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1.
Environ Res ; 257: 119298, 2024 May 31.
Artigo em Inglês | MEDLINE | ID: mdl-38823616

RESUMO

Antibiotic resistance poses a considerable global public health concern, leading to heightened rates of illness and mortality. However, the impact of seasonal variations and environmental factors on the health risks associated with antibiotic resistance genes (ARGs) and their assembly mechanisms is not fully understood. Based on metagenomic sequencing, this study investigated the antibiotic resistome, mobile genetic elements (MGEs), and microbiomes in a subtropical coastal ecosystem of the Beibu Gulf, China, over autumn and winter, and explored the factors influencing seasonal changes in ARG and MGE abundance and diversity. Results indicated that ARG abundance and diversity were higher in winter than in autumn, with beta-lactam and multidrug resistance genes being the most diverse and abundant, respectively. Similarly, MGE abundance and diversity increased in winter and were strongly correlated with ARGs. In contrast, more pronounced associations between microbial communities, especially archaea, and the antibiotic resistome were observed in autumn than in winter. The co-occurrence network identified multiple interactions between MGEs and various multidrug efflux pumps in winter, suggesting a potential for ARG dissemination. Multivariate correlation analyses and path modeling indicated that environmental factors driving microbial community changes predominantly influenced antibiotic resistome assembly in autumn, while the relative importance of MGEs increased significantly in winter. These findings suggest an elevated health risk associated with antimicrobial resistance in the Beibu Gulf during winter, attributed to the dissemination of ARGs by horizontal gene transfer. The observed seasonal variations highlight the dynamic nature of antibiotic resistance dissemination in coastal ecosystems, emphasizing the need for comprehensive surveillance and management measures to address the growing threat of antimicrobial resistance in vulnerable environments.

2.
Opt Express ; 32(12): 21696-21707, 2024 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-38859518

RESUMO

Edge-enhanced imaging by spiral phase contrast has proven instrumental in revealing phase or amplitude gradients of an object, with notable applications spanning feature extraction, target recognition, and biomedical fields. However, systems deploying spiral phase plates encounter limitations in phase mask modulation, hindering the characterization of the modulation function during image reconstruction. To address this need, we propose and demonstrate an innovative nonlinear reconstruction method using a Laguerre-Gaussian composite vortex filter, which modulates the spectrum of the target. The involved nonlinear process spectrally transforms the incident short-wavelength-infrared (SWIR) signal from 1550 to 864 nm, subsequently captured by a silicon charge-coupled device. Compared with conventional schemes, our novel filtering method effectively suppresses the diffraction noise, significantly enhancing image contrast and resolution. By loading specific phase holograms on the spatial light modulator, bright-field imaging, isotropic, amplitude-controlled anisotropic, and directional second-order edge-enhanced imaging are realized. Anticipated applications for the proposed SWIR edge-enhanced imaging system encompass domains such as artificial intelligence recognition, deep tissue medical diagnostics, and non-destructive defect inspection. These applications underscore the valuable potential of our cutting-edge methodology in furthering both scientific exploration and practical implementations.

3.
Opt Express ; 32(7): 11323-11336, 2024 Mar 25.
Artigo em Inglês | MEDLINE | ID: mdl-38570982

RESUMO

The lensless camera with incoherent illumination has gained significant research interest for its thin and flexible structure. However, it faces challenges in resolving scenes with a wide depth of field (DoF) due to its depth-dependent point spread function (PSF). In this paper, we present a single-shot method for extending the DoF in Fresnel zone aperture (FZA) cameras at visible wavelengths through passive depth estimation. The improved ternary search method is utilized to determine the depth of targets rapidly by evaluating the sharpness of the back propagation reconstruction. Based on the depth estimation results, a set of reconstructed images focused on targets at varying depths are derived from the encoded image. After that, the DoF is extended through focus stacking. The experimental results demonstrate an 8-fold increase compared with the calibrated DoF at 130 mm depth. Moreover, our depth estimation method is five times faster than the traversal method, while maintaining the same level of accuracy. The proposed method facilitates the development of lensless imaging in practical applications such as photography, microscopy, and surveillance.

4.
ACS Nano ; 18(12): 9100-9113, 2024 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-38478044

RESUMO

Reactive oxygen species (ROS) mediated tumor cell death is a powerful anticancer strategy. Cuproptosis is a copper-dependent and ROS-mediated prospective tumor therapy strategy. However, the complex tumor microenvironment (TME), low tumor specificity, poor therapy efficiency, and lack of imaging capability impair the therapy output of current cuproptosis drugs. Herein, we designed a dual-responsive two-dimensional metal-organic framework (2D MOF) nanotheranostic via a coordination self-assembly strategy using Au(III) tetra-(4-pyridyl) porphine (AuTPyP) as the ligand and copper ions (Cu2+) as nodes. The dual-stimulus combined with the protonation of the pyridyl group in AuTPyP and deep-penetration ultrasound (US) together triggered the controlled release in an acidic TME. The ultrathin structure (3.0 nm) of nanotheranostics promoted the release process. The released Cu2+ was reduced to Cu+ by depleting the overexpressed glutathione (GSH) in the tumor, which not only activated the Ferredoxin 1 (FDX1)-mediated cuproptosis but also catalyzed the overexpressed hydrogen peroxide (H2O2) in the tumor into reactive oxygen species via Fenton-like reaction. Simultaneously, the released AuTPyP could specifically bind with thioredoxin reductase and activate the redox imbalance of tumor cells. These together selectively induced significant mitochondrial vacuoles and prominent tumor cell death but did not damage the normal cells. The fluorescence and magnetic resonance imaging (MRI) results verified this nanotheranostic could target the HeLa tumor to greatly promote the self-enhanced effect of chemotherapy/cuproptosis and tumor inhibition efficiency. The work helped to elucidate the controlled assembly of multiresponsive nanotheranostics and the high-specificity ROS regulation for application in anticancer therapy.


Assuntos
Estruturas Metalorgânicas , Nanopartículas , Neoplasias , Humanos , Cobre , Estruturas Metalorgânicas/farmacologia , Espécies Reativas de Oxigênio , Peróxido de Hidrogênio , Estudos Prospectivos , Glutationa , Concentração de Íons de Hidrogênio , Neoplasias/diagnóstico por imagem , Neoplasias/tratamento farmacológico , Linhagem Celular Tumoral , Microambiente Tumoral
5.
Chem Commun (Camb) ; 60(33): 4423-4426, 2024 Apr 18.
Artigo em Inglês | MEDLINE | ID: mdl-38523593

RESUMO

A pair of isomeric Py-BT-COFs with the same composition, but slightly different atomic arrangements, were designed and synthesized. The minute structural variations of the Py-BT-COF isomers generated significantly different redox and photophysical properties and correspondingly led to different photocatalytic manifestations in H2 evolution and rhodamine B degradation.

6.
Chemistry ; 29(66): e202302380, 2023 Nov 24.
Artigo em Inglês | MEDLINE | ID: mdl-37668073

RESUMO

2D covalent organic frameworks with Kagome (kgm) topology are a promising class of crystalline frameworks that possess both triangular and hexagonal pores. These dual-pore structures enable kgm COFs to exhibit unique advantages in selective separation, mass transfer, and targeted drug release. However, the synthesis of 2D kgm COFs has been hindered by the reliance on empirical methods. This review systematically summarizes the conventional macrocycle-to-framework strategy, typical [4+2] co-polymerization synthetic strategy, and bifunctional molecules self-condensation approach for constructing 2D kgm COFs. Factors influencing the formation of kgm lattice are surveyed, such as monomer type, solvent polarity, substrate concentration, etc., and highlight the representative examples on targeted synthesis. Additionally, applications of 2D kgm COFs and relationships between structure and performances are summarized. Finally, key fundamental perspectives are proposed to accelerate the further development of this intriguing material.

7.
Front Med (Lausanne) ; 10: 1160828, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37425301

RESUMO

Introduction: Hand hygiene is a cost-effective measure to reduce healthcare-associated infections (HAIs) in healthcare facilities. The impact of the coronavirus disease 2019 (COVID-19) pandemic on hand hygiene performance (HHP) provided evidence for targeted hand hygiene intervention measures. Methods: This study evaluated the HHP rate in a tertiary hospital before and after the COVID-19 outbreak. HHP was checked by infection control doctors or nurses every day, and they inputted the HHP rate to the full-time infection control staff every week. A random examination of HHP was conducted by a confidential worker every month. The HHP of healthcare workers (HCWs) was monitored in the outpatient department, inpatient ward, and operating room from January 2017 to October 2022. The influence of COVID-19 prevention and control strategies on HHP was elucidated by analyzing the results of HHP during the study period. Results: The average HHP rate of HCWs was 86.11% from January 2017 to October 2022. The HHP rate of HCWs after the COVID-19 pandemic was statistically significantly higher than that before the pandemic (P < 0.001). The HHP rate was the highest (93.01%) in September 2022 when the local epidemic occurred. Among the different occupation categories, medical technicians showed the highest HHP rate (89.10%). The HHP rate was the highest after contact with body fluids or blood of patients (94.47%). Conclusion: The HHP rate of HCWs in our hospital showed an increasing trend in the recent 6 years, especially during the COVID-19 pandemic, and the increase was most obvious during the local epidemic.

8.
Chem Commun (Camb) ; 59(60): 9211-9214, 2023 Jul 25.
Artigo em Inglês | MEDLINE | ID: mdl-37409590

RESUMO

We report on the fast reaction kinetics of an imine based 2D polymer (2DP) formed from a single monomer carrying both aldehyde and amine groups. Our results point towards a direct monomer-to-crystalline polymer transition without an amorphous intermediate.

9.
Water Res ; 242: 120270, 2023 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-37392508

RESUMO

Estuaries are hotspots of plastic pollution due to accumulated waste from surrounding rivers and coasts. However, the molecular ecological resources that possess plastic-degrading traits and their biogeographic distributions in estuarine waters remain to be elucidated. In this study, we mapped the distribution profiles of plastic-degrading genes (PDGs) in 30 subtropical estuaries in China based on metagenomic sequencing. A total of 41 PDG subtypes were observed in these estuaries. The Pearl River Estuary had higher diversity and abundance of PDGs than the east and west region estuaries. Genes for degrading synthetic heterochain and natural plastics were the most diverse and abundant types, respectively. The abundance of synthetic PDGs was significantly higher in estuaries affected by intense anthropogenic activities. Further binning strategies revealed diverse microbes with plastic-degrading ability in these estuaries. Rhodobacteraceae, a dominant plastic-degrading bacterial family, primarily carried PDGs for degrading natural plastics. Pseudomonas veronii carrying diverse PDGs was identified, which may be of value for further technical improvement of plastic degradation. In addition, phylogenetic and structural analyses of 19 putative 3HV dehydrogenases, the most diverse and abundant DPGs, showed inconsistent evolution with their hosts, but different sequences were conserved with consistent key functional amino acids. A potential biodegradation pathway for polyhydroxybutyrate by Rhodobacteraceae was proposed. The result implied that plastic-degrading functions are widely distributed in estuarine waters and metagenomics could be used as a promising screening tool for large-scale profiling of plastic-degrading potential in the natural environment. Our findings have important implications and provide potential molecular ecological resources for developing plastic waste removal technologies.


Assuntos
Estuários , Poluentes Químicos da Água , Plásticos , Metagenômica , Filogenia , China , Rios/química , Monitoramento Ambiental , Poluentes Químicos da Água/análise
10.
Nanoscale ; 15(10): 4762-4771, 2023 Mar 09.
Artigo em Inglês | MEDLINE | ID: mdl-36756711

RESUMO

Isomeric covalent organic frameworks possessing the same chemical constitutions but different atomic arrangement structures and physicochemical properties are fascinating branches of covalent organic frameworks (COFs). However, the rational design and targeted synthesis of isomeric COFs remain conundrums, so the investigation of isomeric COFs is still in a fledging period. According to the diversity of frameworks, positional isomers with similar structures and framework isomers having distinct constructions are the main existing subspecies of isomeric COFs. In this review, we focus on the research progress and substantial achievements in this fascinating embranchment and systematically summarize and highlight the design principles of both positional isomeric and framework isomeric COFs, which will potentially facilitate further exploitation and investigation of novel isomeric COFs. The application and structure-property relationship of these isomeric COFs have been briefly introduced. Moreover, key constraints of current isomeric COFs and further advancement of this promising field are proposed and anticipated.

11.
RSC Adv ; 13(3): 1587-1593, 2023 Jan 06.
Artigo em Inglês | MEDLINE | ID: mdl-36688064

RESUMO

A rapid, simple, and sensitive fluorescent detection method for brown spot of tobacco is established by lambda exonuclease-induced Mg2+-dependent DNAzyme amplification. It contains hybridization of the Alternaria alternata genome and HP1, digestion of the 5'-phosphorylated strand of the hybrid dsDNA by lambda exonuclease, acquisition of complete Mg2+-dependent DNAzyme, cleavage of the substrate modified with FAM and BHQ-1, and fluorescent detection. The proposed assay exhibits good sensitivity (10 pg L-1), selectivity and reproducibility. The method does not require pure DNA and expensive instruments, and can be performed within 2.5 hours. To the best of our knowledge, this is the first report of fluorescent detection of Alternaria alternata and its tobacco field samples. This method can be applied to the rapid and sensitive detection of Alternaria alternata in tobacco and its seedlings, and is particularly important for the green prevention and control of tobacco brown spot disease.

12.
Nanomaterials (Basel) ; 13(2)2023 Jan 13.
Artigo em Inglês | MEDLINE | ID: mdl-36678085

RESUMO

Tobacco bacterial wilt is a serious disease caused by the soil-borne bacterium Ralstonia solanacearum (R. solanacearum). Herein, a rapid and purification-free α-hemolysin (α-HL) nanopore-sensing strategy based on polymerase chain reaction (PCR) and lambda exonuclease digestion was established to detect R. solanacearum. A 198-nucleotide-long single-stranded DNA was obtained via asymmetric PCR or the lambda exonuclease-mediated digestion of the PCR product. The DNA fragment produced unique long-lived, current-blocking signals when it passed through the α-HL nanopore. This sensing approach can allow for the determination of R. solanacearum in tobacco samples and can be conveniently extended to other DNA monitoring because of the extremely wide range of PCR applications.

13.
Angew Chem Int Ed Engl ; 62(10): e202216795, 2023 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-36627239

RESUMO

Targeted synthesis of kagome (kgm) topologic 2D covalent organic frameworks remains challenging, presumably due to the severe dependence on building units and synthetic conditions. Herein, two isomeric "two-in-one" monomers with different lengths of substituted arms based on naphthalene core (p-Naph and m-Naph) are elaborately designed and utilized for the defined synthesis of isomeric kgm Naph-COFs. The two isomeric frameworks exhibit splendid crystallinity and showcase the same chemical composition and topologic structure with, however, different pore channels. Interestingly, C60 is able to uniformly be encapsulated into the triangle channels of m-Naph-COF via in situ incorporation method, while not the isomeric p-Naph-COF, likely due to the different pore structures of the two isomeric COFs. The resulting stable C60 @m-Naph-COF composite exhibits much higher photoconductivity than the m-Naph-COF owing to charge transfer between the conjugated skeletons and C60 guests.

14.
Microbiol Spectr ; 11(1): e0368322, 2023 02 14.
Artigo em Inglês | MEDLINE | ID: mdl-36507672

RESUMO

Microbial communities in coastal waters are diverse and dynamic and play important roles in ecosystem functions and services. Despite the ecological impact of bacterioplankton or pathogens, little is known about whether bacterioplankton and pathogen communities exhibit similar patterns. Here, using 16S RNA gene amplicon sequencing, the geographic patterns and assembly processes of bacterioplankton and pathogen communities in 30 subtropical estuaries were studied. Results showed that the estuarine bacterioplankton communities mainly consisted of Proteobacteria (49.06%), Actinobacteria (17.62%), and Bacteroidetes (16.33%), among which 31 pathogen genera (186 amplicon sequence variants [ASVs]) were identified. Under the influence of salinity, bacterioplankton and pathogens showed similar biogeographic patterns. Redundancy and correlation analyses indicated that the bacterioplankton communities were strongly correlated with estuarine environmental factors, but potential pathogens were less influenced. Co-occurrence network analysis revealed a close relationship between bacterioplankton and potential pathogens, with two pathogens identified as connectors (i.e., ASV340 [Clostridium perfringens] and ASV1624 [Brevundimonas diminuta]), implying potential impacts of pathogens on structure, function, and stability of estuarine bacterioplankton communities. Null-model analysis revealed that deterministic processes (heterogeneous selection) dominated bacterioplankton community assembly, while stochastic processes (undominated effect) shaped the potential pathogen community. Our findings illustrate the biogeographic patterns and community assembly mechanisms of bacterioplankton and pathogens in estuaries, which should provide guidance and a reference for the control of potential pathogenic bacteria. IMPORTANCE Bacterioplankton play an important role in estuarine ecosystem functions and services; however, potentially pathogenic bacteria may exhibit infectivity and pose a serious threat to environmental and human health. In this study, geographic patterns and assembly processes of bacterioplankton communities in 30 subtropical estuaries were explored, and potential pathogenic bacteria in the estuaries were detected and profiled. Our results demonstrate here that bacterioplankton and pathogens show similar biogeographic patterns under the influence of salinity. Interestingly, heterogeneous selection dominated bacterioplankton assembly, while stochasticity dominated pathogen assembly. This study provides important information for future risk assessment of potential pathogenic bacteria as well as management in estuarine ecosystems.


Assuntos
Ecossistema , Microbiota , Humanos , Estuários , Microbiota/genética , Bactérias/genética , Proteobactérias , Organismos Aquáticos
15.
Polymers (Basel) ; 14(22)2022 Nov 13.
Artigo em Inglês | MEDLINE | ID: mdl-36433020

RESUMO

Covalent organic frameworks (COFs) with donor-acceptor (D-A) units are credible photocatalysts for their per-designed structure, inherent porosity, large surface area, splendid stability and so forth. Developing COFs with an excellent photocatalytic efficiency for hydrogen evolution is of a great significance in alleviating the energy crisis. Herein, a D-A type imine-linked crystalline Zn-Por-TT COF was fabricated successfully via the co-polymerization of electron-deficient Zinc (II) 5,10,15,20-tetrakis(para-aminophenyl) porphyrin (Zn-TAPP), and electron-rich thieno[3,2-b]thiophene-2,5-dicarbaldehyde (TT). Profiting from the D-A complex structure, the obtained Zn-Por-TT COF showcases an excellent photocatalytic activity with a hydrogen evolution rate of 8200 µmol/g/h, while the Zn-TAPP monomer presents practically no capacity for the generation of hydrogen under identical conditions. In addition, the counterparts Por-TT COF and COF-366-Zn were employed to illustrate the enhancement of the photocatalytic performance by metal catalytic sites and D-A structures. In addition, the counterparts Por-TT COF and COF-366-Zn were employed to illustrate the enhancement of metal catalytic sites and D-A structures for the photocatalytic performance.

16.
Zootaxa ; 5134(1): 113-124, 2022 May 09.
Artigo em Inglês | MEDLINE | ID: mdl-36101074

RESUMO

A new species, Neodontobutis lani (Odontobutidae) is described from the Zuojiang River, a tributary of the Xijiang River of the Pearl River basin, at Longzhou Town, Guangxi Zhuang Autonomous Region, Southern China. This species can be distinguished from other Neodontobutis species by following characters: anterior head flat, with interorbital width / eye diameter = 1.41.9 (vs. less than 1.4); several rows (vs. single row) of transforming ctenii on posterior edges of body scales; sensory papilla on lower jaw arranged in two oblong clusters (vs. two single lines). It can be distinguished from Odontobutis species by: separated right and left gill membrane (vs. joined); barbel-like projection present on sensory papillae. Molecular phylogenetic analysis of 2,076 nuclear coding loci indicates that N. lani is a sister species of N. hainanensis, the only Neodontobutis species that has been described from China.


Assuntos
Perciformes , Animais , Núcleo Celular , China , Filogenia , Rios
17.
Chem Asian J ; 17(21): e202200747, 2022 Nov 02.
Artigo em Inglês | MEDLINE | ID: mdl-36029274

RESUMO

The main protease (Mpro ), which is highly conserved and plays a critical role in the replication of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), is a natural biomarker for SARS-CoV-2. Accurate assessment of the Mpro activity is crucial for the detection of SARS-CoV-2. Herein, we report a nanopore-based sensing strategy that uses an enzyme-catalyzed cleavage reaction of a peptide substrate to measure the Mpro activity. The peptide was specifically cleaved by the Mpro , thereby releasing the output products that, when translocated through aerolysin, quantitatively produced the signature current events. The proposed method exhibited high sensitivity, allowing the detection of Mpro concentrations as low as 1 nM without the use of any signal amplification techniques. This simple, convenient, and label-free nanopore assay may expand the diagnostic tools for viruses.


Assuntos
COVID-19 , Proteases 3C de Coronavírus , Nanoporos , Humanos , COVID-19/diagnóstico , Peptídeos , SARS-CoV-2/enzimologia , Proteases 3C de Coronavírus/análise
18.
Sci Adv ; 8(12): eabm3541, 2022 Mar 25.
Artigo em Inglês | MEDLINE | ID: mdl-35319984

RESUMO

Single-molecule junctions (SMJs) offer a novel strategy for miniaturization of electronic devices. In this work, we realize a graphene-porphyrin-graphene SMJ driven by electric field and proton transfer in two configurations. In the transistor configuration with ionic liquid gating, an unprecedented field-effect performance is achieved with a maximum on/off ratio of ~4800 and a gate efficiency as high as ~179 mV/decade in consistence with the theoretical prediction. In the other configuration, controllable proton transfer, tautomerization switching, is directly observed with bias dependence. Room temperature proton transfer leads to a two-state conductance switching, and more precise tautomerization is detected, showing a four-state conductance switching at high bias voltages and low temperatures. Such an SMJ in two configurations provides new insights into not only building multifunctional molecular nanocircuits toward real applications but also deciphering the intrinsic properties of matters at the molecular scale.

19.
Nano Lett ; 22(1): 157-163, 2022 01 12.
Artigo em Inglês | MEDLINE | ID: mdl-34958579

RESUMO

The preparation of self-assembled porphyrins with orderly stacked nanostructures for emulating natural photosynthesis has stimulated extensive efforts to optimize the energy conversion efficiency. However, the elucidation of how orderly stacked structures promote photocatalysis at the molecular level remains a great challenge. Here, unique porphyrin nanoleaves with designed and ordered structure are synthesized and show a hydrogen evolution rate higher than that of commercial powder. Photodeposition of cocatalysts and Kelvin probe force microscopy measurement suggest selective aggregation of photogenerated electrons and holes at different active sites. Combined with theoretical calculations, we find that the orderly packing changes molecular symmetry and induces a molecular dipole, which increases linearly along the π-π stacking direction and forms a strong built-in electric field. The built-in electric field drives photogenerated electrons and holes for the unique crossed transportation along different directions. These findings reveal how orderly stacked structures promote photocatalysis and provide a novel approach for highly efficient water splitting.


Assuntos
Nanoestruturas , Porfirinas , Catálise , Hidrogênio/química , Nanoestruturas/química , Fotossíntese , Porfirinas/química
20.
Angew Chem Int Ed Engl ; 60(38): 20754-20759, 2021 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-34309145

RESUMO

The development of new linkages is one of the most efficient strategies to enrich the diversity of covalent organic frameworks (COFs). Particularly, functional linkages can endow COFs with additional tailored properties besides the building units, which further diversify COFs with desirable functions. Herein, we have developed a new arylamine linkage for the construction of COFs. Two new arylamine-linked COFs (AAm-TPB and AAm-Py) were prepared by condensing cost-effective dimethyl succinyl succinate (DMSS) with corresponding multitopic amines (TPB-NH2 and Py-NH2 ). Due to the abundant electroactive diphenylamine moieties in the COF skeletons resembling that of polyaniline (PANI), a state-of-the-art conductive polymer, the pseudocapacitive energy storage performance of AAm-TPB was further investigated. Remarkably, the AAm-TPB electrode exhibits a high capacitance of 271 F g-1 with a three-electrode setup at a discharge rate of 1 A g-1 , which represents one of the highest capacitances among the reported COF-based electrode materials.

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