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1.
Macromol Rapid Commun ; : e1900573, 2020 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-32022971

RESUMO

Nanocomposite hydrogels (NCs) with mechanical properties suitable for a diverse range of applications can be made by combining polymer hydrogel networks with various inorganic nanoparticles. However, the mechanical properties and functions of conventional NCs are seriously limited by the poor structural or functional tunability of common nanofillers and by the low amounts of such fillers that can be added. Here, the fabrication of novel elastically stretchable and compressible nanocomposite hydrogels (MIL-101-MAAm/PAAm) with a distinctive pearl-net microstructure and a metal-organic framework (MOF) content in the range of 20-60 wt% through post-synthetic polymerization (PSP) is reported. The MOFs, which are compatible with polymers and have a high degree of modifiability in structure and functions, are used as nanofillers. Such MOF-laden hydrogels can withstand 500% tensile strain or 90% compressive strain without fracture and recover quickly upon unloading. They are also resistant to freezing at -25 °C. In addition, the problems associated with poor flexibility and processability of MOFs are overcome by the hybridization of hydrogel polymer matrices with MOFs. The results of this work not only provide a new perspective on preparing NCs but also indicate a promising path for applying MOFs in flexible devices.

2.
Int J Pharm ; : 119122, 2020 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-32035259

RESUMO

A facile approach was developed to synthesize an innovative hyaluronic acid-modified carbon dot-doxorubicin nanoparticles drug delivery platform. CD44 targeted HA-modified carbon dots (HA-CDs) were synthesized as carrier by one-step hydrothermal treatment within one hour with citric acid and branch-PEI as core carbon source. HA not only functioned as carbon dot component but also as hydrophilic group and targeting ligand of this system. The as-prepared HA-CDs were then loaded with doxorubicin (HA-CD@p-CBA-DOX) via an acid-cleavable bond, which released drug in a pH-responsive manner. In in vitro experiments, HA-CD@p-CBA-DOX displayed good hemocompatibility and serum stability, while exhibited high cytotoxicity on 4T1 cells. The confocal laser scanning microscopy and flow cytometry results demonstrated that DOX-loaded nanoparticles were internalized by 4T1 cells via HA-mediated CD44-targeting effect. The enhanced in vivo tumor accumulation of HA-CD@p-CBA-DOX was testified by live imaging. Compared with free DOX, superior in vivo anti-tumor efficacy of HA-CD@p-CBA-DOX was observed in both heterotopic and orthotopic 4T1 cell tumor models. Furthermore, blood hematology and blood biochemistry analysis demonstrated that HA-CD@p-CBA-DOX did not induce noticeable toxicity, which further confirmed the good biocompatibility of HA-CD@p-CBA-DOX. The formulated HA-CD@p-CBA-DOX provides an alternative strategy for targeted breast cancer therapy.

3.
Bioinformatics ; 2020 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-32003771

RESUMO

MOTIVATION: LINCS L1000 dataset contains numerous cellular expression data induced by large sets of perturbagens. Although it provides invaluable resources for drug discovery as well as understanding of disease mechanisms, the existing peak deconvolution algorithms cannot recover the accurate expression level of genes in many cases, inducing severe noise in the dataset and limiting its applications in biomedical studies. RESULTS: Here, we present a novel Bayesian-based peak deconvolution algorithm that gives unbiased likelihood estimations for peak locations and characterize the peaks with probability based z-scores. Based on the above algorithm, we build a pipeline to process raw data from L1000 assay into signatures that represent the features of perturbagen. The performance of the proposed pipeline is evaluated using similarity between the signatures of bio-replicates and the drugs with shared targets, and the results show that signatures derived from our pipeline gives a substantially more reliable and informative representation for perturbagens than existing methods. Thus, the new pipeline may significantly boost the performance of L1000 data in the down-stream applications such as drug repurposing, disease modeling, and gene function prediction. AVAILABILITY: The code and the precomputed data for LINCS L1000 Phase II (GSE 70138) are available at https://github.com/njpipeorgan/L1000-bayesian. SUPPLEMENTARY INFORMATION: Supplementary data are available at Bioinformatics online.

4.
Med Eng Phys ; 2020 Jan 13.
Artigo em Inglês | MEDLINE | ID: mdl-31948772

RESUMO

The clinical presentation and natural courses in acute non-A-non-B aortic dissection (AD) are quite different from classical acute type A or type B AD, and the benefit of hybrid technique for this clinical scenario has not been validated. By using computational fluid dynamics (CFD) analysis, we aim to investigate a series of hemodynamic-related changes in aortic morphology in a patient who underwent type I hybrid arch repair (HAR). Computed tomographic angiographies (preoperative, one week, one month and one year after HAR) of a 52-year old male patient with arch-entry type acute non-A-non-B dissection were collected. Three-dimensional models were reconstructed by using an image processing package Mimics (materialize). Morphological and hemodynamic parameters of aorta and its branch vessels were analysed. Post-operatively, the false lumen index (FLI) gradually decreased from 2.02 to 0.38 and the curvature of the aortic arch was also reduced. However, the aortic arch lengthened and the diameter of the distal abdominal aorta expanded. In addition, the blood flow gradually became organised and the pressure in the true lumen (TL) increased over time and eventually approximated the pressure in the false lumen (FL). Moreover, the region of the abnormal wall shear stress (WSS) in the TL progressively decreased while the WSS in most areas of the FL remained below 4 dyne/cm2. The blood supply to most of the aortic branches returned to normal at the one-year follow-up. Type I HAR is an effective procedure for patients with acute non-A-non-B aortic dissection in terms of restoring normal blood flow in TL and facilitating positive remodeling of distal aorta. Long-term surveillance and follow-up is mandatory.

5.
Nat Commun ; 11(1): 537, 2020 Jan 27.
Artigo em Inglês | MEDLINE | ID: mdl-31988288

RESUMO

Despite its small land coverage, urban land and its expansion have exhibited profound impacts on global environments. Here, we present the scenario projections of global urban land expansion under the framework of the shared socioeconomic pathways (SSPs). Our projections feature a fine spatial resolution of 1 km to preserve spatial details. The projections reveal that although global urban land continues to expand rapidly before the 2040s, China and many other Asian countries are expected to encounter substantial pressure from urban population decline after the 2050s. Approximately 50-63% of the newly expanded urban land is expected to occur on current croplands. Global crop production will decline by approximately 1-4%, corresponding to the annual food needs for a certain crop of 122-1389 million people. These findings stress the importance of governing urban land development as a key measure to mitigate its negative impacts on food production.

6.
J Biochem Mol Toxicol ; : e22444, 2020 Jan 18.
Artigo em Inglês | MEDLINE | ID: mdl-31954379

RESUMO

Smoking is associated with an increased risk of respiratory diseases, including lung cancer and asthma. However, the mechanisms or diagnostic markers for smoking-related diseases remain largely unknown. Here we investigated the role of cigarette smoke condensate (CSC) in the regulation of human bronchial epithelial cell (BEAS-2B) behavior. We found that exposure to CSC significantly inhibited BEAS-2B cell viability, impaired cell morphology, induced cell apoptosis, triggered oxidative damage, and promoted inflammatory response, which suggests a deleterious effect of CSC on bronchial epithelial cells. In addition, CSC markedly altered the expression of apoptosis-associated protein factors, including p21, soluble tumor necrosis factor receptor 1, and Fas ligand. In sum, our study identified a panel of novel protein factors that may mediate the actions of CSC on bronchial epithelial cells and have a predictive value for the development and progression of smoking-related diseases, thus providing insights into the development of potential diagnostic and therapeutic strategies against these diseases.

7.
Mol Ther ; 28(1): 279-292, 2020 Jan 08.
Artigo em Inglês | MEDLINE | ID: mdl-31636038

RESUMO

Inflammation is associated with retinal diseases. Our recent data demonstrate that immunoproteasome catalytic subunit ß2i contributes to angiotensin II (Ang II)-induced retinopathy in mice. Here, we investigated the role of another catalytic subunit ß5i in regulating retinopathy and its underlying mechanisms. We induced a murine model of retinopathy by infusing Ang II (3,000 ng/kg/min) for 3 weeks into wild-type (WT) mice, ß5i-knockout (KO) mice, or WT mice injected with either adenovirus-expressing ß5i (Ad-ß5i) or angiotensin II type 1 receptor (AT1R)-associated protein (Ad-ATRAP), which inhibits AT1R. The ß5i expression and chymotrypsin-like activity were most significantly elevated in Ang II-infused retinas and serum from patients with hypertensive retinopathy. Moreover, Ang II infusion-induced retinopathy was markedly attenuated in ß5i-KO mice but aggravated in Ad-ß5i-injected mice. Accordingly, ß5i KO markedly restored Ang II-induced downregulation of ATRAP and activation of AT1R downstream mediators, which was further enhanced in Ad-ß5i-injected mice. Interestingly, overexpression of ATRAP significantly abrogated Ang II-induced retinopathy in Ad-ß5i-injected mice. This study found that ß5i promoted Ang II-induced retinopathy by promoting ATRAP degradation and activation of AT1R-mediated signals.

8.
Aging Cell ; 19(2): e13095, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31880094

RESUMO

To determine whether 1,25-dihydroxyvitamin D (1,25(OH)2 D) can exert an anti-osteoporosis role through anti-aging mechanisms, we analyzed the bone phenotype of mice with 1,25(OH)2 D deficiency due to deletion of the enzyme, 25-hydroxyvitamin D 1α-hydroxylase, while on a rescue diet. 1,25(OH)2 D deficiency accelerated age-related bone loss by activating the p16/p19 senescence signaling pathway, inhibiting osteoblastic bone formation, and stimulating osteoclastic bone resorption, osteocyte senescence, and senescence-associated secretory phenotype (SASP). Supplementation of exogenous 1,25(OH)2 D3 corrected the osteoporotic phenotype caused by 1,25(OH)2 D deficiency or natural aging by inhibiting the p16/p19 pathway. The proliferation, osteogenic differentiation, and ectopic bone formation of bone marrow mesenchymal stem cells derived from mice with genetically induced deficiency of the vitamin D receptor (VDR) were significantly reduced by mechanisms including increased oxidative stress, DNA damage, and cellular senescence. We also demonstrated that p16 deletion largely rescued the osteoporotic phenotype caused by 1,25(OH)2 D3 deficiency, whereas 1,25(OH)2 D3 could up-regulate the enzyme Ezh2 via VDR-mediated transcription thereby enriching H3K27me3 and repressing p16/p19 transcription. Finally, we demonstrated that treatment with 1,25(OH)2 D3 improved the osteogenic defects of human BM-MSCs caused by repeated passages by stimulating their proliferation and inhibiting their senescence via the VDR-Ezh2-p16 axis. The results of this study therefore indicate that 1,25(OH)2 D3 plays a role in preventing age-related osteoporosis by up-regulating Ezh2 via VDR-mediated transcription, increasing H3K27me3 and repressing p16 transcription, thus promoting the proliferation and osteogenesis of BM-MSCs and inhibiting their senescence, while also stimulating osteoblastic bone formation, and inhibiting osteocyte senescence, SASP, and osteoclastic bone resorption.

9.
Comput Methods Biomech Biomed Engin ; 23(1): 33-42, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31805773

RESUMO

This study numerically investigated the hemodynamics of a patient-specific coronary artery fistula (CAF) before and after the fistula closure. The results indicated that the dilated fistula result in inadequate perfusion to other healthy aortas. Disturbed blood flow, aberrant WSSs, local negative pressure gradients and sharp pressure changes are shown in both untreated and occluded fistula. Furthermore, extreme high WSS appeared at the fistula bending after the terminal closure. It was concluded that the fistula closure may effectively improve the phenomenon of stealing blood but worsen the unfavorable hemodyanmics predisposing the thrombosis formation due to its geometrical torturosity.

10.
Food Chem ; 306: 125623, 2020 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-31606633

RESUMO

In this study, apple juice was fermented using Hanseniaspora osmophila X25-5 in pure culture as well as mixed culture with Torulaspora quercuum X24-4, which was inoculated simultaneously or sequentially. H. osmophila inhibited the growth of T. quercuum, while T. quercuum had little effect on the growth of H. osmophila. The simultaneous fermentation consumed relatively more sugar and resulted in the highest ethanol content. The production of organic acids varied depending on the yeast species employed and inoculation modality. Esters and alcohols were the main volatile families produced during fermentation, while ethyl esters and terpenes contributed most to the temperate fruity aroma. Gas chromatography-olfactometry (GC-O) showed that 3-methyl-1-butanol, ethyl 2-methylbutanoate, phenylethyl alcohol, ß-phenethyl acetate, and ß-damascenone were the most potent odorants in all samples. This study suggested that simultaneous fermentation with H. osmophila and T. quercuum might represent a novel strategy for the future production of cider.


Assuntos
Acetatos/análise , Fermentação , Hanseniaspora/metabolismo , Malus/metabolismo , Odorantes/análise , Torulaspora/metabolismo , Bebidas Alcoólicas , Cromatografia Gasosa , Ésteres/análise , Frutas/química , Norisoprenoides/análise , Olfatometria , Vinho/análise
11.
J Hazard Mater ; : 121802, 2019 Nov 30.
Artigo em Inglês | MEDLINE | ID: mdl-31822350

RESUMO

The issue of patulin (PAT) contamination in apple juice has attracted widespread concern. Recently, inactivated yeast based biosorbents have shown great advantages in the removal of toxic contaminants. However, the traditional yeast adsorbents have disadvantages of a limited adsorption capacity in juice and separation difficulty. In the present work, five chemical thiol-functionalization methods were used to increase the PAT adsorption efficiency of yeast cells in apple juice. Thereinto, glutaraldehyde cross-linking increased the thiol (-SH) content of yeast cells to 1.26 mmol g-1 and improved the PAT adsorption capacity of inactivated yeast in apple juice by 150 times. The covalent bonding of -SH and PAT played an important role in the improvement of adsorption capacity. The as-prepared thiol-modification yeast (Y-SH(Gl)) was then embedded in the agar aerogel to obtain Y-SH(Gl)@Agar free of separation. PAT adsorption of Y-SH(Gl)@Agar was consistent with the Freundlich model and the pseudo-second-order kinetic model. Moreover, Y-SH(Gl)@Agar was competent for PAT removal in apple juice and manifested negligible effects on juice quality. Cytotoxicity investigation indicated its good biocompatibility and ignorable food safety risk, thereby demonstrating that Y-SH(Gl)@Agar may be a promising adsorbent material for the control of PAT contaminant in juice.

12.
Front Microbiol ; 10: 2646, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31798564

RESUMO

As natural occurring antimicrobial substances, phenolic compounds have been used to inhibit various bacteria. Stenotrophomonas maltophilia 4-1, a strain isolated from food, exhibited spoilage potential in vitro with proteolysis and lipolysis at 25°C. The present study evaluated the antibacterial properties of 13 polyphenols on S. maltophilia 4-1, and selected 6 compounds (ferulic acid, p-coumaric acid, caffeic acid, chlorogenic acid, (-)-epigallocatechin, and phloretin) for binary combination treatments. The results revealed that antibacterial activities of polyphenols were structure-dependent, and cinnamic acid showed strong inhibitory effects, with a minimum inhibitory concentration (MIC) of 0.125 mg/mL. Importantly, we did not observe any obvious synergistic effects across all binary combinations. The antibacterial mechanism of cinnamic acid was related to membrane damage, caused by the loss of cell membrane integrity and alteration of cell morphology. These findings suggest that cinnamic acid is a promising candidate for the control of spoilage bacteria in food.

13.
Neural Plast ; 2019: 9765276, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31827501

RESUMO

Auditory neuropathy spectrum disorder (ANSD), also called auditory neuropathy (AN), is a unique type of prelingual hearing impairment. Up to 10% of deaf infants and children are affected by this disease. Mutation of the OTOF gene which encodes otoferlin is the common cause of congenital nonsyndromic ANSD. To date, over 110 mutations have been identified in the OTOF gene according to the Human Gene Mutation Database (HGMD). Here, next-generation sequencing (NGS) revealed that the compound heterozygous mutations c.4748G>A/c.2523+1G>T and c.5248G>C/c.5098G>C of the OTOF gene were present in two Chinese ANSD patients. Each patient had a known pathogenic mutation (c.4748G>A or c.5098G>C) and a novel mutation (c.2523+1G>T or c.5248G>C). Comparative amino acid sequence analysis across different species revealed that the residues at these novel mutation sites are evolutionarily highly conservative. This indicated that the novel mutations were possible causes of the disorder in the patients. Our findings extend the OTOF mutation spectrum and further confirm the role of the OTOF gene in ANSD.

14.
Cell Biol Int ; 2019 Dec 24.
Artigo em Inglês | MEDLINE | ID: mdl-31872468

RESUMO

Exosomes circulating in biological fluids have the potential to be utilized as cancer biomarkers and are associated with cancer progression and metastasis. MicroRNA (miR)-663b has been found to be elevated in plasma from patients with bladder cancer (BC). However, the functional role of exosomal miR-663b in BC processes remains unknown. Here, we isolated exosomes from plasma and found that the miR-663b level was elevated in exosomes from plasma of patients with BC compared with healthy controls. Exosomal miR-663b from BC cells promoted cell proliferation and epithelial-mesenchymal transition. Moreover, exosomal miR-663b targeted Ets2-repressor factor and acted as a tumor promoter in BC cells. Taken together, our findings suggested that exosomal miR-663b is a promising potential biomarker and target for clinical detection and therapy in BC.

15.
Bioengineered ; 10(1): 659-667, 2019 12.
Artigo em Inglês | MEDLINE | ID: mdl-31755373

RESUMO

As a kind of renewable resource and natural biomass, starch has been widely used to substitute plastics in the modern industry and is regarded as one of the most promising biodegradable materials. The newly developmental rattan, straw biomass rattan (SBR) as weaving material, has been exploited as per our previous work, which possessed advantages of both natural rattan and pure plastic rattan. The main objective of the work was to improve the properties of SBR by corn starch (CS). Based on the manufacturing of the above composites, the experiments of SBR that enhanced with CS on mechanical properties, melting performance, hydroscopicity, thermogravimetric analysis, and microstructures were tested in this study. The results revealed that when the content of CS increased gradually within the range of 0, 3, 6, 9 12, and 15 wt.%, the mechanical properties and melt index of the composite both increased first and then decreased, with 6 to 12 wt.% as the optimal dosage range. In contrast, the water absorption of SBR kept increased in this range, indicating an easier biodegradable. With CS added, the microstructure of SBR was examined by scanning electron microscope and found the microscopic surfaces and sections to become smoother, and that could improve the compatibility and tenacity between the materials. As a result, CS in moderation can be used as a supplement to enhance SBR, and improve their characteristics which will enhance the mechanical properties of the composites for future perspectives.

16.
J Control Release ; 317: 43-56, 2019 Nov 20.
Artigo em Inglês | MEDLINE | ID: mdl-31758970

RESUMO

Myeloid-derived suppressor cells(MDSCs)are one of the most important immunosuppressive cells in tumor microenvironment, which also promote the development and progression of tumor cells. Nevertheless, due to the different distribution features of MDSCs and tumor cells, selective elimination of MDSCs and tumor cells in tumor microenvironment remain a great challenge. Here we have designed a dual-pH-sensitivity conjugated micelle system (PAH/RGX-104@PDM/PTX) that could deliver liver-X nuclear receptor (LXR) agonist RGX-104 and paclitaxel (PTX) to the perivascular region and tumor cells, respectively. Upon arrival at the acidic tumor microenvironment, the PAH/RGX-104@PDM/PTX undergo structure disintegration and capacitate coinstantaneous release of RGX-104 in the perivascular regions, leaving the intact PTX containing micelles PDM/PTX for tumor deep penetration. The released RGX-104 can be preferentially taken up by leukocytes, endothelial cells and macrophages which are nicely enriched in perivascular regions to active the LXR, and further reduces immunosuppressive MDSC levels. The remained small micelles carrying PTX enable deep tumor penetration as well as rapid specific drug release in the endosomal/lysosomal to kill tumor cells. PAH/RGX-104@PDM/PTX exhibits superior tumor accumulation as well as tumor penetration, and suppresses 74.88% in vivo tumor growth. More importantly, PAH/RGX-104@PDM/PTX has significantly alleviated tumor immunosuppression by eliminating MDSCs and increasing cytotoxic T lymphocytes infiltration. Our studies suggest that the dual-pH-sensitive codelivery nanocarrier not only cause apoptosis of cancer cells but also regulate the tumor immune environment to ultimately enhance the antitumor effect of CTLs through MDSCs depletion.

17.
Ann Transl Med ; 7(18): 473, 2019 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-31700909

RESUMO

Background: The transcellular transport of muramyl dipeptide (MDP) mediated by peptide transporter (PepT1) involves the translocation into intestinal epithelial cell (IEC) stage and the transport out of IEC stage. However, its mechanism has not been fully understood. This study aimed to investigate the pathways and mechanisms of MDP transcellular transport in enterogenous infection. Methods: Firstly, experimental rats were randomly divided into three groups: sham-operation (sham group), MDP perfusion (MDP group), and PepT1 competitive inhibition (MDP + Gly-Gly group). Then, the overall survival (OS) and intestinal weight were measured in MDP and MDP + Gly-Gly group. HE staining was performed to observe the pathological changes of the small intestine. The levels of IL-6, IL-1b, IL-8, IL-10, TNF-α, and nitric oxide (NO) in rat serum and small intestine were determined by ELISA. To further verify the pathways and mechanisms of MDP transcellular transport from IEC in intestinal inflammatory damage, the NFκB inhibitor, PDTC, was used to treated lamina propria macrophages in small intestinal mucosa in sham, MDP, and MDP + Gly-Gly groups. Finally, the expression of CD80/86 and the antigen presentation of dendritic cells (DCs) were measured by flow cytometry. Results: MDP infusion was able to induce death, weight loss, and intestinal pathological injury in rats. Competitive binding of Gly-Gly to PepT1 effectively inhibited these effects induced by MDP. As well, competitive of PepT1 by Gly-Gly inhibited inflammation-related cytokines induced by MDP in rat serum and small intestine. Furthermore, we also found that MDP transported by PepT1 contributes to activation of macrophages and antigen presentation of DCs. Conclusions: PepT1-NFκB signal is pivotal for activation of intestinal inflammatory response and MDP transcellular transport.

18.
Medicine (Baltimore) ; 98(44): e17463, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31689750

RESUMO

RATIONALE: Malignant peripheral nerve sheath tumor (MPNST) is a very rare sarcoma of the heart, and few cases have been reported. Herein, we retrospectively reviewed clinical manifestations, imaging features and management of our patient and other reported cases. PATIENT CONCERNS: A 32-year-old woman was referred to the emergency department of our institution with expiratory dyspnea, edema of face for a month. DIAGNOSIS: The patient was initially diagnosed with asthma at a local hospital based on a history of fatigue, cough and expiratory dyspnea, as well as negative electroencephalogram (ECG) and chest radiography. Based on computed tomography (CT) and cardiac magnetic resonance imaging (CMRI) in our hospital, she was found to have a malignant tumor involving right atrium. The tumor was diagnosed as MPNST according to histopathological results. INTERVENTIONS: The tumor was deemed unresectable during the surgery. Then, the patient was referred for chemotherapy and radiotherapy. OUTCOMES: The patient deteriorated and died 4 months later. LESSONS: Cardiac MPNST is very uncommon with nonspecific clinical and imaging characteristics according to limited cased reported. CMR, due to the high tissue resolution and multiple sequence imaging advantages, is useful for the detection, location and evaluation whether there is involvement of adjacent structures, and may help better clinical decision-making.


Assuntos
Neoplasias Cardíacas/diagnóstico , Neurofibrossarcoma/diagnóstico , Adulto , Feminino , Neoplasias Cardíacas/diagnóstico por imagem , Neoplasias Cardíacas/terapia , Humanos , Imagem por Ressonância Magnética , Neurofibrossarcoma/diagnóstico por imagem , Neurofibrossarcoma/terapia , Tomografia Computadorizada por Raios X
19.
J Phys Chem B ; 123(47): 10124-10130, 2019 Nov 27.
Artigo em Inglês | MEDLINE | ID: mdl-31692348

RESUMO

Previous work utilizing crystal polymorphs has established the importance of the molecular packing environment for modulating solid-gas reactivity. Here, we show, for the first time, that the chemical stability of an amorphous material in contact with a reactive gas can be significantly improved by controlling glass packing. We utilize the reaction of indomethacin with ammonia as this system has been well-characterized for crystalline polymorphs. For these experiments, physical vapor deposition (PVD) is used to prepare glasses of indomethacin with a range of densities and thermal stabilities. The indomethacin-ammonia reactivity is assessed through the increase in mass of glassy thin films exposed to ammonia gas, as characterized by a quartz crystal microbalance. Indomethacin glasses vapor-deposited at substrate temperatures below the glass transition temperature (Tg) show unprecedented decrease in reaction rates relative to the liquid-cooled glass, by as much as 1 order of magnitude, with the densest glasses having the slowest reactions. The diminished solubility of ammonia in dense PVD glasses is found to be a major factor in their remarkable chemical stability. As chemically stable amorphous solids are in demand for applications including pharmaceuticals and organic electronics, this work provides a strategy to improve performance of these materials.

20.
Adv Sci (Weinh) ; 6(21): 1900958, 2019 Nov 06.
Artigo em Inglês | MEDLINE | ID: mdl-31728278

RESUMO

The multistep redox reactions of lithium-sulfur batteries involve undesirably complex transformation between sulfur and Li2S, and it is tough to spontaneously fragmentate polysulfides into shorter chains Li2S originating from the sluggish redox kinetics of soluble polysulfide intermediates, causing serious polarization and consumption of sulfur. In this work, 3,4,9,10-perylenetetracarboxylic diimide (PTCDI)/G is employed as sulfur host to accelerate the conversion process between polysulfides and sulfur, which could facilitate the process of both charging and discharging. Moreover, PTCDI has strong adsorption capacity with polysulfides to restrain shuttle effect, resulting in promotional kinetics and cycle stability. A high initial capacity of 1496 mAh g-1 at 0.05 C and slight capacity decay of 0.009% per cycle at 5 C over 1500 cycles can be achieved. Moreover, the cathode could also achieve a high energy efficiency over 85% at 0.5 C. This research extends the knowledge into an original domain for designing high-performance host materials.

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