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1.
J Am Chem Soc ; 145(39): 21242-21252, 2023 Oct 04.
Article in English | MEDLINE | ID: mdl-37751194

ABSTRACT

Solid-state electrolytes (SSEs) are crucial to high-energy-density lithium metal batteries, but they commonly suffer from slow Li+ transfer kinetics and low mechanical strength, severely hampering the application for all-solid-state batteries. Here, we develop a two-dimensional (2D) high-entropy lithium-ion conductor, lithium-containing transition-metal phosphorus sulfide, HE-LixMPS3 (Lix(Fe1/5Co1/5Ni1/5Mn1/5Zn1/5)PS3) with five transition-metal atoms and lithium ions (Li+) dispersed into [P2S6]2- framework layers, exhibiting high lattice distortions and a large amount of cation vacancies. Such unique features enable to efficiently accelerate the migration of Li+ in 2D [P2S6]2- interlamination, delivering a high ionic conductivity of 5 × 10-4 S cm-1 at room temperature. Moreover, the HE-LixMPS3 laminate can be employed as a building block to construct an ultrathin SSE film (∼10 µm) based on strong C-S bonding between HE-LixMPS3 and nitrile-butadiene rubber. The SSE film delivers a strong mechanical robustness (6.0 MPa, 310% elongation) and a high ionic conductivity of 4 × 10-4 S cm-1, showing a long cycle stability of 800 h in lithium symmetric cells. Coupled with LiFePO4 cathode and lithium anode, the all-solid-state battery presents a high Coulombic efficiency of 99.8% within 2000 cycles at 5.0 C.

2.
Adv Mater ; 35(36): e2301399, 2023 Sep.
Article in English | MEDLINE | ID: mdl-37381914

ABSTRACT

Low-dielectric-constant materials such as silicon dioxide serving as interconnect insulators in current integrated circuit face a great challenge due to their relatively high dielectric constant of ≈4, twice that of the recommended value by the International Roadmap for Devices and Systems, causing severe parasitic capacitance and associated response delay. Here, novel atomic layers of amorphous carbon nitride (a-CN) are prepared via a topological conversion of MXene-Ti3 CNTx under bromine vapor. Remarkably, the assembled a-CN film exhibits an ultralow dielectric constant of 1.69 at 100 kHz, much lower than the previously reported dielectric materials such as amorphous carbon (2.2) and fluorinated-doped SiO2 (3.6), ascribed to the low density of 0.55 g cm-3 and high sp3 C level of 35.7%. Moreover, the a-CN film has a breakdown strength of 5.6 MV cm-1 , showing great potential in integrated circuit application.

3.
Adv Mater ; 35(39): e2302141, 2023 Sep.
Article in English | MEDLINE | ID: mdl-37172077

ABSTRACT

Although 2D transition metal carbides and nitrides (MXenes) have fantastic physical and chemical properties as well as wide applications, it remains challenging to produce stable MXenes due to their rapid structural degradation. Here, unique metal-bonded atomic layers of transition metal carbides with high stabilities are produced via a simple topological reaction between chlorine-terminated MXenes and selected metals, where the metals enable them to not only remove partially Cl terminations, but also bond with adjacent atomic MXene slabs, driven by the symmetry of MAX phases. The films constructed from Al-bonded Ti3 C2 Clx atomic layers show high oxidation resistance up to 400 °C and low sheet resistance of 9.3 Ω sq-1 . Coupled to the multilayer structure, the Al-bonded Ti3 C2 Clx film displays a significantly improved electromagnetic interference (EMI) shielding capability with a total shielding effectiveness value of 39 dB at a low thickness of 3.1 µm, outperforming pure Ti3 C2 Clx film.

4.
Adv Mater ; 35(18): e2212111, 2023 May.
Article in English | MEDLINE | ID: mdl-36813267

ABSTRACT

Lithium-metal-based solid-state batteries (Li-SSBs) are one of the most promising energy storage devices due to their high energy densities. However, under insufficient pressure constraints (

5.
Small Methods ; 7(8): e2201559, 2023 Aug.
Article in English | MEDLINE | ID: mdl-36811328

ABSTRACT

Associated with the rapid development of 2D transition metal carbides, nitrides, and carbonitrides (MXenes), MXene derivatives have been recently exploited and exhibited unique physical/chemical properties, holding promising applications in the areas of energy storage and conversions. This review provides a comprehensive summarization of the latest research and progress on MXene derivatives, including termination-tailored MXenes, single-atom implanted MXenes, intercalated MXenes, van der Waals atomic layers, and non-van der Waals heterostructures. The intrinsic relationship between structure, properties, and corresponding applications for MXene derivatives are then emphasized. Finally, the essential challenges are addressed and perspectives for the MXene derivatives are also discussed.

6.
Talanta ; 256: 124327, 2023 May 01.
Article in English | MEDLINE | ID: mdl-36758506

ABSTRACT

Upconversion nanoparticles (UCNPs)-based fluorescence probes have shown great potential in point-of-care testing (POCT) applications, due to UCNPs' features of high photostability and background-free fluorescence. Ceaseless improvements of UCNPs-probes have been carried out to increase detection sensitivity and to broaden detection range of UCNPs-based POCT. In this paper, we optimized UCNPs-probes by regulating probe density. The optimization was verified by a traditional lateral flow assay (LFA) platform for C-reactive protein (CRP) detection. Further, the optimized UCNPs-LFA integrating with a home-made benchtop fluorescence analyzer holds the capability to achieve high-performance POCT. Finally, nearly a 20 times sensitivity enhancement with a limit of detection of 0.046 ng/mL and a broad detection range of 0.2-300 ng/mL for CRP detection was obtained. Moreover, the optimized UCNPs-LFA was applied to detecting CRP in clinical serum samples and the detection results were consistent with the clinical test, validating its clinical practicability. The proposed optimization method is also expected to optimize other nanoparticles-based bio-probes for wider POCT application.


Subject(s)
Nanoparticles , Limit of Detection , Fluorescent Dyes , C-Reactive Protein
7.
J Hand Surg Am ; 48(2): 198.e1-198.e11, 2023 02.
Article in English | MEDLINE | ID: mdl-35012797

ABSTRACT

PURPOSE: To introduce toe-to-hand transplantation performed with the assistance of both bone and soft tissue modeling using 3-dimensional printing technology. METHODS: From May 2015 to October 2018, 31 patients (group A, 24 thumbs and 7 fingers) were included. Computed tomography scans were acquired using a spiral computed tomography scanner, and the data were processed with software. Bone, skin, and nail models were created for tailoring the flap taken from the great toe. The impact of foot pathology in terms of pain, disability, and activity restriction was assessed using the Foot Function Index. For comparison, we included 35 patients (group B) who underwent toe-to-hand transplantation without the assistance of 3-dimensional computer-aided modeling. RESULTS: The mean duration of follow-up of groups A and B was 26 months (range, 24-31 months) and 27 months (range, 24-33 months), respectively. The mean Foot Function Index of groups A and B was 5 (range: 0-15) and 17 (range, 0-39), respectively. CONCLUSIONS: Three-dimensional computer-aided modeling and printing provide geometric accuracy in toe-to-hand transplantation. It also may reduce the donor foot morbidity by accurate flap designing and harvesting. TYPE OF STUDY/LEVEL OF EVIDENCE: Therapeutic IV.


Subject(s)
Amputation, Traumatic , Finger Injuries , Hand Transplantation , Humans , Toes , Finger Injuries/surgery , Amputation, Traumatic/surgery , Skin Transplantation/methods , Computer-Aided Design , Printing, Three-Dimensional
8.
Biosensors (Basel) ; 12(11)2022 Nov 07.
Article in English | MEDLINE | ID: mdl-36354486

ABSTRACT

Inflammation caused by viral or bacterial infection is a major threat to human health globally. Blood C-reactive protein (CRP) has been proven to be a sensitive indicator for the occurrence and development of inflammation. Furthermore, a tiny change of blood CRP concentration may portend chronic diseases; therefore, high-sensitivity CRP (hs-CRP) detection in a quantitative, rapid, user-friendly, and low-cost manner is highly demanded. In this paper, we developed a europium-chelate polystyrene microsphere (EuPSM)-based lateral flow immunoassay (LFIA) integrating with a benchtop fluorescence analyzer for hs-CRP detection. The optimization of the EuPSM-based LFIA was implemented through adjusting the antibody density on EuPSM from 100% to 60% of the saturated density. Finally, the limit of detection of 0.76 pg/mL and detection range of 0.025-250 ng/mL were obtained. Moreover, the clinical application capability of the proposed platform was validated through detecting CRP in clinical serum samples, showing high consistency with the results obtained from the clinical standard method. Hence, the proposed EuPSM-based LFIA has been verified to be well suitable for hs-CRP detection, while also showing great applicability for sensitively and rapidly detecting other biomarkers.


Subject(s)
C-Reactive Protein , Polystyrenes , Humans , C-Reactive Protein/analysis , Microspheres , Immunoassay/methods , Europium , Inflammation
9.
Quant Imaging Med Surg ; 12(2): 1549-1557, 2022 Feb.
Article in English | MEDLINE | ID: mdl-35111647

ABSTRACT

BACKGROUND: Quantitative assessments based on optical coherence tomographic angiography (OCTA) may have potential promising value in the early detection of non-arteritic anterior ischemic optic neuropathy (NA-AION), but there is limited information on the ability of OCTA to distinguish eyes with NA-AION. This study was conducted to evaluate the ability of measurements of peripapillary perfusion using OCTA to distinguish healthy eyes from eyes with NA-AION. METHODS: In this retrospective case-control study, newly diagnosed NA-AION patients and healthy controls matched at a ratio of 1:3 by gender and age (±5 years) were enrolled from 1 September 2020 to 30 June 2021. Peripapillary vessel density (pVD) was examined based on the area of vessels by means of a 4.5 mm OCTA scan. In addition, peripapillary retinal nerve fiber layer (pRNFL) thickness was obtained from structural optical coherence tomography (OCT), as was the area under the receiver operating characteristic (ROC) curve (AUC). RESULTS: A total of 29 eyes from 28 cases with NA-AION and 99 healthy eyes from 68 participants were imaged. All participants were Chinese. The NA-AION group showed a significant reduction of the pVD (P<0.001), while all subregions of pRNFL thickness were prominent in all 8 quadrants (P>0.05). The pVD of the optic disc in the superior temporal (ST) region showed better diagnostic accuracy (AUC =0.86) in discriminating the NA-AION group from healthy controls. After adjusting for confounders, ST was independently associated with the presence of NA-AION [odds ratio (OR) =0.971, 95% confidence interval (CI): 0.943-0.990, P=0.048]. CONCLUSIONS: Decreased pVD was detected by non-invasive measurements of OCTA in the eyes of NA-AION patients. This finding may reveal an association between the ST region and the presence of NA-AION. The pVD may have potential diagnostic ability and may serve as an additional biomarker in the management of the disease.

10.
ACS Nano ; 15(12): 19275-19283, 2021 Dec 28.
Article in English | MEDLINE | ID: mdl-34898180

ABSTRACT

Although transition metal dichalcogenides (TMDs) monolayers are widely applied in electronics, optics, catalysis, and energy storage, their yield or output is commonly very low (<1 wt % or micrometer level) based on the well-known top-down (e.g., exfoliation) and bottom-up (e.g., chemical vapor deposition) approaches. Here, 1T MoS2 monolayers with a very high fraction of ∼90% were achieved via the conversion of Mo-based MXenes (Mo2CTx and Mo1.33CTx) at high temperatures in hydrogen sulfide gas, in which the Mo-layer of Mo-based MXenes could be transformed to MoS2 monolayers and the Mo vacancies facilitate the gliding of sulfur layers to form 1T MoS2. The resultant 1T MoS2 monolayers with numerous vacancies exhibit strong chemisorption and high catalytic activity for lithium polysulfides (LiPSs), delivering a reversible capacity of 736 mAh g-1 at 0.5 C, a superior rate capability of 532 mAh g-1 at 5 C, and a good stability up to 200 cycles at 1 C in lithium-sulfur (Li-S) batteries.

11.
Front Med (Lausanne) ; 8: 715213, 2021.
Article in English | MEDLINE | ID: mdl-34422870

ABSTRACT

Background: There is little evidence on the changing prevalence, microbiological profile, and outcome of nosocomial Acinetobacter baumannii complex (ABC)-caused bloodstream infection (ABCBSI) specified in intensive care units (ICUs) in long-term studies, especially in China. Objective: We aimed to investigate changes in incidence, antibiotic resistance, therapy, and prognosis of ABCBSI in ICUs in eastern China during 2009-2018. Methods: A multicenter retrospective cohort study was conducted, and microbiological and clinical data for patients with ABCBSI acquired in nine adult ICUs in eastern China from 2009 to 2018. Results: A total of 202 cases were enrolled. For the years 2009-2010, 2011-2012, 2013-2014, 2015-2016, and 2017-2018, the incidence of ABCBSI increased significantly, as did the percentage of pan-drug-resistant isolates and resistant rates to most of antimicrobial agents; the percentage of drug-sensitive isolates decreased (all P < 0.05). The frequency of treatment with carbapenems and tigecycline increased, and that of cephalosporins decreased. Compared with those in the first years (2009-2012), ABCBSI patients in the lattermost years (2017-2018) were less often treated with appropriate empirical therapy, more often underwent pneumonia-related ABCBSI and mechanical ventilation support, and had higher 28-day mortality rates. Multivariate Cox regression indicated that increase in the degree of ABC antibiotics resistance, pneumonia-related ABCBSI, and septic shock were risk factors of 28-day mortality and associated with significant lower survival days. Conclusions: The past decade has witnessed a marked increase in the incidence of ABCBSI and in antibiotic resistance, with increasing pneumonia-related infections and worrisome mortality in ICUs in China. Controlling increasing resistance and preventing nosocomial pneumonia may play important roles in combatting these infections.

12.
Adv Mater ; 33(39): e2101473, 2021 Oct.
Article in English | MEDLINE | ID: mdl-34365658

ABSTRACT

High-entropy materials (HEMs) have great potential for energy storage and conversion due to their diverse compositions, and unexpected physical and chemical features. However, high-entropy atomic layers with fully exposed active sites are difficult to synthesize since their phases are easily segregated. Here, it is demonstrated that high-entropy atomic layers of transition-metal carbide (HE-MXene) can be produced via the selective etching of novel high-entropy MAX (also termed Mn +1 AXn (n = 1, 2, 3), where M represents an early transition-metal element, A is an element mainly from groups 13-16, and X stands for C and/or N) phase (HE-MAX) (Ti1/5 V1/5 Zr1/5 Nb1/5 Ta1/5 )2 AlC, in which the five transition-metal species are homogeneously dispersed into one MX slab due to their solid-solution feature, giving rise to a stable transition-metal carbide in the atomic layers owing to the high molar configurational entropy and correspondingly low Gibbs free energy. Additionally, the resultant high-entropy MXene with distinct lattice distortions leads to high mechanical strain into the atomic layers. Moreover, the mechanical strain can efficiently guide the nucleation and uniform growth of dendrite-free lithium on HE-MXene, achieving a long cycling stability of up to 1200 h and good deep stripping-plating levels of up to 20 mAh cm-2 .

13.
ACS Nano ; 15(3): 4927-4936, 2021 Mar 23.
Article in English | MEDLINE | ID: mdl-33617242

ABSTRACT

Single atom catalysts possess attractive electrocatalytic activities for various chemical reactions owing to their favorable geometric and electronic structures compared to the bulk counterparts. Herein, we demonstrate an efficient approach to producing single atom copper immobilized MXene for electrocatalytic CO2 reduction to methanol via selective etching of hybrid A layers (Al and Cu) in quaternary MAX phases (Ti3(Al1-xCux)C2) due to the different saturated vapor pressures of Al- and Cu-containing products. After selective etching of Al in the hybrid A layers, Cu atoms are well-preserved and simultaneously immobilized onto the resultant MXene with dominant surface functional group (Clx) on the outmost Ti layers (denoted as Ti3C2Clx) via Cu-O bonds. Consequently, the as-prepared single atom Cu catalyst exhibits a high Faradaic efficiency value of 59.1% to produce CH3OH and shows good electrocatalytic stability. On the basis of synchrotron-based X-ray absorption spectroscopy analysis and density functional theory calculations, the single atom Cu with unsaturated electronic structure (Cuδ+, 0 < δ < 2) delivers a low energy barrier for the rate-determining step (conversion of HCOOH* to absorbed CHO* intermediate), which is responsible for the efficient electrocatalytic CO2 reduction to CH3OH.

14.
Clin Infect Dis ; 71(12): 3154-3162, 2020 12 15.
Article in English | MEDLINE | ID: mdl-32556293

ABSTRACT

BACKGROUND: Our aim in this study was to identify a prognostic biomarker to predict the disease prognosis and reduce the mortality rate of coronavirus disease 2019 (COVID-19), which has caused a worldwide pandemic. METHODS: COVID-19 patients were randomly divided into training and test groups. Univariate and multivariate Cox regression analyses were performed to identify the disease prognosis signature, which was selected to establish a risk model in the training group. The disease prognosis signature of COVID-19 was validated in the test group. RESULTS: The signature of COVID-19 was combined with the following 5 indicators: neutrophil count, lymphocyte count, procalcitonin, age, and C-reactive protein. The signature stratified patients into high- and low-risk groups with significantly relevant disease prognosis (log-rank test, P < .001) in the training group. The survival analysis indicated that the high-risk group displayed substantially lower survival probability than the low-risk group (log-rank test, P < .001). The area under the receiver operating characteristic (ROC) curve showed that the signature of COVID-19 displayed the highest predictive accuracy regarding disease prognosis, which was 0.955 in the training group and 0.945 in the test group. The ROC analysis of both groups demonstrated that the predictive ability of the signature surpassed the use of each of the 5 indicators alone. CONCLUSIONS: The signature of COVID-19 presents a novel predictor and prognostic biomarker for closely monitoring patients and providing timely treatment for those who are severely or critically ill.


Subject(s)
COVID-19 , Humans , Pandemics , Prognosis , ROC Curve , SARS-CoV-2
15.
Nature ; 577(7791): 492-496, 2020 01.
Article in English | MEDLINE | ID: mdl-31969724

ABSTRACT

Although two-dimensional (2D) atomic layers, such as transition-metal chalcogenides, have been widely synthesized using techniques such as exfoliation1-3 and vapour-phase growth4,5, it is still challenging to obtain phase-controlled 2D structures6-8. Here we demonstrate an effective synthesis strategy via the progressive transformation of non-van der Waals (non-vdW) solids to 2D vdW transition-metal chalcogenide layers with identified 2H (trigonal prismatic)/1T (octahedral) phases. The transformation, achieved by exposing non-vdW solids to chalcogen vapours, can be controlled using the enthalpies and vapour pressures of the reaction products. Heteroatom-substituted (such as yttrium and phosphorus) transition-metal chalcogenides can also be synthesized in this way, thus enabling a generic synthesis approach to engineering phase-selected 2D transition-metal chalcogenide structures with good stability at high temperatures (up to 1,373 kelvin) and achieving high-throughput production of monolayers. We anticipate that these 2D transition-metal chalcogenides will have broad applications for electronics, catalysis and energy storage.

16.
ACS Nano ; 14(1): 891-898, 2020 Jan 28.
Article in English | MEDLINE | ID: mdl-31913604

ABSTRACT

Lithium (Li) metal has been considered as one of the most prospective anodes for Li-based batteries owing to its high theoretical gravimetric capacity (3860 mAh g-1) and low potential (-3.04 V vs standard hydrogen electrode (SHE)). Unfortunately, there commonly exist uncontrollable dendrites in lithium anodes during the repeated plating-stripping processes, causing short cycle life and even short circuiting of lithium batteries. Here, single zinc atoms immobilized on MXene (Ti3C2Clx) layers (Zn-MXene) were produced to efficiently induce Li nucleation and growth. At the initial plating stage, lithium tended to nucleate homogeneously on the surface of Zn-MXene layers due to the large presence of Zn atoms and then grow vertically along the nucleated sites owing to a strong lightning rod effect at the edges, affording bowl-like lithium without lithium dendrites. Thus, a low overpotential of 11.3 ± 0.1 mV, long cyclic life (1200 h), and deep stripping-plating levels up to 40 mAh cm-2 are obtained by using Zn-MXene films as lithium anodes.

17.
Theriogenology ; 143: 10-17, 2020 Feb.
Article in English | MEDLINE | ID: mdl-31830685

ABSTRACT

The effects of gonadotropin, serum and follicular fluid on the in vitro maturation of canine oocytes were examined. Additionally, spindle size and spindle migration in MI-stage oocytes derived by in vivo or in vitro maturation were evaluated for the first time. Mature oocytes collected from beagle dog ovaries were divided into two experiments. In experiment I, oocytes were cultured in basic TCM 199 medium supplemented with different levels of P4, E2 and FSH. In experiment II, oocytes in the estrus or anestrus stage were cultured in basic medium supplemented with 30% or 40% canine serum plus 20% or 10% follicular fluid. Our results showed that in experiment I, more oocytes reached MI-MII (18.57%) after supplementation with 1 IU/ml FSH+ 5 IU/ml P4 + 5 IU/ml E2 than after supplementation with other levels of reagents. However, there were no significant differences among the groups (three different concentration groups and a control group) with respect to the proportions of oocytes that resumed meiosis, completed meiosis or degenerated. In experiment II, the number of oocytes from the estrus stage that reached MI-MII in TCM 199 medium supplemented with 40% canine serum and 10% follicular fluid (46.72%) was significantly higher (p < 0.01) than the number of oocytes from the anestrus stage that reached MI-MII in medium supplemented with 30% canine serum and 20% follicular fluid (21.84%). In addition, the degeneration rate was significantly lower (p < 0.05) in the 40% canine serum/10% follicular fluid group from follicular stage than in the other three groups. The average spindle length of the MI-stage oocytes that matured in vivo was significantly (p < 0.01) longer than that of the MI-stage oocytes that matured in vitro (21.75 vs. 14.39 µm). These results suggest that supplementation of the culture medium with 40% estrus serum and 10% follicular fluid had a positive influence on the in vitro maturation of canine oocytes and greatly affected spindle size in MI-stage oocytes.


Subject(s)
Culture Media/pharmacology , Dogs/physiology , Follicular Fluid , In Vitro Oocyte Maturation Techniques/veterinary , Oocytes/drug effects , Serum , Animals , Culture Media/chemistry , Estradiol/pharmacology , Estrous Cycle/physiology , Female , Follicle Stimulating Hormone/pharmacology , In Vitro Oocyte Maturation Techniques/methods , Oocytes/physiology , Progesterone/pharmacology
18.
Adv Mater ; 31(44): e1904369, 2019 Nov.
Article in English | MEDLINE | ID: mdl-31538380

ABSTRACT

Owing to the intense charge repulsion of multivalent ions and intrinsic slugggish kenetics, vast and fast storage of zinc ions into electrode materials has remained unattainable. Here, an efficient strategy to unlock the electrochemical activity of rocksalt vanadium oxynitride is developed via the substitution of low-valent oxygen for high-valent nitrogen, forming disordered rocksalt with abundant vacancies/defects due to the charge-compensating function. Unexpectedly, the disordered rocksalt not only provides plentiful active sites for zinc ions but is also beneficial for the rapid diffusion of zinc ions, owing to the large presence of vacancies/defects in the matrix. Hence, a very high reversible capacity (603 mAh g-1 , 0.2C) and high rate capability (124 mAh g-1 at 600C) are achieved for zinc storage. This should open a new and efficient avenue for the design of electrode materials with both high energy and power densities for aqueous zinc-ion batteries.

19.
Small ; 15(45): e1904587, 2019 Nov.
Article in English | MEDLINE | ID: mdl-31556236

ABSTRACT

2D materials have played an important role in electronics, sensors, optics, electrocatalysis, and energy storage. Many methods for the preparation of 2D materials have been explored. It is crucial to develop a high-yield, rapid, and low-temperature method to synthesize 2D materials. A general, fast (5 min), and low-temperature (≈100 °C) salt (CoCl2 ·6H2 O)-templated method is proposed to prepare series of 2D metal oxides/oxychlorides/hydroxides in large scale, such as MoO3 , SnO2 , SiO2 , BiOCl, Sb4 O5 Cl2 , Zn2 Co3 (OH)10 2H2 O, and ZnCo2 O4 . The as-synthesized 2D materials possess an ultrathin feature (2-7 nm) and large aspect ratios. Additionally, these 2D metal oxides/oxychlorides/hydroxides exhibit good electrochemical properties in energy storage (lithium/sodium-ion batteries) and electrocatalysis (hydrogen/oxygen evolution reaction).

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