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1.
Anal Chem ; 96(1): 179-187, 2024 Jan 09.
Artículo en Inglés | MEDLINE | ID: mdl-38100653

RESUMEN

Achieving accurate detection of different speciations of heavy metal ions (HMIs) in an aqueous solution is an urgent problem due to the different bioavailabilities and physiological toxicity. Herein, we nominated a novel strategy to detect HCrO4- and Cr(OH)2+ at a trace level via the electrochemical sensitive surface constructed by Co3O4-rGO modified with amino and carboxyl groups, which revealed that the interactions between distinct functional groups and different oxygen-containing groups of target ions are conducive to the susceptible and anti-interference detection. The detection sensitivities of 19.46 counts µg-1 L for HCrO4- and 13.44 counts µg-1 L for Cr(OH)2+ were obtained under optimal conditions, while the limits of detection were 0.10 and 0.12 µg L-1, respectively. Satisfactory anti-interference and actual water sample analysis results were obtained. A series of advanced optical techniques like X-ray photoelectron spectroscopy, X-ray absorption near-edge structure technology, and density functional theory calculations under an electric field demonstrated that chemical interactions between groups contribute more to the fixation of target ions than electrical attraction alone. The presence of oxygen-containing groups distinct from simple ionic forms was a critical factor in the selectivity and anti-interference detection. Furthermore, the valence cycle of Co(II)/(III) synergistically boosted the detection performance. This research provides a promising tactic from the microscopic perspective of groups' interactions to accomplish the precise speciation analysis of HMIs in the water environment.

2.
Anal Chem ; 96(13): 5232-5241, 2024 Apr 02.
Artículo en Inglés | MEDLINE | ID: mdl-38447030

RESUMEN

Although utilizing nanomaterial-modified electrodes for lead ion detection has achieved great success, most of them are carried out under acidic conditions and ignore the variation of Pb(II) speciation at different pH conditions, leading to the potential inaccuracy of Pb(II) detection in a neutral natural water environment. Thus, designing a novel catalyst with high accuracy for the detection of various forms of the total amount of Pb(II) (Pb2+ and Pb(OH)+) in neutral waters is significant. Herein, Pt nanoclusters (Pt NCs) were elaborately constructed and stabilized on the Co single-atom-doped g-C3N4 with abundant N vacancies (Pt NCs/VN-C3N4), which achieved the ultrasensitive detection (102.16 µM µA-1) of Pb(II) in neutral conditions. The dynamic simulation and theoretical calculations reveal that the parallel deposition of Pb2+ and Pb(OH)+ occurs on the electrode surface modified by Pt NCs/VN-C3N4, and the current peaks of Pb(II) are cocontributed by Pb2+ and Pb(OH)+ species. An "electron inverse" phenomenon in Pt NCs/VN-C3N4 from the VN-C3N4 substrate to Pt NCs endows Pt NCs in an electron-rich state, serving as active centers to promote rapid and efficient reduction for both Pb2+ and Pb(OH)+, facilitating the accurate detection of the total amount of Pb(II) in all forms in the actual water environment.

3.
Anal Chem ; 96(22): 9069-9077, 2024 Jun 04.
Artículo en Inglés | MEDLINE | ID: mdl-38749062

RESUMEN

Solid contact (SC) calcium ion-selective electrodes (Ca2+-ISEs) have been widely applied in the analysis of water quality and body fluids by virtue of the unique advantages of easy operation and rapid response. However, the potential drift during the long-term stability test hinders their further practical applications. Designing novel redox SC layers with large capacitance and high hydrophobicity is a promising approach to stabilize the potential stability, meanwhile, exploring the transduction mechanism is also of great guiding significance for the precise design of SC layer materials. Herein, flower-like copper sulfide (CunS-50) composed of nanosheets is meticulously designed as the redox SC layer by modification with the surfactant (CTAB). The CunS-50-based Ca2+-ISE (CunS-50/Ca2+-ISE) demonstrates a near-Nernstian slope of 28.23 mV/dec for Ca2+ in a wide activity linear range of 10-7 to 10-1 M, with a low detection limit of 3.16 × 10-8 M. CunS-50/Ca2+-ISE possesses an extremely low potential drift of only 1.23 ± 0.13 µV/h in the long-term potential stability test. Notably, X-ray absorption fine-structure (XAFS) spectra and electrochemical experiments are adopted to elucidate the transduction mechanism that the lipophilic anion (TFPB-) participates in the redox reaction of CunS-50 at the solid-solid interface of ion-selective membrane (ISM) and redox inorganic SC layer (CunS-50), thereby promoting the generation of free electrons to accelerate ion-electron transduction. This work provides an in-depth comprehension of the transduction mechanism of the potentiometric response and an effective strategy for designing redox materials of ion-electron transduction triggered by lipophilic anions.

4.
Analyst ; 149(7): 2097-2102, 2024 Mar 25.
Artículo en Inglés | MEDLINE | ID: mdl-38421038

RESUMEN

In this work, we developed a rapid and sensitive label-free ratiometric fluorescent (FL) probe for the detection of bleomycin (BLM). The probe consists of a DNA sequence (D6) and two fluorophore groups, 2-amino-5,6,7-trimethyl-1,8-naphthalene (ATMND) and SYBR Green I (SGI). The D6 sequence could be folded into a three-way junction structure containing a C-C mismatch position in the junction pocket. The unique "Y" structure not only could entrap ATMND in the mismatch pocket with high affinity, leading to FL quenching at 408 nm, but also embed SGI in the grooves of the double-stranded portion, resulting in FL enhancement at 530 nm. In the presence of BLM-Fe(II), the "Y" structure of D6 was destroyed due to the specific cleavage of the BLM recognition site, the 5'-GT-3' site in D6. This caused the release of ATMND and SGI and thus the ratiometric signal change of FL enhancement by ATMND and FL quenching by SGI. Under optimal conditions, the ratiometric probe exhibited a linear correlation between the intensity ratio of F408/F530 and the concentration of BLM in the range of 0.5-1000 nM, with a detection limit of 0.2 nM. In addition, the probe was applied to detect BLM in human serum samples with satisfactory results, indicating its good clinical application potential.


Asunto(s)
Benzotiazoles , Bleomicina , Diaminas , Colorantes Fluorescentes , Quinolinas , Humanos , Colorantes Fluorescentes/química , Límite de Detección , Espectrometría de Fluorescencia/métodos
5.
World J Surg ; 2024 Jul 04.
Artículo en Inglés | MEDLINE | ID: mdl-38964867

RESUMEN

PURPOSE: It is well established that hollow viscus perforation leads to sepsis and acute kidney injury (AKI) in non-trauma patients. However, the relationship between traumatic hollow viscus injury (HVI) and AKI is not well understood. Utilizing data from the National Trauma Data Bank, we investigated whether HVI serves as a risk factor for AKI. Additionally, we examined the characteristics of AKI in stable patients who underwent conservative treatment. METHODS: We reviewed blunt abdominal trauma (BAT) cases from 2012 to 2015, comparing patients with and without AKI. Significant factors from univariate analysis were tested in a multivariate logistic regression (MLR) to identify independent AKI determinants. We also analyzed subsets: patients without HVI and stable patients given conservative management. RESULTS: Out of the 563,040 BAT patients analyzed, 9073 (1.6%) developed AKI. While a greater proportion of AKI patients had HVI than those without AKI (13.3% vs. 5.2%, p < 0.001), this difference wasn't statistically significant in the MLR (p = 0.125). Notably, the need for laparotomy (odds = 3.108, p < 0.001) and sepsis (odds = 13.220, p < 0.001) were identified as independent risk factors for AKI. For BAT patients managed conservatively (systolic blood pressure >90 mmHg, without HVI or laparotomy; N = 497,066), the presence of sepsis was a significant predictor for the development of AKI (odds = 16.914, p < 0.001). CONCLUSIONS: While HVI wasn't a significant risk factor for AKI in BAT patients, the need for laparotomy was. Stable BAT patients managed conservatively are still at risk for AKI due to non-peritonitis related sepsis.

6.
Ann Plast Surg ; 92(1S Suppl 1): S27-S32, 2024 Jan 01.
Artículo en Inglés | MEDLINE | ID: mdl-38285992

RESUMEN

BACKGROUND: Patients with traumatic brain injuries (TBIs) often experience concurrent facial bone fractures. In 2021, a prediction model with 10 variables was published and precisely predicted concomitant facial fractures in TBI patients. Herein, external validation and simplification of this model was performed. METHODS: Traumatic brain injury patients treated at a major referral trauma center were retrospectively reviewed for 1 year. The original prediction model (published in 2021), which was developed from a rural level II trauma center, was applied for external validation. A new and simplified model from our level I trauma center was developed and backwardly validated by rural level II trauma center data. RESULTS: In total, 313 TBI patients were enrolled; 101 (32.3%) had concomitant facial fractures. When the previous prediction model was applied to the validation cohort, it achieved acceptable discrimination, with an area under the receiver operating characteristic curve (AUC) of 0.713 and good precision, with a Brier score of 0.083. A new and simplified model with 6 variables (age, tooth rupture, epistaxis, facial lesion, eye injury, and intracranial hemorrhage) was created with excellent discrimination (AUC = 0.836) and good precision (Brier score of 0.055). The backward validation of this new model also showed excellent discrimination in the cohort used to develop the original model (AUC = 0.875). CONCLUSION: The original model provides an acceptable and reproducible prediction of concomitant facial fractures among TBI patients. A simplified model with fewer variables and the same accuracy could be applied in the emergency department and at higher- and lower-level trauma centers.


Asunto(s)
Lesiones Traumáticas del Encéfalo , Fracturas Craneales , Humanos , Estudios Retrospectivos , Fracturas Craneales/complicaciones , Fracturas Craneales/diagnóstico , Lesiones Traumáticas del Encéfalo/complicaciones , Lesiones Traumáticas del Encéfalo/diagnóstico , Curva ROC , Centros Traumatológicos
7.
Anal Chem ; 95(7): 3666-3674, 2023 Feb 21.
Artículo en Inglés | MEDLINE | ID: mdl-36656141

RESUMEN

Traditional nanomodified electrodes have made great achievements in electrochemical stripping voltammetry of sensing materials for As(III) detection. Moreover, the intermediate states are complicated to probe because of the ultrashort lifetime and complex reaction conditions of the electron transfer process in electroanalysis, which seriously hinder the identification of the actual active site. Herein, the intrinsic interaction of highly sensitive analytical behavior of nanomaterials is elucidated from the perspective of electronic structure through density functional theory (DFT) and gradient boosting regression (GBR). It is revealed that the atomic radius, d-band center (εd), and the largest coordinative TM-N bond length play a crucial role in regulating the arsenic reduction reaction (ARR) performance by the established ARR process for 27 sets of transition-metal single atoms supported on N-doped graphene. Furthermore, the database composed of filtered intrinsic electronic structural properties and the calculated descriptors of the central metal atom in TM-N4-Gra were also successfully extended to oxygen evolution reaction (OER) systems, which effectively verified the reliability of the whole approach. Generally, a multistep workflow is developed through GBR models combined with DFT for valid screening of sensing materials, which will effectively upgrade the traditional trial-and-error mode for electrochemical interface designing.

8.
Anal Chem ; 95(8): 4104-4112, 2023 Feb 28.
Artículo en Inglés | MEDLINE | ID: mdl-36688529

RESUMEN

Significant progress has been made in nanomaterial-modified electrodes for highly efficient electroanalysis of arsenic(III) (As(III)). However, the modifiers prepared using some physical methods may easily fall off, and active sites are not uniform, causing the potential instability of the modified electrode. This work first reports a promising practical strategy without any modifiers via utilizing only soluble Fe3+ as a trigger to detect trace-level As(III) in natural water. This method reaches an actual detection limit of 1 ppb on bare glassy carbon electrodes and a sensitivity of 0.296 µA ppb-1 with excellent stability. Kinetic simulations and experimental evidence confirm the codeposition mechanism that Fe3+ is preferentially deposited as Fe0, which are active sites to adsorb As(III) and H+ on the electrode surface. This facilitates the formation of AsH3, which could further react with Fe2+ to produce more As0 and Fe0. Meanwhile, the produced Fe0 can also accelerate the efficient enrichment of As0. Remarkably, the proposed sensing mechanism is a general rule for the electroanalysis of As(III) that is triggered by iron group ions (Fe2+, Fe3+, Co2+, and Ni2+). The interference analysis of coexisting ions (Cu2+, Zn2+, Al3+, Hg2+, Cd2+, Pb2+, SO42-, NO3-, Cl-, and F-) indicates that only Cu2+, Pb2+, and F- showed inhibitory effects on As(III) due to the competition of active sites. Surprisingly, adding iron power effectively eliminates the interference of Cu2+ in natural water, achieving a higher sensitivity for 1-15 ppb As(III) (0.487 µA ppb-1). This study provides effective solutions to overcome the potential instability of modified electrodes and offers a practical sensing platform for analyzing other heavy-metal anions.

9.
World J Surg ; 47(12): 3116-3123, 2023 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-37851065

RESUMEN

PURPOSE: This study aimed to validate the previously reported association between delayed bladder repair and increased infection rates using the National Trauma Data Bank (NTDB). METHODS: Bladder injury patients with bladder repair in the NTDB from 2013 to 2015 were included. Propensity score matching (PSM) was used to compare mortality, infection rates, and hospital length of stay (LOS) between patients who underwent bladder repair within 24 h and those who underwent repair after 24 h. Linear regression and multivariate logistic regression analyses were also performed. RESULTS: A total of 1658 patients were included in the study. Patients who underwent bladder repair after 24 h had significantly higher infection rates (5.4% vs. 1.2%, p = 0.032) and longer hospital LOS (17.1 vs. 14.0 days, p = 0.032) compared to those who underwent repair within 24 h after a well-balanced 1:1 PSM (N = 166). Linear regression analysis showed a positive correlation between time to bladder repair and hospital LOS for patients who underwent repair after 24 h (B-value = 0.093, p = 0.034). Multivariate logistic regression analysis indicated that bladder repair after 24 h increased the risk of infection (odds = 3.162, p = 0.018). Subset analyses were performed on patients who underwent bladder repairs within 24 h and were used as a control group. These analyses showed that the time to bladder repair did not significantly worsen outcomes. CONCLUSIONS: Delayed bladder repair beyond 24 h increases the risk of infection and prolongs hospital stays. Timely diagnosis and surgical intervention remain crucial for minimizing complications in bladder injury patients.


Asunto(s)
Traumatismos Abdominales , Traumatismos Torácicos , Humanos , Vejiga Urinaria/cirugía , Tiempo de Internación , Procedimientos Quirúrgicos Urológicos , Resultado del Tratamiento , Estudios Retrospectivos
10.
Mikrochim Acta ; 190(12): 487, 2023 11 27.
Artículo en Inglés | MEDLINE | ID: mdl-38010451

RESUMEN

A new ratiometric fluorescent probe for efficient determination of ALP was developed. The probe was constructed by combining Ce3+-crosslinked copper nanoclusters (Ce3+-CuNCs) which exhibit the aggregation-induced emission (AIE) feature with carbon dots (CDs). The introduction of phosphate (Pi) induced the generation of CePO4 precipitation, resulting in significant decrease of fluorescence emission of CuNCs at 634 nm. At the same time, the fluorescence of CDs at 455 nm was obviously enhanced, thus generating ratiometric fluorescence response. Based on the fact that the hydrolysis of pyrophosphate (PPi) by ALP can produce Pi, the CD/Ce3+-CuNCs ratiometric probe was successfully used to determine ALP. A good linear relationship between the ratiometric value of F455/F634 and ALP concentrations ranging from 0.2 to 80 U·L- 1 was obtained, with a low detection limit of 0.1 U·L- 1. The ratiometric responses of the probe resulted in the visible fluorescence color change from orange red to blue with the increase of ALP concentration. The smartphone-based RGB recognition of the fluorescent sample images was used for ALP quantitative determination. A novel ratiometric fluorescent system based on Ce3+-CuNCs with AIE feature and CDs were constructed for efficient detection of ALP.


Asunto(s)
Puntos Cuánticos , Cobre , Fosfatasa Alcalina , Carbono , Fluorescencia
11.
Anal Chem ; 94(7): 3211-3218, 2022 02 22.
Artículo en Inglés | MEDLINE | ID: mdl-35104121

RESUMEN

Vacancy and doping engineering are promising pathways to improve the electrocatalytic ability of nanomaterials for detecting heavy metal ions. However, the effects of the electronic structure and the local coordination on the catalytic performance are still ambiguous. Herein, cubic selenium vacancy-rich CoSe2 (c-CoSe2-x) and P-doped orthorhombic CoSe2-x (o-CoSe2-x|P) were designed via vacancy and doping engineering. An o-CoSe2-x|P-modified glass carbon electrode (o-CoSe2-x|P/GCE) acquired a high sensitivity of 1.11 µA ppb-1 toward As(III), which is about 40 times higher than that of c-CoSe2-x, outperforming most of the reported nanomaterial-modified glass carbon electrodes. Besides, o-CoSe2-x|P/GCE displayed good selectivity toward As(III) compared with other divalent heavy metal cations, which also exhibited excellent stability, repeatability, and practicality. X-ray absorption fine structure spectroscopy and density functional theory calculation demonstrate that electrons transferred from Co and Se to P sites through Co-P and Se-P bonds in o-CoSe2-x|P. P sites obtained plentiful electrons to form active centers, which also had a strong orbital coupling with As(III). In the detection process, As(III) was bonded with P and reduced by the electron-rich sites in o-CoSe2-x|P, thus acquiring a reinforced electrochemical sensitivity. This work provides an in-depth understanding of the influence of the intrinsic physicochemical properties of sensitive materials on the behavior of electroanalysis, thus offering a direct guideline for creating active sites on sensing interfaces.


Asunto(s)
Electrónica , Electrones , Teoría Funcional de la Densidad , Espectroscopía de Absorción de Rayos X , Rayos X
12.
Anal Chem ; 94(16): 6225-6233, 2022 04 26.
Artículo en Inglés | MEDLINE | ID: mdl-35404584

RESUMEN

Interference among multiple heavy metal ions (HMIs) is a significant problem that must be solved in electroanalysis, which extremely restricts the practical popularization of electrochemical sensors. However, due to the limited exploration of the intrinsic mechanism, it is still difficult to confirm the influencing factors. In this work, a series of experimental and theoretical electroanalysis models have been established to investigate the electroanalysis results of Cu(II), Cd(II), As(III), and their mixtures, which were based on the simple structure and stable coordination of nickel single-atom catalysts. X-ray absorption spectroscopy and density functional theory calculations were used to reveal the underlying detection mechanism of the 50-fold boosting effect of Cu(II) on As(III) while Cd(II) inhibits As(III). Combining the application of the thermodynamic model and Fourier transform infrared reflection, the specific interaction of the nanomaterials and HMIs on the interface is considered to be the fundamental source of the interference. This work opens up a new way of thinking about utilizing the unique modes of interplay between nanomaterials and HMIs to achieve anti-interference intelligent electrodes in stripping analysis.


Asunto(s)
Metales Pesados , Materiales Inteligentes , Cadmio/química , Iones , Metales Pesados/química , Termodinámica
13.
Anal Chem ; 94(40): 13631-13641, 2022 10 11.
Artículo en Inglés | MEDLINE | ID: mdl-36150119

RESUMEN

Constructing high-effective electrode sensing interfaces has been considered an effective method for electrochemical detection toward heavy metal ions (HMIs). However, most research has been devoted to enhancing the stripping currents of HMIs by simply improving the adsorptive capacity and conductivity of the electrode modified materials, while lacking theoretical guidelines in fabricating catalytic sensing interfaces. Besides, the understanding of detection mechanisms is quite unscientific from the perspective of catalysis. This perspective summarizes five general strategies in designing highly efficient sensing interfaces in the recent five years, including modulating crystal phases, orientations and planes, defect engineering, ionic valence state cycle engineering, adsorption in situ catalysis strategy, and construction of atomic level catalytic active sites. What's more, the catalytic mechanisms for improving the signals of HMIs, such as boosting the electron transfer rates and conversion rates, lowering the energy barriers, etc., are introduced and emphasized. This study has a great significance in directionally controlling functionalized electrochemical sensors to achieve excellent sensitivity and selectivity in detecting environmental pollutants from the view of catalysis, and it also brings enlightenments and guidance to develop new electroanalytical methods.


Asunto(s)
Contaminantes Ambientales , Metales Pesados , Catálisis , Electrodos , Iones/química , Metales Pesados/química
14.
BMC Public Health ; 22(1): 2019, 2022 Nov 04.
Artículo en Inglés | MEDLINE | ID: mdl-36333699

RESUMEN

BACKGROUND: There is still a relatively serious disease burden of infectious diseases and the warning time for different infectious diseases before implementation of interventions is important. The logistic differential equation models can be used for predicting early warning of infectious diseases. The aim of this study is to compare the disease fitting effects of the logistic differential equation (LDE) model and the generalized logistic differential equation (GLDE) model for the first time using data on multiple infectious diseases in Jilin Province and to calculate the early warning signals for different types of infectious diseases using these two models in Jilin Province to solve the disease early warning schedule for Jilin Province throughout the year. METHODS: Collecting the incidence of 22 infectious diseases in Jilin Province, China. The LDE and GLDE models were used to calculate the recommended warning week (RWW), the epidemic acceleration week (EAW) and warning removed week (WRW) for acute infectious diseases with seasonality, respectively. RESULTS: Five diseases were selected for analysis based on screening principles: hemorrhagic fever with renal syndrome (HFRS), shigellosis, mumps, Hand, foot and mouth disease (HFMD), and scarlet fever. The GLDE model fitted the above diseases better (0.80 ≤ R2 ≤ 0.94, P <  0. 005) than the LDE model. The estimated warning durations (per year) of the LDE model for the above diseases were: weeks 12-23 and 40-50; weeks 20-36; weeks 15-24 and 43-52; weeks 26-34; and weeks 16-25 and 41-50. While the durations of early warning (per year) estimated by the GLDE model were: weeks 7-24 and 36-51; weeks 13-37; weeks 11-26 and 39-54; weeks 23-35; and weeks 12-26 and 40-50. CONCLUSIONS: Compared to the LDE model, the GLDE model provides a better fit to the actual disease incidence data. The RWW appeared to be earlier when estimated with the GLDE model than the LDE model. In addition, the WRW estimated with the GLDE model were more lagged and had a longer warning time.


Asunto(s)
Enfermedades Transmisibles , Epidemias , Paperas , Escarlatina , Humanos , Enfermedades Transmisibles/diagnóstico , Enfermedades Transmisibles/epidemiología , China/epidemiología , Paperas/epidemiología , Escarlatina/epidemiología , Incidencia
15.
Mikrochim Acta ; 189(2): 55, 2022 01 10.
Artículo en Inglés | MEDLINE | ID: mdl-35006333

RESUMEN

A novel ratiometric fluorescence nanoprobe based on long-wavelength emission carbon dots (CDs) was designed for high sensitive and selective detection of Zn2+. The CDs were conveniently prepared by a one-step solvothermal treatment of formamide and glutathione (GSH). Under single excitation wavelength (420 nm), the obtained CDs exhibit three emission peaks at 470, 650, and 685 nm, respectively. For the long-wavelength emission region of the CDs, the fluorescence at 685 nm can be quenched with different levels upon the addition of most metal ions. However, the presence of Zn2+ not only results in the fluorescence quenching at 685 nm effectively but also enhances at 650 nm remarkably, which may be due to the formation of CD-Zn2+ chelate complex inducing the dispersion of CDs aggregates and changes in the group distribution on the surface of CDs. Taking the advantage of the unique fluorescence response induced by Zn2+, the prepared CDs were successfully employed as nanoprobe for self-ratiometric fluorescence determination of Zn2+ with F650/F685 as signal output. A good linear relationship in the concentration range 0.01 to 2 µM, and a detection limit as low as 5.1 nM has been obtained. The ratiometric nanoprobe was successfully applied to  Zn2+ determination  in human serum samples.


Asunto(s)
Carbono/química , Nanoestructuras/química , Puntos Cuánticos/química , Zinc/química , Colorantes Fluorescentes , Microscopía Electrónica de Transmisión , Sensibilidad y Especificidad , Difracción de Rayos X
16.
Anal Chem ; 93(45): 15115-15123, 2021 11 16.
Artículo en Inglés | MEDLINE | ID: mdl-34714618

RESUMEN

Designing new catalysts with high activity and stability is crucial for the effective analysis of environmental pollutants under mild conditions. Here, we developed a superior catalyst of Pt single atoms anchored on MoS2 (Pt1/MoS2) to catalyze the determination of As(III). A detection sensitivity of 3.31 µA ppb-1 was obtained in acetate buffer solution at pH 6.0, which is the highest compared with those obtained by other Pt-based nanomaterials currently reported. Pt1/MoS2 exhibited excellent electrochemical stability during the detection process of As(III), even in the coexistence of Cu(II), Pb(II), and Hg(II). X-ray absorption fine structure spectroscopy and theoretical calculations revealed that Pt single atoms were stably fixed by four S atoms and activated the adjacent S atoms. Then, Pt and S atoms synergistically interacted with O and As atoms, respectively, and transferred some electrons to H3AsO3, which change the rate-determining step of H3AsO3 reduction and reduce reaction energy barriers, thereby promoting rapid and efficient accumulation for As(0). Compared with Pt nanoparticles, the weaker interaction between arsenic species and Pt1/MoS2 enabled the effortless regeneration and cyclic utilization of active centers, which is more favorable for the oxidation of As(0). This work provides inspiration for developing highly efficient sensing platforms from the perspective of atomic-level catalysis and affords references to explore the detection mechanism of such contaminants.


Asunto(s)
Arsenicales , Nanoestructuras , Arsenicales/química , Catálisis , Molibdeno , Oxidación-Reducción , Platino (Metal)
17.
Anal Chem ; 93(41): 14014-14023, 2021 10 19.
Artículo en Inglés | MEDLINE | ID: mdl-34607426

RESUMEN

An atomic-level Au nanocluster, as an excellent photocatalyst, is generally not considered as an efficient electrocatalyst due to its poor stability. Herein, a method is proposed to stabilize abundant Au25 on Fe2O3 nanoplates (Au25/OV-Fe2O3) successfully with oxygen vacancies (OV) created. Au25/OV-Fe2O3 shows superhigh catalysis in the electrochemical reduction toward As(III). The record-breaking sensitivity (161.42 µA ppb-1) is two orders of magnitude higher than currently reported, where an ultratrace limit of detection (9 ppt) is obtained, suggesting promising applications in the analysis of organic and bioactive substances. The stability of Au25 is attributed to the Au-Fe bond formed after loading Au25 nanoclusters on Fe2O3 nanoplates through "electron compensation" and bond length (Au-S) shortening. Moreover, the ligand S atoms in Au25 nanoclusters significantly contribute to the reduction of As(III). The fantastic stability and superior catalytic ability of Au25/OV-Fe2O3 provide guidelines to stabilize Au nanoclusters on metal oxides, indicating their potential electroanalytical applications.


Asunto(s)
Oro , Oxígeno , Catálisis , Ligandos
18.
J Viral Hepat ; 28(10): 1464-1473, 2021 10.
Artículo en Inglés | MEDLINE | ID: mdl-34314082

RESUMEN

Yichang is a city in central China in the Hubei Province. This study aimed to estimate the dynamics of the transmissibility of hepatitis C using a mathematical model and predict the transmissibility of hepatitis C in 2030. Data of hepatitis C cases from 13 counties or districts (cities) in Yichang from 2008 to 2016 were collected. A susceptible-infectious-chronic-recovered (SICR) model was developed to fit the data. The transmissibility of hepatitis C at the counties or districts was calculated based on new infections (including infected or chronically infected cases) reported monthly in the city caused by one infectious individual (MNI). The trend of the MNI was fitted and predicted using 11 models, with the coefficient of determination (R2 ) was being used to test the goodness of fit of these models. A total of 3065 cases of hepatitis C were reported in Yichang from 2008 to 2016. The median MNI of Yichang was 0.0768. According to the fitting results and analysis, the trend of transmissibility of hepatitis C in Yichang City conforms with the logarithmic (R2  = 0.918, p < 0.001):MNI = 0.265-0.108 log(t) and exponential (R2  = 0.939, p < 0.001): MNI = 0.344e(-0.278t) models. Hence, the transmission of hepatitis C virus at the county level has a downward trend. In conclusion, the transmissibility of hepatitis C in Yichang has a downward trend. With the current preventive and control measures in place, the spread of hepatitis C can be controlled.


Asunto(s)
Hepacivirus , Hepatitis C , China/epidemiología , Ciudades , Hepatitis C/epidemiología , Humanos , Modelos Teóricos
19.
Mikrochim Acta ; 188(8): 259, 2021 07 16.
Artículo en Inglés | MEDLINE | ID: mdl-34268632

RESUMEN

A novel ratiometric fluorescence nanoprobe based on carbon dots (CDs) and Cu nanoclusters (CuNCs) was designed for the label-free determination of uric acid (UA). The metal-organic framework (MOF) encapsulated CuNCs (ZIF-CuNC), and nitrogen-doped CDs can self-assemble into well-defined spherical nanocomposites (CD@ZIF-CuNC) due to physical adsorption. Under the excitation wavelength of 360 nm, the CD@ZIF-CuNC nanocomposites exhibit two evident intrinsic emissions peaked at 460 nm (CDs) and 620 nm (ZIF-CuNC), respectively. In the presence of H2O2, the fluorescence of CD@ZIF-CuNC at 620 nm is quenched remarkably within 1 min, while little effect on the emission at 460 nm is observed. Therefore, taking the fluorescence at 620 nm as the report signal and 460 nm as the reference signal, ratiometric quantitative determination of H2O2 was achieved with a linear range of 1-100 µM and a detection limit of 0.30 µM. The CD@ZIF-CuNC nanoprobe was successfully applied to the determination of UA that is catalyzed by uricase to produce H2O2, obtaining the linear range of 1-30 µM and the detection limit of 0.33 µM. Eventually, this strategy has been successfully applied to the determination of UA in human urine samples. A novel and convenient CDs@ZIF-CuNCs-based nanoplatform was constructed for sensitive ratiometric fluorescence determination of UA.


Asunto(s)
Colorantes Fluorescentes/química , Nanocompuestos/química , Ácido Úrico/orina , Carbono/química , Cobre/química , Humanos , Peróxido de Hidrógeno/análisis , Límite de Detección , Nanopartículas del Metal/química , Estructuras Metalorgánicas/química , Puntos Cuánticos/química , Espectrometría de Fluorescencia/métodos
20.
J Sci Food Agric ; 101(5): 1744-1757, 2021 Mar 30.
Artículo en Inglés | MEDLINE | ID: mdl-32974893

RESUMEN

Food loss of fruit and vegetables caused by postharvest diseases is a major issue worldwide. The method used to prevent and control postharvest diseases is usually to use chemical fungicides, but long-term and large-scale use will make the pathogens resistant and potentially have a negative impact on human health and the ecological environment. Therefore, finding a safe and effective biological control method instead of chemical control is a hot research topic in recent years. Endophytes, colonizing plants asymptomatically, can promote the growth of the hosts and enhance their resistance. The use of endophytes as biological control agents for postharvest diseases of fruit and vegetables has attracted increasing attention in the last 20 years. Compared with chemical control, endophytes have the advantages of being more environmentally friendly, sustainable, and safer. However, there are relatively few relevant studies, so herein we summarize the available literature. This review focuses mainly on the recent progress of using endophytes to enhance the resistance of postharvest fruit and vegetables to diseases, with the emphasis on the possible mechanisms and the potential applications. Furthermore, this article suggests future areas for study using antagonistic endophytes to prevent and control fruit and vegetable postharvest diseases: (i) screening more potential broad-spectrum anti-pathogen endophytes and their metabolic active substances by the method of macrogenomics; (ii) elucidating the underlining molecular mechanism among endophytes, harvested vegetables and fruit, pathogens, and microbial communities; (iii) needing more application research to overcome the difficulties of commercialization practice. © 2020 Society of Chemical Industry.


Asunto(s)
Endófitos/fisiología , Frutas/microbiología , Enfermedades de las Plantas/inmunología , Verduras/microbiología , Bacterias/clasificación , Bacterias/genética , Bacterias/aislamiento & purificación , Resistencia a la Enfermedad , Endófitos/clasificación , Endófitos/genética , Endófitos/aislamiento & purificación , Frutas/química , Frutas/inmunología , Enfermedades de las Plantas/microbiología , Enfermedades de las Plantas/prevención & control , Verduras/química , Verduras/inmunología
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