Cytochrome P450 gene CYP6BQ8 mediates terpinen-4-ol susceptibility in the red flour beetle, Tribolium castaneum (Herbst) (Coleoptera: Tenebrionidae).

Cytochrome P450 proteins (CYPs) in insects can encode various detoxification enzymes and catabolize heterologous substances, conferring tolerance to insecticides. This study describes the identification of a P450 gene (CYP6BQ8) from Tribolium castaneum (Herbst) and investigation of its spatiotemporal expression profile and potential role in the detoxification of terpinen-4-ol, a component of plant essential oils. The developmental expression profile showed that TcCYP6BQ8 expression was relatively higher in early- and late-larval stages of T. castaneum compared with other developmental stages. Tissue expression profiles showed that TcCYP6BQ8 was mainly expressed in the head and integument of both larvae and adults. The expression profiling of TcCYP6BQ8 in developmental stages and tissues is closely related to the detoxification of heterologous substances. TcCYP6BQ8 expression was significantly induced after exposure to terpinen-4-ol, and RNA interference against TcCYP6BQ8 increased terpinen-4-ol-induced larval mortality from 47.78 to 66.67%. This indicates that TcCYP6BQ8 may be involved in T. castaneum's metabolism of terpinen-4-ol. Correlation investigation between the CYP6BQ8 gene and terpinen-4-ol resistance in T. castaneum revealed that the TcCYP6BQ8 gene was one of the factors behind T. castaneum's resistance to terpinen-4-ol. This discovery may provide a new theoretical foundation for future regulation of T. castaneum.

Enabling Scalable Polymer Electrolyte with Synergetic Ion Conductive Channels via a Two Stage Rheology Tuning UV Polymerization Strategy.

Lithium metal batteries with polyethylene oxide (PEO) electrolytes are considered as one of the ideal candidates for next generation power sources. However, the low ambient operation capability and conventional solvent-based fabrication process of PEO limit their large-scale application. In this work, a comb-like quasi-solid polymer electrolyte (QPE) reinforced with polyethylene glycol terephthalate nonwoven is fabricated. Combining the density functional theory calculation analysis and polymer structure design, optimized and synergized ion conductive channels are established by copolymerization of tetrahydrofurfuryl acrylate and introduction of plasticizer tetramethyl urea. Additionally, a unique two-stage solventless UV polymerization strategy is utilized for rheology tuning and electrolyte fabrication. Compared with the conventional one-step UV process, this strategy is ideally suited for the roll-to-roll continuous coating fabrication process with environmental friendliness. The fabricated QPE exhibits high ionic conductivity of 0.40 mS cm-1 and Li+ transference number (t = 0.77) at room temperature. LiFePO4 //Li batteries are assembled to evaluate battery performance, which deliver excellent discharge capacity (144.9 mAh g-1 at 0.5 C) and cycling stability (with the retention rate 94.5% at 0.5 C after 200 cycles) at room temperature. The results demonstrate that it has high potential for solid-state lithium metal batteries.

Allosteric inhibition of SHP2 phosphatase inhibits cancers driven by receptor tyrosine kinases.

The non-receptor protein tyrosine phosphatase SHP2, encoded by PTPN11, has an important role in signal transduction downstream of growth factor receptor signalling and was the first reported oncogenic tyrosine phosphatase. Activating mutations of SHP2 have been associated with developmental pathologies such as Noonan syndrome and are found in multiple cancer types, including leukaemia, lung and breast cancer and neuroblastoma. SHP2 is ubiquitously expressed and regulates cell survival and proliferation primarily through activation of the RAS­ERK signalling pathway. It is also a key mediator of the programmed cell death 1 (PD-1) and B- and T-lymphocyte attenuator (BTLA) immune checkpoint pathways. Reduction of SHP2 activity suppresses tumour cell growth and is a potential target of cancer therapy. Here we report the discovery of a highly potent (IC50 = 0.071 µM), selective and orally bioavailable small-molecule SHP2 inhibitor, SHP099, that stabilizes SHP2 in an auto-inhibited conformation. SHP099 concurrently binds to the interface of the N-terminal SH2, C-terminal SH2, and protein tyrosine phosphatase domains, thus inhibiting SHP2 activity through an allosteric mechanism. SHP099 suppresses RAS­ERK signalling to inhibit the proliferation of receptor-tyrosine-kinase-driven human cancer cells in vitro and is efficacious in mouse tumour xenograft models. Together, these data demonstrate that pharmacological inhibition of SHP2 is a valid therapeutic approach for the treatment of cancers.

The Fabrication of High-Hardness and Transparent PMMA-Based Composites by an Interface Engineering Strategy.

The high-hardness and transparent PMMA-based composites play a significant role in modern optical devices. However, a well-known paradox is that conventional PMMA-based composites with high loadings of nanoparticles usually possess high surface hardness at the cost of poor transparency and toughness due to the aggregation of nanoparticles. In this work, ideal optical materials (SiO2/PMMA composites) with high transparency and high surface hardness are successfully fabricated through the introduction of the flow modifier Si-DPF by conventional melt blending. Si-DPF with low surface energy and high transparency, which is located at the SiO2/PMMA interface, and nano-SiO2 particles are homogeneously dispersed in the PMMA matrix. As an example, the sample SiO2/PMMA/Si-DPF (30/65/5) shows outstanding transparency (>87.2% transmittance), high surface hardness (462.2 MPa), and notched impact strength (1.18 kJ/m2). Moreover, SiO2/PMMA/Si-DPF (30/65/5) also presents a low torque value of composite melt (21.7 N⋅m). This work paves a new possibility for the industrial preparation of polymer-based composites with excellent transparency, surface hardness, processability, and toughness.

Hollow Lindqvist-like-Shaped {V6} Cluster-Based Metal-Organic Framework for the Highly Efficient Detoxification of Mustard Gas Simulant.

A polyoxovanadate-based nickel-organic framework, [Ni(bib)2]{V2O6}({V6}-MOF, bib = 1,4-bis(1H-imidazoly-1-yl)benzene), was facilely prepared under gentle hydrothermal conditions and structurally characterized. Single-crystal X-ray diffraction analysis indicates that the {V6} cluster in the {V6}-MOF is constructed of two VO5 tetragonal pyramids and four VO4 tetrahedrons via the apex sharing of O atoms, presenting a hollow Linqvist-like structure, which is different from these reported hexanuclear vanadium clusters. The {V6}-MOF not only expands the structure of polyoxovanadates (POVs) but also catalyzes the rapid detoxification of mustard gas simulant (2-chloroethyl ethyl sulfide, CEES) at 25 °C. The catalytic results were determined by means of GC, GC-MS, and 1H NMR. Using {V6}-MOF as a heterogeneous catalyst, CEES underwent catalyzed oxidation to only nontoxic product 2-chloroethyl ethyl sulfoxide (CEESO) within 40 min, and the conversion and selectivity were almost 100%. In addition, {V6}-MOF exhibits high sustainability, and no obvious reductions in conversion and selectivity are observed after five runs.

Factors associated with social isolation in community-dwelling older adults: a cross-sectional study.

PURPOSE: Social isolation in older adults is a major public health problem and associated with increased morbidity and mortality. There are limited data on the association between social isolation and physical function including gait speed. Hence, this study is to determine the prevalence of social isolation and its association with gait speed, frailty, cognition, depression and comorbidities amongst community-dwelling older adults. METHODS: Social isolation, depression, frailty and perceived general health were assessed using 6-item Lubben Social Network Scale (LSNS-6), Geriatric Depression Scale (GDS), FRAIL scale and EuroQol EQ-5D-5L questionnaire which includes EQ Visual Analogue Scale (EQ-VAS), respectively. Cognition was assessed using the Chinese Mini Mental State Examination (cMMSE), while physical performance test included gait speed and short physical performance battery test. Binary logistic regression was performed to determine the influence of socio-demographic, medical, functional and cognitive variables on social isolation. RESULTS: Out of 202 participants, 27.7% were robust, 66.8% of participants were pre-frail, and 5.4% of participants were frail. Almost half (45.5%, n = 92) of the participants were found to be at risk of social isolation. A poor social network was negatively associated with mean gait speed (OR = 0.674, CI 0.464-0.979, p = 0.039), EQ-VAS (OR = 0.561, CI 0.390-0.806, p < 0.01) and cMMSE (OR = 0.630, 95% CI 0.413-0.960, p = 0.032). CONCLUSION: Almost half of older adults in the community are at risk of social isolation with a very significant association with gait speed, cMMSE and EQ-VAS scores.

Identification of quality gaps in healthcare services using the SERVQUAL instrument and importance-performance analysis in medical intensive care: a prospective study at a medical center in Taiwan.

BACKGROUND: Assessing patients' expectations and perceptions of health service delivery is challenging. To understand the service quality in intensive care units (ICUs), we investigated the expected and perceived service quality of ICU care. METHODS: We conducted this study at an ICU of a university-affiliated medical center in Taiwan from April to September 2019. Admitted patients or their family members responded to a questionnaire survey adopted from the SERVQUAL instrument consisting of 22 items in five dimensions. The questionnaire was provided on ICU admission for expectation and before ICU discharge for perception. We analyzed the quality gaps between the surveys and applied important-performance analysis (IPA). RESULTS: A total of 117 patients were included (62.4% males, average age: 65.9 years, average length of stay: 10.1 days, and 76.9% survival to ICU discharge). The overall weighted mean scores for the surveys were similar (4.57 ± 0.81 and 4.58 ± 0.52, respectively). The 'tangibles' dimension had a higher perception than expectation (3.99 ± 0.55 and 4.31 ± 0.63 for expectation and perception, respectively, p < 0.001). IPA showed that most of the items in 'reliability,' 'responsiveness' and 'assurance' were located in the quadrant of high expectation and high perception, whereas most of the items in 'tangibles' and 'empathy' were located in the quadrant of low expectation and low perception. One item (item 1 for 'tangibles') was found in the quadrant of high expectation and low perception. CONCLUSIONS: The SERVQUAL approach and IPA might provide useful information regarding the feedback by patients and their families for ICU service quality. In most aspects, the performance of the ICU satisfactorily matched the needs perceived by the patients and their families.

Aminated Graphene Oxide Impregnated with Photocatalytic Polyoxometalate for Efficient Adsorption of Dye Pollutants and Its Facile and Complete Photoregeneration.

Contamination of industrial sewage by organic dye pollutants is one of the most common challenges to the daily life. De-contamination can be achieved by adsorption and photodegradation of the pollutants. However, the former technique is generally limited by the poor loading capacity of the adsorbent and/or the difficulty in its regeneration for reuse, while the latter often suffers from sluggish reaction kinetics and thus requires long reaction time and powerful light source to be successful. Herein, a solution to these challenges by creating nanocomposites featuring porous diamine-functionalized graphene oxide (FGO) impregnated with photocatalytically active polyoxometalates (POMs) is presented. Cross-linking of GO via diamination not only generates porous structures with positively charged interior that attracts and stabilizes the anionic POM guests, but also modulates the GO bandgap. The introduction of POMs improves loading capacity of FGO for cationic dyes and promotes effective separation of electron-hole pair by trapping and transferring photogenerated electron. Thus, the two components act in synergy to result in much improved adsorption of certain common organic dyes as well as enhanced oxidative degradation by both the GO host and the POMs that lead to complete regeneration of the adsorbents without compromising their performance in multiple rounds of reuse.

Extreme diversity and multiple SCCmec elements in coagulase-negative Staphylococcus found in the Clinic and Community in Beijing, China.

BACKGROUND: Coagulase-negative staphylococci (CoNS) are recognized as a large reservoir of staphylococcal cassette chromosome mec (SCCmec) harboured by Staphylococcus aureus. However, data of SCCmec in CoNS are relatively absent particularly in China. METHODS: Seventy-eight CoNS clinical and 47 community isolates were collected in Beijing. PCR was performed to classify SCCmec types. Under oxacillin treatment, quantitative real-time reverse transcription PCR (qRT-PCR) was performed to compare mecA mRNA levels and mRNA half-life between isolates with single SCCmec element and those with multiple one. Their growth curves were analysed. Their bacterial cell wall integrity was also compared by performing a Gram stain. All ccr complex segments were sequenced and obtained ccr segments were analysed by phylogenetic analyses. RESULTS: All 78 clinical isolates had mecA segments compared with 38% in community isolates (total 47). Only 29% clinical isolates and 33% community isolates (among mecA positive isolates) harboured a single previously identified SCCmec type; notably, 17% clinical isolates and 28% community isolates had multiple SCCmec types. Further studies indicated that isolates with multiple SCCmec elements had more stable mecA mRNA expression compared with isolates with single SCCmec elements. CoNS with multiple SCCmec elements demonstrated superior cell wall integrity. Interestingly, phylogenetic analyses of obtained 70 ccr segments indicated that horizontal gene transfer of the ccr complex might exist among various species of clinical CoNS, community CoNS and S. aureus. CONCLUSIONS: CoNS recovered from patients carried extremely diverse but distinctive SCCmec elements compared with isolates from the community. More attention should be given to CoNS with multiple SCCmec not only because they had superior cell wall integrity, but also because CoNS and S. aureus might acquire multiple SCCmec through the ccr complex.

[Effect of atopy on serum glucocorticoid receptor levels in children with bronchiolitis].

OBJECTIVE: To investigate the effect of atopy on the expression of glucocorticoid receptors in children with bronchiolitis. METHODS: ELISA was used to measure the changes in the serum levels of glucocorticoid receptor α (GRα) and glucocorticoid receptor ß (GRß) in the bronchiolitis group (77 children, including 34 children with atopy) and pneumonia group (68 children). Thirty-eight children who were prepared to undergo surgeries for non-infectious diseases and had no atopy or family history of allergic diseases were enrolled as the control group. RESULTS: The bronchiolitis group and the pneumonia group had significant increases in the serum levels of GRα and GRß compared with the control group (P<0.01), and the bronchiolitis group had significant increases in these levels compared with the pneumonia group (P<0.01). Compared with the control group and the pneumonia group, the bronchiolitis group had a significant increase in the GRα/GRß ratio (P<0.01). Compared with the control group, the children with or without atopy in the bronchiolitis group had significant increases in the serum levels of GRα and GRß (P<0.01). The non-atopic children in the bronchiolitis group had a significant increase in the serum level of GRß compared with the atopic children (P<0.01). The atopic children in the bronchiolitis group had a significant increase in the GRα/GRß ratio compared with the control group and non-atopic children in the bronchiolitis group (P<0.01). CONCLUSIONS: Children with bronchiolitis have increased serum levels of GRα and GRß. The children with atopy have an increased GRα/GRß ratio, suggesting that the atopic children with bronchiolitis are highly sensitive to glucocorticoids.

Outdoor temperature, blood pressure, and cardiovascular disease mortality among 23 000 individuals with diagnosed cardiovascular diseases from China.

INTRODUCTION: Blood pressure is a major cause of cardiovascular disease (CVD) and both may increase as outdoor temperatures fall. However, there are still limited data about seasonal variation in blood pressure and CVD mortality among patients with prior-CVD. METHODS: We analysed data on 23 000 individuals with prior-CVD who were recruited from 10 diverse regions into the China Kadoorie Biobank during 2004-8. After 7 years of follow-up, 1484 CVD deaths were recorded. Baseline survey data were used to assess seasonal variation in systolic blood pressure (SBP) and its association with outdoor temperature. Cox regression was used to examine the association of usual SBP with subsequent CVD mortality, and seasonal variation in CVD mortality was assessed by Poisson regression. All analyses were adjusted for age, sex, and region. RESULTS: Mean SBP was significantly higher in winter than in summer (145 vs. 136 mmHg, P < 0.001), especially among those without central heating. Above 5°C, each 10°C lower outdoor temperature was associated with 6.2 mmHg higher SBP. Systolic blood pressure predicted subsequent CVD mortality, with each 10 mmHg higher usual SBP associated with 21% (95% confidence interval: 16-27%) increased risk. Cardiovascular disease mortality varied by season, with 41% (21-63%) higher risk in winter compared with summer. CONCLUSION: Among adult Chinese with prior-CVD, there is both increased blood pressure and CVD mortality in winter. Careful monitoring and more aggressive blood pressure lowering treatment in the cold months are needed to help reduce the winter excess CVD mortality in high-risk individuals.

[Status of exclusive breastfeeding and influencing factors for 1,882 pairs of mother and neonate during 0- 7 days postpartum in China].

OBJECTIVE: To investigate the status of exclusive breastfeeding(EBF) and possible influencing factors during 0-7 days postpartum in China. METHODS: During 2011 to 2013, healthy mothers and neonates who were in the period of 0- 7 days postpartum from 8 provinces across different regions of China were recruited to take the questionnaire investigations and physical examinations. Information about socio-economic, pregnant, and delivery status, infant healthy situation and feeding indicators was collected to calculate the rate of exclusive breastfeeding during 0- 7 days postpartum and analyze the influencing factors. RESULTS: A total of 1 882 pairs of mothers and neonates were covered by this study. The rate of EBF was 13.3% (250 cases) during 0- 7 days postpartum. Bottle feeding (OR=0.08, 95% CI: 0.05- 0.12), the mothers themselves mixed fed at their 0-4 months old (OR=0.22, 95%CI: 0.08-0.58), the mothers who had used methods to stimulate milk secretion (OR=0.58, 95% CI: 0.35- 0.94) might decrease the EBF rate. Compared with the mothers who believed that their breast milk was not enough for their infants, the mothers who believed breastmilk was enough may increase the EBF rate (OR=6.04, 95%CI: 3.34-10.94). Comparing to the EBF rate of Beijing, Yunnan (OR=0.10, 95%CI: 0.04-0.24), and Gansu(OR=0.03,95%CI: 0.01-0.08) had lower EBF rate during 0-7 days postpartum. What's more, the EBF rate increased with the increasing neonates' age (OR=1.33, 95% CI: 1.16- 1.53). CONCLUSION: The EBF rate during 0- 7 days postpartum is still low in China and had significant differences in different regions. Suboptimal feeding knowledge and practices affected the EBF rate significantly.

Crystal Facets Make a Profound Difference in Polyoxometalate-Containing Metal-Organic Frameworks as Catalysts for Biodiesel Production.

An inherent challenge in using metal-organic frameworks (MOFs) for catalysis is how to access the catalytic sites generally confined inside the porous structure, in particular for substrates larger than the pores. We present here a promising solution to bypass this roadblock by modulating the facets of a crystalline MOF NENU-3a to enhance the facet exposure of the catalytic sites and the adsorption of substrates. Specifically, by transforming it with encapsulated catalysis-responsible polyoxometalate from octahedron characterized entirely by {111} facets to cube with only {100} facets, much enhanced catalytic activities were observed, especially for sterically demanding substrates that are otherwise hard to diffuse into the pores. Crystallographic analysis and adsorption/desorption experiments collectively established the critical effects of morphological control on the enhanced catalysis. The cubic crystals were then applied for biodiesel production, reaching more than 90% conversion of fatty acids (C12-C22) in comparison to <22% using octahedral crystals.

Molecular-caged metal-organic frameworks for energy management.

Metal-organic frameworks (MOFs) hold great promise for diverse applications when combined with polymers. However, a persistent challenge lies in the susceptibility of exposed MOF pores to molecule and polymer penetration, compromising the porosity and overall performance. Here, we design a molecular-caged MOF (MC-MOF) to achieve contracted window without sacrificing the MOF porosity by torsional conjugated ligands. These molecular cages effectively shield against the undesired molecule penetration during polymerization, thereby preserving the pristine porosity of MC-MOF and providing outstanding light and thermal management to the composites. The polymer containing 0.5 wt % MC-MOF achieves an 83% transmittance and an exceptional haze of 93% at 550 nanometers, coupled with remarkable thermal insulation. These MC-MOF/polymer composites offer the potential for more uniform daylighting and reduced energy consumption in sustainable buildings when compared to traditional glass materials. This work delivers a general method to uphold MOF porosity in polymers through molecular cage design, advancing MOF-polymer applications in energy and sustainability.

Copper hexacyanoferrate/carbon sheet combination with high selectivity and capacity for copper removal by pseudocapacitance.

The efficient capture of copper ions (Cu2+) in wastewater has dual significance in pollution control and resource recovery. Prussian blue analog (PBA)-based pseudocapacitive materials with open frameworks and abundant metal sites have attracted considerable attention as capacitive deionization (CDI) electrodes for copper removal. In this study, the efficiency of copper hexacyanoferrate (CuHCF) as CDI electrode for Cu2+ treating was evaluated for the first time upon the successful synthesis of copper hexacyanoferrate/carbon sheet combination (CuHCF/C) by introducing carbon sheet as conductive substrate. CuHCF/C exhibited significant pseudocapacitance and high specific capacitance (52.92 F g-1) through the intercalation, deintercalation, and coupling of Cu+/Cu2+ and Fe2+/Fe3+ redox pairs. At 0.8 an applied voltage and CuSO4 feed liquid concentration of 100 mg L-1, the salt adsorption capacity was 134.47 mg g-1 higher than those of most reported electrodes. Moreover, CuHCF/C demonstrated excellent Cu2+ selectivity in multi-ion coexisting solutions and in actual wastewater experiments. Density functional theory (DFT) calculations were employed to elucidate the mechanism. This study not only reveals the essence of Cu2+ deionization by PBAs pseudocapacitance with promising potential applications but also provides a new strategy for selecting efficient CDI electrodes for Cu2+ removal.

Upregulation of inflammatory genes and pathways links obesity to severe COVID-19.

Obesity is a risk factor for developing severe COVID-19. However, the mechanism underlying obesity-accelerated COVID-19 remains unclear. Here, we report results from a study in which 2-3-month-old K18-hACE2 (K18) mice were fed a western high-fat diet (WD) or normal chow (NC) over 3 months before intranasal infection with a sublethal dose of SARS-CoV2 WA1 (a strain ancestral to the Wuhan variant). After infection, the WD-fed K18 mice lost significantly more body weight and had more severe lung inflammation than normal chow (NC)-fed mice. Bulk RNA-seq analysis of lungs and adipose tissue revealed a diverse landscape of various immune cells, inflammatory markers, and pathways upregulated in the infected WD-fed K18 mice when compared with the infected NC-fed control mice. The transcript levels of IL-6, an important marker of COVID-19 disease severity, were upregulated in the lung at 6-9 days post-infection in the WD-fed mice when compared to NC-fed mice. Transcriptome analysis of the lung and adipose tissue obtained from deceased COVID-19 patients found that the obese patients had an increase in the expression of genes and the activation of pathways associated with inflammation as compared to normal-weight patients (n = 2). The K18 mouse model and human COVID-19 patient data support a link between inflammation and an obesity-accelerated COVID-19 disease phenotype. These results also indicate that obesity-accelerated severe COVID-19 caused by SARS-CoV-2 WA1 infection in the K18 mouse model would be a suitable model for dissecting the cellular and molecular mechanisms underlying pathogenesis.

[Determination and clinical significance of serum surfactant proteins A and D in children with bronchiolitis].

OBJECTIVE: To study the variation and clinical significance of serum levels of surfactant proteins A (SP-A) and D (SP-D) among children with different degrees of bronchiolitis. METHODS: Seventy children with bronchiolitis were divided into acute (n=42) and recovery phase groups (n=28). According to the severity of symptoms, the acute phase group was further divided into severe (n=12) and mild subgroups (n=30). Another 26 children who were hospitalized in the same period due to non-infectious diseases and had not undergone surgery were used as the control group. Competitive enzyme-linked immunosorbent assay was performed to measure serum levels of SP-A and SP-D in each group. RESULTS: The acute phase group had significantly higher serum levels of SP-A and SP-D compared with the recovery phase (P<0.01) and control groups (P<0.01). Compared with the control group, the recovery phase group had elevated levels of SP-A and SP-D (P<0.01). Within the acute phase group, serum levels of SP-A and SP-D in the severe subgroup were significantly higher than in the mild subgroup (P<0.01). CONCLUSIONS: Serum levels of SP-A and SP-D are significantly elevated in children with acute bronchiolitis, and severe cases have higher serum levels of SP-A and SP-D than mild cases. Even after the relief of clinical symptoms, serum levels of SP-A and SP-D remain high. These findings suggest that serum levels of SP-A and SP-D might be useful biomarkers for evaluating the severity of bronchiolitis among children.

Design of Imide Oligomer-Mediated MOF Clusters for Solar Cell Encapsulation Systems by Interface Fusion Strategy.

Dielectric encapsulation materials are promising for solar cell areas, but the unsatisfactory light-management capability and relatively poor dielectric properties restrict their further applications in photovoltaic and microelectronic devices. Herein, an interface fusion strategy to engineer the interface of MOF (UiO-66-NH2 ) with anhydride terminated imide oligomer (6FDA-TFMB) is designed and a novel MOF cluster (UFT) with enhanced forward scattering and robust porosity is prepared. UFT is applied as an optical and dielectric modifier for bisphenol A epoxy resin (DGEBA), and UFT epoxy composites with high transmittance (>80%), tunable haze (45-58%) and excellent dielectric properties can be prepared at low UFT contents (0.5-1 wt%), which delivers an optimal design for dielectric encapsulation systems with efficient light management in solar cells. Additionally, UFT epoxy composites also show excellent UV blocking, and hydrophobic, thermal and mechanical properties. This work provides a template for the synthesis of covalent bond-mediated nanofillers and for the modulation of haze and dielectric properties of dielectric encapsulation materials for energy systems, semiconductors, microelectronics, and more.

Enabling Scalable Polymer Electrolyte with Dual-Reinforced Stable Interface for 4.5 V Lithium-Metal Batteries.

Hitherto, it remains a great challenge to stabilize electrolyte-electrode interfaces and impede lithium dendrite proliferation in lithium-metal batteries with high-capacity nickel-rich LiNx Coy Mn1- x-y O2 (NCM) layer cathodes. Herein, a special molecular-level-designed polymer electrolyte is prepared by the copolymerization of hexafluorobutyl acrylate and methylene bisacrylamide to construct dual-reinforced stable interfaces. Verified by X-ray photoelectron spectroscopy depth profiling, there are favorable solid electrolyte interphase (SEI) layers on Li metal anodes and robust cathode electrolyte interphase (CEI) on Ni-rich cathodes. The SEI enriched in lithiophilic N-(C)3 guides the homogenous distribution of Li+ and facilitates the transport of Li+ through LiF and Li3 N, promoting uniform Li+ plating and stripping. Moreover, the CEI with antioxidative amide groups can suppress the parasitic reactions between cathode and electrolyte and the structural degradation of cathode. Meanwhile, a unique two-stage rheology-tuning UV polymerization strategy is utilized, which is quite suited for continuous electrolyte fabrication with environmental friendliness. The fabricated polymer electrolyte exhibits a high ionic conductivity of 1.01 mS cm-1 at room temperature. 4.5 V NCM622//Li batteries achieve prolonged operation with a retention rate of 85.0% after 500 cycles at 0.5 C. This work provides new insights into molecular design and processibility design for polymer-based high-voltage batteries.

{Ta12}/{Ta16} cluster-containing polytantalotungstates with remarkable photocatalytic H2 evolution activity.

Four novel polytantalotungstates K(5)Na(4)[P(2)W(15)O(59)(TaO(2))(3)]·17H(2)O (1), K(8)Na(8)H(4)[P(8)W(60)Ta(12)(H(2)O)(4)(OH)(8)O(236)]·42H(2)O (2), Cs(3)K(3.5)H(0.5)[SiW(9)(TaO(2))(3)O(37)]·9H(2)O (3), and Cs(10.5)K(4)H(5.5)[Ta(4)O(6)(SiW(9)Ta(3)O(40))(4)]·30H(2)O (4) were synthesized. Compounds 1 and 3 are tris-(peroxotantalum)-substituted Dawson- and Keggin-type derivatives, whereas 2 and 4 are tetrameric oligomers containing respectively an unprecedented {Ta(12)} and {Ta(16)} cluster core. The photocatalytic activities of 2 and 4 for H(2) evolution from water were evaluated. The significantly enhanced performance against the control K(6)[P(2)W(18)O(62)] can be attributed to the modulation of the electronic structures of these novel POMs by Ta incorporation. The highest activity observed so far with the use of 2 can be further rationalized by the presence of distorted heptacoordinate Ta atoms in the form of TaO(7) pentagonal bipyramid.