigurable integrated quantum photonic devices.

16.
Molecules ; 29(2)2024 Jan 22.
Artigo em Inglês | MEDLINE | ID: mdl-38276630

RESUMO

Thyroid transcription factor 1 (TTF1) is an important cancer-related biomarker for clinical diagnosis, especially for carcinomas of lung and thyroid origin. Herein, a novel label-free electrochemical immunosensor was prepared for TTF1 detection based on nanohybrids of ribbon-like tungsten disulfide-reduced graphene oxide (WS2-rGO) and gold nanoparticles (AuNPs). The proposed immunosensor employed H2O2 as the electrochemical probe because of the excellent peroxidase-like activity of ribbon-like WS2-rGO. The introduction of AuNPs not only enhanced the electrocatalytic activity of the immunosensor, but also provided immobilization sites for binding TTF1 antibodies. The electrochemical signals can be greatly amplified due to their excellent electrochemical performance, which realized the sensitive determination of TTF1 with a wide linear range of 0.025-50 ng mL-1 and a lower detection limit of 0.016 ng mL-1 (S/N = 3). Moreover, the immunosensor exhibited high selectivity, good reproducibility, and robust stability, as well as the ability to detect TTF1 in human serum with satisfactory results. These observed properties of the immunosensor enhance its potential practicability in clinical applications. This method can also be used for the detection of other tumor biomarkers by using the corresponding antigen-antibody complex.


Assuntos
Técnicas Biossensoriais , Grafite , Nanopartículas Metálicas , Sulfetos , Compostos de Tungstênio , Humanos , Ouro/química , Técnicas Eletroquímicas/métodos , Técnicas Biossensoriais/métodos , Reprodutibilidade dos Testes , Fator Nuclear 1 de Tireoide , Peróxido de Hidrogênio , Nanopartículas Metálicas/química , Imunoensaio/métodos , Grafite/química , Biomarcadores Tumorais , Limite de Detecção
17.
Angew Chem Int Ed Engl ; : e202410397, 2024 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-38896110

RESUMO

The valorization of native lignin to functionalized aromatic compounds under visible light is appealing yet challenging. In this communication, colloidal mercaptoalkanoic acid capped ultrathin ZnIn2S4 (ZIS) microbelts was successfully fabricated, which was used as a superior catalyst for depolymerization of native lignin in birch woodmeal under visible light, with an optimum yield of 28.8 wt% to functionalized aromatic monomers achieved in 8 h. The capped mercaptoalkanoic acid not only enables a solvent modulated reversible interchange of ZIS between the colloidal state for efficient reaction and the aggregated state for facile separation, but also serves as a precursor for light initiated generation of reactive thiyl radical for highly selective cleavage of ß-O-4 bond in native lignin. This work provides a green and efficient strategy for the depolymerization of native lignin to functionalized aromatic monomers under mild conditions, which involves a new mechanism for the cleavage of ß-O-4 bonds in native lignin. The capability of cleavage of ß-O-4 bonds in native lignin by photogenerated thiyl radicals also demonstrates the great potential of using photogenerated thiyl radicals in organics transformations.

18.
Anal Chem ; 95(31): 11641-11648, 2023 08 08.
Artigo em Inglês | MEDLINE | ID: mdl-37489999

RESUMO

Reproductive hormones play vital roles in reproductive health and can be used to assess a woman's ovarian function and diagnose diseases associated with reproductive endocrine disorders. As these hormones are important biomarkers for reproductive health monitoring and diagnosis, a rapid, high-throughput, and low-invasive detection and simultaneous assessment of the levels of multiple reproductive hormones has important clinical applications. In this work, a quadruplex ultrasensitive immunoassay was developed for simultaneous assessment of 4 human reproductive hormone proteins (follicle-stimulating hormone (FSH), luteinizing hormone (LH), prolactin (PRL), and anti-Müllerian hormone (AMH)) in a variety of human biofluid samples. This assay takes advantage of single-molecule imaging of microwell arrays and capture antibody beads as a reaction interface to construct multiplex bead array immunoassays. The analyte-bound beads can easily be parsed to individual wells and detected via fluorophores, emitting distinct wavelengths associated to the beads. As a result, this proposed quadruplex immunoassay exhibits four good 4-parameter logistic calibration curves ranging from 2.7 to 2000, 1.6 to 1200, 1.8 to 1300, and 0.3 to 220 pg/mL with limits of detection of 0.32, 0.28, 0.14, and 0.02 pg/mL for FSH, LH, PRL, and AMH, respectively. Furthermore, the developed quadruplex immunoassay was used to test clinical venous serum samples where it showed remarkable consistency with clinical test results in methodological comparison and the diagnosis of polycystic ovary syndrome. In addition, we successfully applied the ultrasensitive capability of this assay to the simultaneous testing and evaluation of four proteins in fingertip blood as well as urine samples, in which the urinary AMH level (1.42-156 pg/mL) was measured and assessed quantitatively for the first time.


Assuntos
Hormônio Luteinizante , Síndrome do Ovário Policístico , Feminino , Humanos , Hormônio Foliculoestimulante , Síndrome do Ovário Policístico/diagnóstico , Hormônio Antimülleriano , Imunoensaio
19.
Anal Chem ; 95(13): 5678-5686, 2023 04 04.
Artigo em Inglês | MEDLINE | ID: mdl-36952638

RESUMO

Sensing systems based on cholinesterase and carboxylesterase coupled with different transduction technologies have emerged for pesticide screening owing to their simple operation, fast response, and suitability for on-site analysis. However, the broad spectrum and specificity screening of pyrethroids over organophosphates and carbamates remains an unmet challenge for current enzymatic sensors. Human serum albumin (HSA), a multifunctional protein, can promote various chemical transformations and show a high affinity for pyrethroids, which offer a route for specific and broad-spectrum pyrethroid screening. Herein, for the first time, we evaluated the catalytic hydrolysis function of human serum albumin (HSA) on the coumarin lactone bond and revealed that HSA can act as an enzyme to catalyze the hydrolysis of the coumarin lactone bond. Molecular docking and chemical modifications indicate that lysine 199 and tyrosine 411 serve as the catalytic general base and contribute to most of the catalytic activity. Utilizing this enzymatic activity, a broad specific ratiometric fluorescence pyrethroids sensing system was developed. The binding energetics and binding constants of pesticides and HSA show that pyrethroids bind to HSA more easily than organophosphates and carbamates, which is responsible for the specificity of the sensing system. This study provides a general sensor platform and strategy for screening pesticides and reveals the catalytic activity of HSA on the hydrolysis of the coumarin lactone bond, which may open innovative horizons for the chemical sensing and biomedical applications of HSA.


Assuntos
Praguicidas , Piretrinas , Humanos , Albumina Sérica Humana/metabolismo , Hidrólise , Piretrinas/química , Simulação de Acoplamento Molecular , Cumarínicos/química , Carbamatos , Organofosfatos , Lactonas , Ligação Proteica , Espectrometria de Fluorescência
20.
Small ; 19(44): e2303044, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37403301

RESUMO

Lightweight porous hydrogels provide a worldwide scope for functional soft mateirals. However, most porous hydrogels have weak mechanical strength, high density (>1 g cm-3 ), and high heat absorption due to weak interfacial interactions and high solvent fill rates, which severely limit their application in wearable soft-electronic devices. Herein, an effective hybrid hydrogel-aerogel strategy to assemble ultralight, heat-insulated, and tough polyvinyl alcohol (PVA)/SiO2 @cellulose nanoclaws (CNCWs) hydrogels (PSCG) via strong interfacial interactions with hydrogen bonding and hydrophobic interaction is demonstrated. The resultant PSCG has an interesting hierarchical porous structure from bubble template (≈100 µm), PVA hydrogels networks introduced by ice crystals (≈10 µm), and hybrid SiO2 aerogels (<50 nm), respectively. PSCG shows unprecedented low density (0.27 g cm-3 ), high tensile strength (1.6 MPa) & compressive strength (1.5 MPa), excellent heat-insulated ability, and strain-sensitive conductivity. This lightweight porous and tough hydrogel with an ingenious design provides a new way for wearable soft-electronic devices.

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