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1.
J Am Chem Soc ; 146(10): 6591-6603, 2024 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-38420768

RESUMO

Polymer-in-ceramic composite solid electrolytes (PIC-CSEs) provide important advantages over individual organic or inorganic solid electrolytes. In conventional PIC-CSEs, the ion conduction pathway is primarily confined to the ceramics, while the faster routes associated with the ceramic-polymer interface remain blocked. This challenge is associated with two key factors: (i) the difficulty in establishing extensive and uninterrupted ceramic-polymer interfaces due to ceramic aggregation; (ii) the ceramic-polymer interfaces are unresponsive to conducting ions because of their inherent incompatibility. Here, we propose a strategy by introducing polymer-compatible ionic liquids (PCILs) to mediate between ceramics and the polymer matrix. This mediation involves the polar groups of PCILs interacting with Li+ ions on the ceramic surfaces as well as the interactions between the polar components of PCILs and the polymer chains. This strategy addresses the ceramic aggregation issue, resulting in uniform PIC-CSEs. Simultaneously, it activates the ceramic-polymer interfaces by establishing interpenetrating channels that promote the efficient transport of Li+ ions across the ceramic phase, the ceramic-polymer interfaces, and the intervening pathways. Consequently, the obtained PIC-CSEs exhibit high ionic conductivity, exceptional flexibility, and robust mechanical strength. A PIC-CSE comprising poly(vinylidene fluoride) (PVDF) and 60 wt % PCIL-coated Li3Zr2Si2PO12 (LZSP) fillers showcasing an ionic conductivity of 0.83 mS cm-1, a superior Li+ ion transference number of 0.81, and an elongation of ∼300% at 25 °C could be produced on meter-scale. Its lithium metal pouch cells show high energy densities of 424.9 Wh kg-1 (excluding packing films) and puncture safety. This work paves the way for designing PIC-CSEs with commercial viability.

2.
Breast Cancer Res ; 26(1): 80, 2024 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-38773552

RESUMO

BACKGROUND: Cancer-related fatigue (CRF) is a pervasive, persistent, and distressing symptom experienced by cancer patients, for which few treatments are available. We investigated the efficacy and safety of infrared laser moxibustion (ILM) for improving fatigue in breast cancer survivors. METHODS: A three-arm, randomized, sham-controlled clinical trial (6-week intervention plus 12-week observational follow-up) was conducted at a tertiary hospital in Shanghai, China. The female breast cancer survivors with moderate to severe fatigue were randomized 2:2:1 to ILM (n = 56) sham ILM (n = 56), and Waitlist control (WLC)(n = 28) groups. Patients in the ILM and sham ILM (SILM) groups received real or sham ILM treatment, 2 sessions per week for 6 weeks, for a total of 12 sessions. The primary outcome was change in the Brief Fatigue Inventory (BFI) score from baseline to week 6 with follow-up until week 18 assessed in the intention-to-treat population. RESULTS: Between June 2018 and July 2021, 273 patients were assessed for eligibility, and 140 patients were finally enrolled and included in the intention-to-treat analysis. Compared with WLC, ILM reduced the average BFI score by 0.9 points (95% CI, 0.3 to 1.6, P = .007) from baseline to week 6, with a difference between the groups of 1.1 points (95% CI, 0.4 to 1.8, P = .002) at week 18. Compared with SILM, ILM treatment resulted in a non-significant reduction in the BFI score (0.4; 95% CI, -0.2 to 0.9, P = .206) from baseline to week 6, while the between-group difference was significant at week 18 (0.7; 95% CI, 0.2 to 1.3, P = .014). No serious adverse events were reported. CONCLUSION: While ILM was found to be safe and to significantly reduce fatigue compared with WLC, its promising efficacy against the sham control needs to be verified in future adequately powered trials. TRIAL REGISTRATION: Clinicaltrials.gov: NCT04144309. Registered 12 June 2018.


Assuntos
Neoplasias da Mama , Sobreviventes de Câncer , Fadiga , Moxibustão , Humanos , Feminino , Moxibustão/métodos , Moxibustão/efeitos adversos , Neoplasias da Mama/complicações , Neoplasias da Mama/terapia , Fadiga/etiologia , Fadiga/terapia , Pessoa de Meia-Idade , Resultado do Tratamento , Adulto , Qualidade de Vida , China/epidemiologia , Idoso , Raios Infravermelhos/uso terapêutico
3.
Support Care Cancer ; 30(12): 10461-10470, 2022 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-36048280

RESUMO

PURPOSE: This study sought to explore and summarize the global state of acupuncture clinical trials enrolling cancer patients included in international registries to date. METHODS: All relevant trials evaluating acupuncture-related interventions for the treatment of cancer that were registered in 16 trial registries from January 1, 2001, through December 31, 2020, were identified. Subsequent publications related to these trials were additionally retrieved from the PubMed, Cochrane Library, Embase, CNKI (China National Knowledge Infrastructure), VIP (China Science and Technology Journal Database), and Wanfang databases. We compared information included in these registries regarding completed trials with any associated publications, with a focus on study design, sample size, and selective reporting, based on the registered protocol. RESULTS: In total, 222 eligible trials across 19 countries were identified. These trials included 17 specific cancer types and 32 symptoms. The five most common cancer types were breast cancer, head and neck cancer, colorectal cancer, lung cancer, and gastric cancer, accounting for almost half of all registered trials (48.2%). The top five symptoms included in these trials were chemotherapy-induced peripheral neuropathy (CIPN), cancer-related pain, cancer-related fatigue, chemotherapy-induced nausea and vomiting (CINV), and gastrointestinal dysfunction. The overall rate of article publication was low, with publications being associated with just 33.3% of these registered trials. CONCLUSIONS: This review is the first snapshot of the landscape of acupuncture clinical trials registered in international trial registries, providing a methodological basis for the management of common treatment- and disease-related side effects among cancer patients undergoing acupuncture and offering useful information that will guide future acupuncture-focused research.


Assuntos
Terapia por Acupuntura , Acupuntura , Antineoplásicos , Neoplasias da Mama , Feminino , Humanos , Terapia por Acupuntura/métodos , Náusea/terapia , Ensaios Clínicos como Assunto
4.
J Am Chem Soc ; 142(25): 11173-11182, 2020 06 24.
Artigo em Inglês | MEDLINE | ID: mdl-32459963

RESUMO

Hydrous materials are ubiquitous in the natural environment and efforts have previously been made to investigate the structures and dynamics of hydrated surfaces for their key roles in various chemical and physical applications, with the help of theoretical modeling and microscopy techniques. However, an overall atomic-scale understanding of the water-solid interface, including the effect of water on surface ions, is still lacking. Herein, we employ ceria nanorods with different amounts of water as an example and demonstrate a new approach to explore the water-surface interactions by using solid-state NMR in combination with density functional theory. NMR shifts and relaxation time analysis provide detailed information on the local structure of oxygen ions and the nature of water motion on the surface: the amount of molecularly adsorbed water decreases rapidly with increasing temperature (from room temperature to 150 °C), whereas hydroxyl groups are stable up to 150 °C, and dynamic water molecules are found to instantaneously coordinate to the surface oxygen ions. The applicability of dynamic nuclear polarization for selective detection of surface oxygen species is also compared to conventional NMR with surface selective isotopic-labeling: the optimal method depends on the feasibility of enrichment and the concentration of protons in the sample. These results provide new insight into the interfacial structure of hydrated oxide nanostructures, which is important to improve performance for various applications.

5.
J Clin Gastroenterol ; 54(10): e93-e102, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-31904680

RESUMO

BACKGROUND: Quantitative information is scarce with regard to guidelines for currently prescribed medications for constipation. Furthermore, these guidelines do not reflect the differences in the number of bowel movements caused by each drug. GOALS: In this study, we used a model-based meta-analysis to quantitatively estimate the deviations from the baseline number of spontaneous bowel movements (SBMs) and complete spontaneous bowel movements (CSBMs) associated with pharmacotherapy for chronic constipation to bridge the knowledge gap in the guidelines for current medications. STUDY: A comprehensive survey was conducted using literature databases. In this study, we also included randomized placebo-controlled trials on chronic constipation. Pharmacodynamic models were established to describe the time course of the numbers of SBMs and CSBMs produced by each drug. RESULTS: Data from 20 studies (comprising 9998 participants and 8 drugs) were used to build this model. The results showed that bisacodyl had the greatest effect on increasing the frequency of bowel movements, whereas plecanatide yielded the lowest increase in the number of SBMs and CSBMs. After eliminating the placebo effect, the maximal increase in bowel movement frequency associated with bisacodyl was 6.8 for SBMs (95% confidence interval: 6.1-7.6) and 4.7 for CSBMs (95% confidence interval: 4.3-5.1) per week. These numbers are ∼4 times higher than the number of bowel movements produced by plecanatide. The change in the frequency of SBMs and CSBMs for other drugs, such as sodium picosulfate, velusetrag, linaclotide, elobixibat, lubiprostone, and prucalopride, was similar. The highest increases in the frequency of SBM and CSBM were 2.5 to 4 and 1 to 2.1 per week, respectively. Bisacodyl had the most noticeable loss of efficacy between week 1 and week 4; it reduced the frequencies of SBMs and CSBMs by 2.3 and 2.2, respectively. By contrast, the changes in the frequencies of SBMs and CSBMs were not as great with other drugs. CONCLUSIONS: The data provided in this study may be a valuable supplement to the medication guidelines for the treatment of chronic constipation.


Assuntos
Constipação Intestinal , Preparações Farmacêuticas , Bisacodil , Constipação Intestinal/tratamento farmacológico , Defecação , Método Duplo-Cego , Humanos , Ensaios Clínicos Controlados Aleatórios como Assunto , Resultado do Tratamento
6.
Eur J Clin Pharmacol ; 75(4): 497-509, 2019 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-30612155

RESUMO

PURPOSE: This study aimed to establish a non-linear mixed effects model to quantitatively analyze the placebo responses of neuropsychiatric symptoms (NPS) in Alzheimer's disease (AD). METHODS: A comprehensive literature search was conducted in public databases. Placebo-controlled randomized AD clinical trials using the neuropsychiatric inventory (NPI) score as the primary or secondary outcome were included. Non-linear mixed effects model was used to describe the time course of the placebo responses of NPS in AD clinical trials. Potential affecting factors were tested as covariates. RESULTS: A total of 32 clinical studies (involving 3942 subjects) were included in model-based analysis. We found that the maximal placebo responses of NPS were reached at week 4 approximately, after which rebound effects appeared. The baseline NPI score had a significant impact on the placebo responses. Higher baseline NPI score tended to cause greater reductions in NPI score at week 8 and a smaller degree of rebound. For AD patients whose normalized baseline NPI score was 10 points and 30 points, the reduction in normalized NPI score at week 8 was estimated to be 0.83 and 7.43 points, respectively; and the rebound rate after week 8 was estimated to be 0.1 points/week and 0.08 points/week, respectively. CONCLUSIONS: The duration of 4 weeks is sufficient to determine the drug efficacy for assessing NPS in AD clinical trials. The baseline NPI score was a key factor associated with placebo responses of NPS, which should be considered when designing future clinical trials and conducting comparisons across trials.


Assuntos
Doença de Alzheimer/tratamento farmacológico , Dinâmica não Linear , Efeito Placebo , Idoso , Idoso de 80 Anos ou mais , Doença de Alzheimer/psicologia , Inibidores da Colinesterase/uso terapêutico , Método Duplo-Cego , Feminino , Humanos , Masculino , Nootrópicos/uso terapêutico , Escalas de Graduação Psiquiátrica , Ensaios Clínicos Controlados Aleatórios como Assunto
7.
Prostate ; 78(7): 512-520, 2018 05.
Artigo em Inglês | MEDLINE | ID: mdl-29542178

RESUMO

PURPOSE: Recent years have brought many changes in the management of localized prostate cancer as national screening guidelines have been updated and diagnostic practice patterns evolved. We sought to better understand how the changing landscape influenced treatment utilization in the United States. METHODS: We used the SEER database in this retrospective analysis of patients with clinically localized prostate cancer between 2004 and 2013. We evaluated utilization of primary treatment modalities over time with descriptive and trend analyses, and examined treatment utilization by cancer risk group and age at diagnosis. RESULTS: Of 398 074 patients in the analytic data set, 38% elected radiation therapy, 38% underwent radical prostatectomy, and 24% opted for expectant management. While in 2004 radiation treatment was almost twice as common as expectant management (42% vs 23%), by 2013 approximately equal percentages of patients were treated with each of the three modalities. Expectant management use increased over time, while the proportion of patients opting for surgery decreased remarkably with increasing age at diagnosis in intermediate- and higher-risk disease. Among radiotherapy options, brachytherapy was most common among lower-risk patients in 2004 but substantially decreased over time (P < 0.001). CONCLUSIONS: Management of localized prostate cancer changed substantially over time in the United States. Utilization of expectant management has increased for men with low- and intermediate risk cancer. Among those who pursue curative therapy, younger men remain more likely to elect surgery whereas older men tend to choose radiotherapy. Further studies are needed to better characterize factors contributing to treatment selection.


Assuntos
Neoplasias da Próstata/terapia , Fatores Etários , Idoso , Idoso de 80 Anos ou mais , Braquiterapia/estatística & dados numéricos , Humanos , Masculino , Pessoa de Meia-Idade , Prostatectomia/estatística & dados numéricos , Neoplasias da Próstata/epidemiologia , Neoplasias da Próstata/patologia , Radioterapia/estatística & dados numéricos , Estudos Retrospectivos , Programa de SEER , Estados Unidos/epidemiologia
8.
Angew Chem Int Ed Engl ; 57(37): 12012-12016, 2018 Sep 10.
Artigo em Inglês | MEDLINE | ID: mdl-30063282

RESUMO

Selective conversion of syngas (CO/H2 ) into C2+ oxygenates is a highly attractive but challenging target. Herein, we report the direct conversion of syngas into methyl acetate (MA) by relay catalysis. MA can be formed at a lower temperature (ca. 473 K) using Cu-Zn-Al oxide/H-ZSM-5 and zeolite mordenite (H-MOR) catalysts separated by quartz wool (denoted as Cu-Zn-Al/H-ZSM-5|H-MOR) and also at higher temperatures (603-643 K) without significant deactivation using spinel-structured ZnAl2 O4 |H-MOR. The selectivity of MA and acetic acid (AA) reaches 87 % at a CO conversion of 11 % at 643 K. Dimethyl ether (DME) is the key intermediate and the carbonylation of DME results in MA with high selectivity. We found that the relay catalysis using ZnAl2 O4 |H-MOR|ZnAl2 O4 gives ethanol as the major product, while ethylene is formed with a layer-by-layer ZnAl2 O4 |H-MOR|ZnAl2 O4 |H-MOR combination. Close proximity between ZnAl2 O4 and H-MOR increases ethylene selectivity to 65 %.

9.
Int J Clin Pharmacol Ther ; 54(9): 682-92, 2016 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-27390049

RESUMO

OBJECTIVE: This study was aimed at exploring the accuracy of population pharmacokinetic method in evaluating the bioequivalence of pidotimod with sparse data profiles and whether this method is suitable for bioequivalence evaluation in special populations such as children with fewer samplings. Methods In this single-dose, two-period crossover study, 20 healthy male Chinese volunteers were randomized 1 : 1 to receive either the test or reference formulation, with a 1-week washout before receiving the alternative formulation. Noncompartmental and population compartmental pharmacokinetic analyses were conducted. Simulated data were analyzed to graphically evaluate the model and the pharmacokinetic characteristics of the two pidotimod formulations. Various sparse sampling scenarios were generated from the real bioequivalence clinical trial data and evaluated by population pharmacokinetic method. RESULTS: The 90% confidence intervals (CIs) for AUC0-12h, AUC0-∞, and Cmax were 97.3 - 118.7%, 96.9 - 118.7%, and 95.1 - 109.8%, respectively, within the 80 - 125% range for bioequivalence using noncompartmental analysis. The population compartmental pharmacokinetics of pidotimod were described using a one-compartment model with first-order absorption and lag time. In the comparison of estimations in different dataset, the estimation of random three- and< fixed four-point sampling strategies can provide results similar to those obtained through rich sampling. The nonlinear mixed-effects model requires fewer data points. Moreover, compared with the noncompartmental analysis method, the pharmacokinetic parameters can be more accurately estimated using nonlinear mixed-effects model. CONCLUSIONS: The population pharmacokinetic modeling method was used to assess the bioequivalence of two pidotimod formulations with relatively few sampling points and further validated the bioequivalence of the two formulations. This method may provide useful information for regulating bioequivalence evaluation in special populations.


Assuntos
Fatores Imunológicos/farmacocinética , Modelos Biológicos , Ácido Pirrolidonocarboxílico/análogos & derivados , Tiazolidinas/farmacocinética , Adolescente , Adulto , Área Sob a Curva , Povo Asiático , Estudos Cross-Over , Humanos , Fatores Imunológicos/administração & dosagem , Masculino , Dinâmica não Linear , Ácido Pirrolidonocarboxílico/administração & dosagem , Ácido Pirrolidonocarboxílico/farmacocinética , Equivalência Terapêutica , Tiazolidinas/administração & dosagem , Adulto Jovem
10.
J Appl Clin Med Phys ; 17(3): 147-157, 2016 05 08.
Artigo em Inglês | MEDLINE | ID: mdl-27167272

RESUMO

This study investigated the impact of beam complexities on planar quality assur-ance and plan quality robustness by introducing MLC errors in intensity-modulate radiation therapy. Forty patients' planar quality assurance (QA) plans were enrolled in this study, including 20 dynamic MLC (DMLC) IMRT plans and 20 static MLC (SMLC) IMRT plans. The total beam numbers were 150 and 160 for DMLC and SMLC, respectively. Six different magnitudes of MLC errors were introduced to these beams. Gamma pass rates were calculated by comparing error-free fluence and error-induced fluence. The plan quality variation was acquired by comparing PTV coverage. Eight complexity scores were calculated based on the beam flu-ence and the MLC sequence. The complexity scores include fractal dimension, monitor unit, modulation index, fluence map complexity, weighted average of field area, weighted average of field perimeter, and small aperture ratio (< 5 cm2 and < 50cm2). The Spearman's rank correlation coefficient was calculated to analyze the correlation between these scores and gamma pass rate and plan quality varia-tion. For planar QA, the most significant complexity index was fractal dimension for DMLC (p = -0.40) and weighted segment area for SMLC (p = 0.27) at low magnitude MLC error. For plan quality, the most significant complexity index was weighted segment perimeter for DMLC (p = 0.56) and weighted segment area for SMLC (p= 0.497) at low magnitude MLC error. The sensitivity of planar QA was weakly associated with the field complexity with low magnitude MLC error, but the plan quality robustness was associated with beam complexity. Plans with simple beams were more robust to MLC error.


Assuntos
Garantia da Qualidade dos Cuidados de Saúde/métodos , Radioterapia de Intensidade Modulada/normas , Humanos , Planejamento da Radioterapia Assistida por Computador/métodos , Radioterapia de Intensidade Modulada/instrumentação , Projetos de Pesquisa
11.
Yao Xue Xue Bao ; 50(11): 1456-60, 2015 Nov.
Artigo em Chinês | MEDLINE | ID: mdl-26911042

RESUMO

Due to a great amount of data in clinical trials, the data cleansing needs to adopt a variety of measures, including the latest developed visual check approach. According to the different types of clinical data and the different stages in the course of clinical data management, this study reviews 8 types of visual graphics that show the relevance and trend among the data. The series of graphics can rapidly detect abnormal data, monitor clinical research in real-time, make the data management process much easier and improve the clinical trial efficiency and data quality.


Assuntos
Ensaios Clínicos como Assunto/normas , Coleta de Dados/normas , Armazenamento e Recuperação da Informação/métodos
12.
Yao Xue Xue Bao ; 50(11): 1461-3, 2015 Nov.
Artigo em Chinês | MEDLINE | ID: mdl-26911043

RESUMO

Electronic case report forms (eCRFs) instead of the traditional paper case report forms (pCRFs) are increasingly used by investigators and sponsors of clinical research. We include a total of 14 phase III studies (8 pCRF, 6 eCRF) to compare paper and electronic data documentation both quantitatively and qualitatively in clinical studies. The result suggests that adaptions of electronic data capture (EDC) in clinical trials have the advantages in optimization of data capture process, improvement of data quality and earlier clinical decision compared to paper-based methods. Furthermore, the successful implementation of EDC requires accouplements with corresponding data management processes and reallocation of resources.


Assuntos
Ensaios Clínicos Fase III como Assunto , Coleta de Dados/métodos , Armazenamento e Recuperação da Informação/métodos , Informática Médica
13.
Yao Xue Xue Bao ; 50(11): 1470-3, 2015 Nov.
Artigo em Chinês | MEDLINE | ID: mdl-26911045

RESUMO

With the wide application of electronic data management (EDC), the data management is shifting to a new mode. In order to recognize the advantages of EDC, we choose 20 representative registered clinical trials, which involve 5 404 subjects and 321 sites. We found that EDC has many beneficial impacts on the course of clinical trial data management, including the process of data collection, data cleaning, data quality control and clinical trial decision-making. The result also provides a reference for the adoption of EDC in clinical trials.


Assuntos
Ensaios Clínicos como Assunto , Coleta de Dados/normas , Armazenamento e Recuperação da Informação/normas , Controle de Qualidade
14.
ACS Omega ; 8(24): 21906-21913, 2023 Jun 20.
Artigo em Inglês | MEDLINE | ID: mdl-37360471

RESUMO

The utilization of CO2 is extremely important to solve the environmental problems and coal spontaneous combustion in goaf. There are three kinds of CO2 utilization in goaf: adsorption, diffusion, and seepage. Since adsorption will consume CO2 in goaf, the optimization of CO2 injection amount is very critical. A self-developed adsorption experimental device was used to determine the CO2 adsorption capacity of three different particle sizes of lignite coal samples at 30-60 °C and 0.1-0.7 MPa. The factors affecting CO2 adsorption by coal and its thermal effect were studied. In the coal and CO2 system, the CO2 adsorption characteristic curve is not affected by temperature, but there are differences in that with different particle sizes. The adsorption capacity increases with the increase of pressure, while it decreases with the increase of temperature and particle size. Under atmospheric pressure, the adsorption capacity of coal is a logistic function relationship with temperature. Furthermore, the average adsorption heat of CO2 on lignite shows that the interaction force between CO2 molecules has a stronger effect on CO2 adsorption than the effect of heterogeneity and anisotropy on the coal surface. Finally, the existing gas injection equation is improved theoretically with CO2 dissipation, which provides a new idea for the work of CO2 prevention and fire suppression in goaf.

15.
Cancers (Basel) ; 15(10)2023 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-37345104

RESUMO

This study quantified the differences in the efficacy and safety of different stimulation domains of anti-CD19 chimeric antigen receptor (CAR) T therapy for B-cell acute lymphoblastic leukemia (B-ALL). Clinical trials related to anti-CD19 CAR T-cell therapy for B-ALL were searched in public databases from database inception to 13 November 2021. The differences in overall survival (OS) and progression-free survival (PFS) of B-ALL patients treated with anti-CAR T-cell therapy containing 4-1BB and CD28 co-stimulatory domains were compared by establishing a parametric survival function. The overall remission rate (ORR), the proportion of people with minimal residual disease (MRD)-negative complete remission (CR), the incidence of cytokine release syndrome (CRS), and the neurotoxicity across different co-stimulatory domains was assessed using a random-effects model. The correlation between the ORR, MRD-negative CR, PFS, and OS was tested. The results showed that the median OS of anti-CAR T-cell treatment containing 4-1BB and CD28 co-stimulatory domains was 15.0 months (95% CI: 11.0-20.0) and 8.5 months (95% CI: 5.0-14.0), and the median PFS was 7.0 months (95% CI: 4.0-11.5) and 3.0 months (95% CI: 1.5-7.0), respectively. Anti-CD19 CAR T-cells in the 4-1BB co-stimulatory domain showed superior benefits in patients who achieved ORR. The incidence of neurotoxicity was significantly higher in the CD28 co-stimulatory domain of anti-CD19 CAR T-cells than in the 4-1BB co-stimulatory domain. In addition, the ORR and MRD-negative CR were strongly correlated with OS and PFS, and PFS and OS were strongly correlated. The 4-1BB co-stimulatory domain suggested a better benefit-risk ratio than the CD28 co-stimulatory domain in B-ALL.

16.
Polymers (Basel) ; 15(10)2023 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-37242909

RESUMO

Despite the unique features of poly-L-lactic acid (PLLA), its mechanical properties, such as the elongation at break, need improvement to broaden its application scope. Herein, poly(1,3-propylene glycol citrate) (PO3GCA) was synthesized via a one-step reaction and evaluated as a plasticizer for PLLA films. Thin-film characterization of PLLA/PO3GCA films prepared via solution casting revealed that PO3GCA shows good compatibility with PLLA. The addition of PO3GCA slightly improves the thermal stability and enhances the toughness of PLLA films. In particular, the elongation at break of the PLLA/PO3GCA films with PO3GCA mass contents of 5%, 10%, 15%, and 20% increases to 172%, 209%, 230%, and 218%, respectively. Therefore, PO3GCA is promising as a plasticizer for PLLA.

17.
Nat Commun ; 14(1): 2301, 2023 Apr 21.
Artigo em Inglês | MEDLINE | ID: mdl-37085534

RESUMO

Solid polymer electrolytes (SPEs), which are favorable to form intimate interfacial contacts with electrodes, are promising electrolyte of choice for long-cycling lithium metal batteries (LMBs). However, typical SPEs with easily oxidized oxygen-bearing polar groups exhibit narrow electrochemical stability window (ESW), making it impractical to increase specific capacity and energy density of SPE based LMBs with charging cut-off voltage of 4.5 V or higher. Here, we apply a polyfluorinated crosslinker to enhance oxidation resistance of SPEs. The crosslinked network facilitates transmission of the inductive electron-withdrawing effect of polyfluorinated segments. As a result, polyfluorinated crosslinked SPE exhibits a wide ESW, and the Li|SPE|LiNi0.5Co0.2Mn0.3O2 cell with a cutoff voltage of 4.5 V delivers a high discharge specific capacity of ~164.19 mAh g-1 at 0.5 C and capacity retention of ~90% after 200 cycles. This work opens a direction in developing SPEs for long-cycling high-voltage LMBs by using polyfluorinated crosslinking strategy.

18.
J Phys Chem Lett ; 13(2): 471-478, 2022 Jan 20.
Artigo em Inglês | MEDLINE | ID: mdl-34995456

RESUMO

Investigation of LiOH decomposition in nonaqueous electrolytes not only expands the fundamental understanding of four-electron oxygen evolution reactions in aprotic media but also is crucial to the development of high-performance lithium-air batteries involving the formation/decomposition of LiOH. In this work, we have shown that the decomposition of LiOH by ruthenium metal catalysts in a wet DMSO electrolyte occurs at the catalyst-electrolyte interface, initiated via a potential-triggered dissolution/reprecipitation process. The in situ UV-vis methodology devised herein provides direct experimental evidence that the hydroxyl radical is a common reaction intermediate formed in several nonaqueous electrolytes; this method is applicable to study other battery systems. Our results highlight that the reactivity of the hydroxyl radical toward nonaqueous electrolyte represents a major factor limiting O2 evolution during LiOH decomposition. Coupling catalysts restraining hydroxyl reactivity with electrolytes more resistant to hydroxyl radical attack could help improve the reversibility of this reaction.

19.
Sci Adv ; 8(11): eabj7698, 2022 Mar 18.
Artigo em Inglês | MEDLINE | ID: mdl-35302845

RESUMO

Solid electrolytes are highly important materials for improving safety, energy density, and reversibility of electrochemical energy storage batteries. However, it is a challenge to modulate the coordination structure of conducting ions, which limits the improvement of ionic conductivity and hampers further development of practical solid electrolytes. Here, we present a skeleton-retained cationic exchange approach to produce a high-performance solid electrolyte of Li3Zr2Si2PO12 stemming from the NASICON-type superionic conductor of Na3Zr2Si2PO12. The introduced lithium ions stabilized in under-coordination structures are facilitated to pass through relatively large conduction bottlenecks inherited from the Na3Zr2Si2PO12 precursor. The synthesized Li3Zr2Si2PO12 achieves a low activation energy of 0.21 eV and a high ionic conductivity of 3.59 mS cm-1 at room temperature. Li3Zr2Si2PO12 not only inherits the satisfactory air survivability from Na3Zr2Si2PO12 but also exhibits excellent cyclic stability and rate capability when applied to solid-state batteries. The present study opens an innovative avenue to regulate cationic occupancy and make new materials.

20.
Chem Sci ; 13(37): 11083-11090, 2022 Sep 28.
Artigo em Inglês | MEDLINE | ID: mdl-36320476

RESUMO

Determining the different surfaces of oxide nanocrystals is key in developing structure-property relations. In many cases, only surface geometry is considered while ignoring the influence of surroundings, such as ubiquitous water on the surface. Here we apply 17O solid-state NMR spectroscopy to explore the facet differences of morphology-controlled ceria nanocrystals considering both geometry and water adsorption. Tri-coordinated oxygen ions at the 1st layer of ceria (111), (110), and (100) facets exhibit distinct 17O NMR shifts at dry surfaces while these 17O NMR parameters vary in the presence of water, indicating its non-negligible effects on the oxide surface. Thus, the interaction between water and oxide surfaces and its impact on the chemical environment should be considered in future studies, and solid-state NMR spectroscopy is a sensitive approach for obtaining such information. The work provides new insights into elucidating the surface chemistry of oxide nanomaterials.

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