Metal-organic frameworks (MOFs) based on high-connected nets are generally very attractive due to their combined robustness and porosity. Here, we describe the synthesis of BCN-348, a new ...high-connected Zr-MOF built from an 8-connected (8-c) cubic Zr-oxocluster and an 8-c organic linker. BCN-348 contains a minimal edge-transitive 3,4,8-c eps net, and combines mesoporosity with thermal and hydrolytic stability. Encouraging results from preliminary studies on its use as a catalyst for hydrolysis of a nerve-agent simulant suggest its potential as an agent for detoxification of chemical weapons and other pernicious compounds.
We present BCN-348, a new high-connected MOF built from an 8-c cubic Zr-oxocluster and an 8-c organic linker. BCN-348 shows a 3,4,8-c eps net, mesoporosity, hydrolytic stability, and acts as a catalyst for hydrolysis of a nerve-agent simulant.
Space cooling and heating, ventilation, and air conditioning (HVAC) accounts for roughly 10% of global electricity use and are responsible for ca. 1.13 gigatonnes of CO2 emissions annually. ...Adsorbent‐based HVAC technologies have long been touted as an energy‐efficient alternative to traditional refrigeration systems. However, thus far, no suitable adsorbents have been developed which overcome the drawbacks associated with traditional sorbent materials such as silica gels and zeolites. Metal–organic frameworks (MOFs) offer order‐of‐magnitude improvements in water adsorption and regeneration energy requirements. However, the deployment of MOFs in HVAC applications has been hampered by issues related to MOF powder processing. Herein, three high‐density, shaped, monolithic MOFs (UiO‐66, UiO‐66‐NH2, and Zr‐fumarate) with exceptional volumetric gas/vapor uptake are developed—solving previous issues in MOF‐HVAC deployment. The monolithic structures across the mesoporous range are visualized using small‐angle X‐ray scattering and lattice‐gas models, giving accurate predictions of adsorption characteristics of the monolithic materials. It is also demonstrated that a fragile MOF such as Zr‐fumarate can be synthesized in monolithic form with a bulk density of 0.76 gcm−3 without losing any adsorption performance, having a coefficient of performance (COP) of 0.71 with a low regeneration temperature (≤ 100 °C).
Monolithic zirconium‐based metal‐organic frameworks (UiO‐66, UiO‐66‐NH2 and Zr‐fumarate) with high density and exceptional water sorption capacity are developed to replace traditional refrigeration systems with energy‐efficient alternatives. The adsorption characteristics of monolithic materials have been predicted using small‐angle X‐ray scattering and lattice‐gas models. Unlike traditional MOFs, these monolithic MOFs have overcome processing issues, making them suitable for real‐world applications.
Here, we report the synthesis of BCN-93, a meltable, functionalized, and permanently porous metal–organic polyhedron (MOP) and its subsequent transformation into amorphous or crystalline, shaped, ...self-standing, transparent porous films via melting and subsequent cooling. The synthesis entails the outer functionalization of a MOP with meltable polymer chains: in our model case, we functionalized a Rh(II)-based cuboctahedral MOP with poly(ethylene glycol). Finally, we demonstrate that once melted, BCN-93 can serve as a porous matrix into which other materials or molecules can be dispersed to form mixed-matrix composites. To illustrate this, we combined BCN-93 with one of various additives (either two MOF crystals, a porous cage, or a linear polymer) to generate a series of mixed-matrix films, each of which exhibited greater CO2 uptake relative to the parent film.
Purpose
HSP90 (Heat shock protein 90kD) has been validated as a therapeutic target in Castrate Resistant Prostate Cancer. Unfortunately, HSP90 inhibitors suffer from dose-limiting toxicities that ...hinder their clinical applications. Previously developed polymeric delivery systems for HSP90 inhibitors had either low drug content or low biological activity suggesting the need for better delivery system for HSP90 inhibitors.
Methods
We developed a simplified synthetic strategy to prepare polyethylene glycol based water-soluble polymeric system for model HSP90 inhibitor geldanamycin (GDM). We then investigated the effect of cathepsin B degradable linker and drug content in polymeric conjugates on their growth inhibitory property using DU145 (androgen independent) and LNCaP (androgen dependent) cell lines.
Results
Water-soluble polymeric conjugates were synthesized with GDM content ranging from 9 to 30% wt/wt. We demonstrated the importance of cathepsin B degradable linker from the context of drug content and different prostate cancer cell lines. The most active conjugate against DU145 cells exhibited IC
50
value of 2.9 μM. This was similar to the IC
50
(2.1 μM) of small molecular drug aminohexane geldanamycin.
Conclusion
Water-soluble polymeric conjugate with high drug content was synthesized that exhibited
in-vitro
growth inhibitory activity similar to small molecular weight HSP90 inhibitor.
Graphical Abstract
Water soluble degradable polymeric conjugate for the delivery of Geldanamycin
Porosity and surface area analysis play a prominent role in modern materials science. At the heart of this sits the Brunauer–Emmett–Teller (BET) theory, which has been a remarkably successful ...contribution to the field of materials science. The BET method was developed in the 1930s for open surfaces but is now the most widely used metric for the estimation of surface areas of micro‐ and mesoporous materials. Despite its widespread use, the calculation of BET surface areas causes a spread in reported areas, resulting in reproducibility problems in both academia and industry. To prove this, for this analysis, 18 already‐measured raw adsorption isotherms were provided to sixty‐one labs, who were asked to calculate the corresponding BET areas. This round‐robin exercise resulted in a wide range of values. Here, the reproducibility of BET area determination from identical isotherms is demonstrated to be a largely ignored issue, raising critical concerns over the reliability of reported BET areas. To solve this major issue, a new computational approach to accurately and systematically determine the BET area of nanoporous materials is developed. The software, called “BET surface identification” (BETSI), expands on the well‐known Rouquerol criteria and makes an unambiguous BET area assignment possible.
A round‐robin study involving 61 labs is performed, and it is shown that the determination of Brunauer–Emmett–Teller (BET) areas from identical isotherms is a largely ignored issue. To solve this, a new computational approach called “BET surface identification” (BETSI) is presented, which expands on the Rouquerol criteria, and which makes an unambiguous BET area calculation possible.
It is now clear that growing flat graphene nanostructures from the gas phase on planar substrates is possible. One of the keys to success —particularly in producing a very large specific surface in a ...reduced space— is the use of 3D carbon nanostructures (i.e., vertical graphene nanowalls, VGNWs) over a planar substrate as a growth template for the deposition of electrochemically active materials (as, for example, transition metal oxides (TMO)). Vertical graphene nanowalls, also known as petal-like, vertical graphene flakes or vertical graphene, can achieve a very large specific surface area of 1100 m2/g, which is comparable to or greater than that of carbon nanotubes —the reference material for its use in high-performance supercapacitors or in other energy-related applications requiring a large active surface area. Vertical graphene nanowalls also exhibit high vertical and in-plane electrical conductivity when grown on metal electrodes, which benefits their use in electrochemical applications. Here, we focus on the growth of VGNWs on flexible stainless-steel substrates (SS310), in principle suitable for applications to electrodes of electrochemical systems (batteries, supercapacitors, catalysts), by inductively coupled plasma chemical vapour deposition (ICP-CVD), from methane as a carbon precursor, in a wide range of temperatures (575 to 900 °C). We will discuss the effect of growth temperature on morphological and structural characteristics of VGNWs based on the results of Raman spectroscopy and field emission scanning electron microscopy (FE-SEM) analysis. Because the nanostructures of graphene nanowalls reported to date are, for the most part, based on multi-layered graphene, here we seek to highlight the effect of temperature on the number of atomic layers of VGNW. In the 700–750 °C range, and under the plasma conditions explored, vertical graphene nanowalls are bilayer, which is foreseen to directly affect the magnitude of the VGNW specific surface.
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•Growth of graphene nanowalls by ICP-CVD on stainless steel in the range 675–775 °C.•Monatomic two-layer graphene nanowalls grown at 750 °C by ICP-CVD.•Defects mainly at the edges and not at the faces of the graphene nanowalls.•Easy anchorage of MeOx particles on edges and high chemical stability of the system.
We aimed to develop and validate a prediction model, based on clinical history and examination findings on initial diagnosis of coronavirus disease 2019 (COVID-19), to identify patients at risk of ...critical outcomes.
We used data from the SEMI-COVID-19 Registry, a cohort of consecutive patients hospitalized for COVID-19 from 132 centres in Spain (23rd March to 21st May 2020). For the development cohort, tertiary referral hospitals were selected, while the validation cohort included smaller hospitals. The primary outcome was a composite of in-hospital death, mechanical ventilation, or admission to intensive care unit. Clinical signs and symptoms, demographics, and medical history ascertained at presentation were screened using least absolute shrinkage and selection operator, and logistic regression was used to construct the predictive model.
There were 10 433 patients, 7850 in the development cohort (primary outcome 25.1%, 1967/7850) and 2583 in the validation cohort (outcome 27.0%, 698/2583). The PRIORITY model included: age, dependency, cardiovascular disease, chronic kidney disease, dyspnoea, tachypnoea, confusion, systolic blood pressure, and SpO2 ≤93% or oxygen requirement. The model showed high discrimination for critical illness in both the development (C-statistic 0.823; 95% confidence interval (CI) 0.813, 0.834) and validation (C-statistic 0.794; 95%CI 0.775, 0.813) cohorts. A freely available web-based calculator was developed based on this model (https://www.evidencio.com/models/show/2344).
The PRIORITY model, based on easily obtained clinical information, had good discrimination and generalizability for identifying COVID-19 patients at risk of critical outcomes.
Abstract The Canary Islands inhabitants, a recently admixed population with significant North African genetic influence, has the highest incidence of childhood-onset type 1 diabetes (T1D) in Spain ...and one of the highest in Europe. HLA accounts for half of the genetic risk of T1D. Aims To characterize the classical HLA-DRB1 and HLA-DQB1 alleles in children from Gran Canaria with and without T1D. Methods We analyzed classic HLA-DRB1 and HLA-DQB1 alleles in childhood-onset T1D patients ( n = 309) and control children without T1D ( n = 222) from the island of Gran Canaria. We also analyzed the presence or absence of aspartic acid at position 57 in the HLA-DQB1 gene and arginine at position 52 in the HLA-DQA1 gene. Genotyping of classical HLA-DQB1 and HLA-DRB1 alleles was performed at two-digit resolution using Luminex technology. The chi-square test (or Fisher's exact test) and odds ratio (OR) were computed to assess differences in allele and genotype frequencies between patients and controls. Logistic regression analysis was also used. Results Mean age at diagnosis of T1D was 7.4 ± 3.6 years (46% female). Mean age of the controls was 7.6 ± 1.1 years (55% female). DRB1*03 (OR = 4.2; p = 2.13 –13 ), DRB1*04 (OR = 6.6; p ≤ 2.00 –16 ), DRB1* 07 (OR = 0.37; p = 9.73 –06 ) , DRB1*11 (OR = 0.17; p = 6.72 –09 ) , DRB1*12, DRB1 * 13 (OR = 0.38; p = 1.21 –05 ) , DRB1*14 (OR = 0.0; p = 0.0024), DRB1 * 15 (OR = 0.13; p = 7.78 –07 ) and DRB1 * 16 (OR = 0.21; p = 0.00 3 ) exhibited significant differences in frequency between groups . Among the DQB1* alleles , DQB1*02 (OR: 2.3; p = 5.13 –06 ), DQB1*03 (OR = 1.7; p = 1.89 –03 ), DQB1*05 (OR = 0.64; p = 0.027) and DQB1*06 (OR = 0.19; p = 6.25 –14 ) exhibited significant differences. A total of 58% of the studied HLA-DQB1 genes in our control population lacked aspartic acid at position 57. Conclusions In this population, the overall distributions of the HLA-DRB1 and HLA-DQB1 alleles are similar to those in other European populations. However, the frequency of the non-Asp-57 HLA-DQB1 molecules is greater than that in other populations with a lower incidence of T1D. Based on genetic, historical and epidemiological data, we propose that a common genetic background might help explain the elevated pediatric T1D incidence in the Canary Islands, North-Africa and middle eastern countries.
This longitudinal study addressed whether mindfulness practice prevents psychological and behavioral symptoms, especially mood disorders, in Alzheimer's disease (AD).
To assess the incidence of ...depression in the course of AD and to determine which non-pharmacological treatment (NPT) is most effective in preventing psychopathological symptoms.
We conducted a longitudinal, non-inferiority and equivalence randomized clinical trial, repeated-measures design, with a control group and three experimental treatments: mindfulness, cognitive stimulation, and relaxation. Each experimental group performed three weekly sessions for two years. The pharmacological treatment of all participants was donepezil (10 mg). Participants were patients with probable AD without diagnosed depression from the public neurology services of the Canary Health Service, Spain. Psychological evaluation was performed using the Geriatric Depression Scale (GDS), Hamilton Depression Rating Scale (HDRS), and Neuropsychiatric Inventory (NPI-Q). The statistical analysis included only patients who attended at least 75% of the sessions. A nonparametric, repeated-measures analysis was performed with Kruskal-Wallis H test and between-group differences with Mann-Whitney U test with Bonferroni correction (p < 0.008). Effect size was calculated with partial eta-squared.
The results showed significant differences with large effect sizes (η2p>0.14) between mindfulness and the rest of the experimental groups as well as the control in the GDS, HDRS, and NPI-Q scales.
Compared to the other experimental groups, only mindfulness prevented the onset of depression and other psychopathologies in early-stage AD. Based on its effectiveness in maintaining cognitive functions and preventing psychopathology, we recommend mindfulness as the first-choice NPT for mild to moderate AD.
The Persea mite, Oligonychus perseae Tuttle, Baker & Abbatiello (Acari: Tetranychidae), is an economically important foliar pest of avocados in Spain. The effects of this mite on the foliar damage, ...production losses and economic impact were assessed in two avocado, cv. Hass, orchards located in the main growing areas of Spain (Northern Tenerife and Málaga) for 3 and 5 consecutive years, respectively. The economic injury level (EIL) for the optimization of the use of acaricides to control this mite was also established, considering three spraying strategies: (i) mite-free treatment (<50 mites per leaf), (ii) conventional treatment (50–150 mites per leaf), and (iii) control treatment (the absence of spraying). Persea mite populations were sampled fortnightly and foliar damage was estimated. At the end of each season, fruits were harvested, weighed and production losses were quantified. The cumulate mite-days (CMDs) had a significant effect on the percentage of leaf area damaged (PLAD) and yield reduction. High numbers of the Persea mite caused extensive damage to leaves, so a loss in tree yield was evident. However, for the middle population level, there was no evidence of yield losses. The quantitative EIL was estimated at a PLAD of 17%, equivalent to a CMDs of 178 mites per leaf, which is the amount of damage that should not be exceeded. In Northern Tenerife, with a mild climate, the Persea mite can reach significant populations that are maintained throughout the months. In avocado orchards in Málaga, the summer is hotter and drier, so the presence of the mite exists for a shorter duration in the seasons, with less damage to the leaves. In Tenerife, yield loss can be compensated by chemical treatments that permit pest control.
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