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The defect models of the orthorhombical and tetragonal Cu2+ centers in Pb[Zr0.54Ti0.46]O3 are attributed to Cu2+ ions occupying the sixfold coordinated octahedral Ti4+ site with and without charge compensation, respectively. The electron paramagnetic resonance (EPR) g factors gi (i = x, y, z) of the Cu2+ centers in Pb[Zr0.54Ti0.46]O3 are theoretically studied by using the perturbation formulas of a 3d9 ion under orthorhombically and tetragonally elongated octahedra. Based on the calculation, the impurity off-center displacements are about 0.253 and 0.162 Å for the orthorhombical and tetragonal Cu2+ centers, respectively. Meanwhile, the planar Cu2+-O2- bonds are found to experience the relative variation ΔR (≈0.102 Å) along the a- and b-axes for the orthorhombical Cu2+ center due to the Jahn-Teller (JT) effect. The theoretical EPR g factors based on the above local structures agree well with the observed values.
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BACKGROUND: To explore the time-frequency structure and cross-scale coupling of electroencephalography (EEG) signals during seizure in juvenile myoclonic epilepsy (JME), correlations between different leads, as well as dynamic evolution in epileptic discharge, progression and end of seizure were examined. METHODS: EEG data were obtained for 10 subjects with JME and 10 normal controls and were decomposed using gauss continuous wavelet transform (CWT). The phase amplitude coupling (PAC) relationship between the 11th (4.57 Hz) and 17th (0.4 Hz) scale was investigated. Correlations were examined between the 11th and 17th scale EEG signals in different leads during seizure, using multi-scale cross correlation analysis. RESULTS: The time-frequency structure of JME subjects showed strong rhythmic activity in the 11th and 17th scales and a close PAC was identified. Correlation analysis revealed that the ictal JME correlation first increased in the anterior head early in seizure and gradually expanded to the posterior head. CONCLUSION: PAC was exhibited between the 11th and 17th scales during JME seizure. The results revealed that the correlation in the anterior leads was higher than the posterior leads. In the perictal period, the 17th scale EEG signal preceded the 11th scale signal and remained for some time after a seizure. This suggests that the 17th scale signal may play an important role in JME seizure.
Subject(s)
Electroencephalography , Myoclonic Epilepsy, Juvenile , Humans , Myoclonic Epilepsy, Juvenile/physiopathology , Myoclonic Epilepsy, Juvenile/diagnosis , Electroencephalography/methods , Male , Female , Young Adult , Adult , Adolescent , Wavelet Analysis , Brain/physiopathology , Brain Waves/physiology , Signal Processing, Computer-AssistedABSTRACT
Objective: To investigate the changes in the wavelet entropy during wake and different sleep stages in patients with insomnia disorder. Methods: Sixteen patients with insomnia disorder and sixteen normal controls were enrolled. They underwent scale assessment and two consecutive nights of polysomnography (PSG). Wavelet entropy analysis of electroencephalogram (EEG) signals recorded from all participants in the two groups was performed. The changes in the integral wavelet entropy (En) and individual-scale wavelet entropy (En(a)) during wake and different sleep stages in the two groups were observed, and the differences between the two groups were compared. Results: The insomnia disorder group exhibited lower En during the wake stage, and higher En during the N3 stage compared with the normal control group (all P < 0.001). In terms of En(a), patients with insomnia disorder exhibited lower En(a) in the ß and α frequency bands during the wake stage compared with normal controls (ß band, P < 0.01; α band, P < 0.001), whereas they showed higher En(a) in the ß and α frequency bands during the N3 stage than normal controls (ß band, P < 0.001; α band, P < 0.001). Conclusion: Wavelet entropy can reflect the changes in the complexity of EEG signals during wake and different sleep stages in patients with insomnia disorder, which provides a new method and insights about understanding of pathophysiological mechanisms of insomnia disorder. Wavelet entropy provides an objective indicator for assessing sleep quality.
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BACKGROUND: Epilepsy is a neurological disorder characterized by recurrent seizures. We aimed to investigate the association between the percentage of dietary carbohydrate intake (DCI) and epilepsy prevalence among American adults. METHODS: We analyzed the data from 9,584 adults aged 20-80 years who participated in the National Health and Nutrition Examination Survey from 2013 to 2018. Logistic regression was applied to explore the association between the percentage of DCI and epilepsy prevalence. RESULTS: A total of 146 (1.5%) individuals with epilepsy were enrolled in this study. The average age of the participants was 56.4 years, and 5,454 (56.9%) individuals were female. A high DCI was associated with an increased prevalence of epilepsy (odds ratio [OR], 4.56; 95% confidence interval [CI], 1.11-18.69; P = 0.035) after adjusting for age, sex, marital status, race/ethnicity, educational level, family income, body mass index, smoking status, drinking status, hypertension, diabetes, and cardiovascular disease. Stratified analyses indicated a positive correlation between DCI and epilepsy prevalence in adults with different characteristics. Compared with individuals in quartile 1 of DCI (<40.5%), those in quartile 4 (>55.4%) had an adjusted OR for epilepsy of 1.72 (95% CI, 1.09-2.73, P = 0.02, P for trend = 0.012). CONCLUSIONS: A high percentage of DCI was associated with an increased prevalence of epilepsy. The risk of epilepsy increased 3.5-fold with a 1% increase in DCI. These results suggest an important role of DCI in the dietary management of epilepsy.
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The flame-retardant paper has gradually evolved into a necessary material in various industries as a result of the rising importance of fire safety, energy efficiency, and environmental preservation. Traditional cellulose paper requires the addition of a large amount of flame retardants to achieve flame retardancy, which poses a serious threat to mechanical quality and the environment. Therefore, there is an urgent need to develop inorganic fiber flame-retardant paper with good flexibility, high thermal stability, and inherent flame retardancy. Herein, inspired by the "brick-and-mortar" layered structure of nature nacre, we developed a layered composite paper with a unique alternating arrangement of organic-inorganic fibers by synergistically integrating environmentally sustainable basalt fiber (BF) and high-performance aramid nanofibers (ANFs) through a vacuum-assisted filtration process. The as-prepared ANFs/BF composite paper exhibited low thermal conductivity (0.024 W m-1 K-1), high tensile strength (54.22 MPa), and excellent flexibility. Thanks to its excellent thermal stability, the mechanical strength remains at a high level (92%) after heat treatment at 300 °C for 60 min. Furthermore, the peak heat release rate and smoke generation of ANFs/BF composite paper decreased by 44.6 and 95.3%, respectively. Therefore, the composite paper is promising for applications as a protective layer in flexible electronic devices, cables, and fire-retardant and high-temperature fields.
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The local structure and spin Hamiltonian parameters (SHPs) g factors (gx , gy , gz ) and the hyperfine structure constants (Ax , Ay , Az ) for Cu2+ doped in the LiTaO3 crystal are theoretically investigated by the perturbation formulas for a 3d9 ion under rhombically elongated octahedral based on the cluster approach. The impurity Cu2+ was assumed to occupy the host trigonally-distorted octahedral Li+ site and experience the Jahn-Teller (JT) distortion from the host trigonal octahedral [TaO6 ]10- to the impurity rhombically elongated octahedral [CuO6 ]10- . Based on the calculations, the impurity-ligand bond lengths parallel and perpendicular to the C2 -axis are found to be R|| (≈ 2.305 Å) and R⥠(≈ 2.112 Å) for the studied [CuO6 ]10- cluster, with the planar bond angle θ (≈ 78.2°). Meanwhile, the ground-state wave function for Cu2+ center in LiTaO3 was also obtained. The calculated SHPs based on the above local lattice distortions agree well with the experimental data, and the results are discussed.
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Silicate scales are commonly incorporated into cellulose nanofiber (CNF) as functional fillers to enhance electrical insulation and UV-shielding properties. Nevertheless, the addition of substantial quantities of silicate scales in the quest for enhanced functional properties results in reduced interface bonding capability and compromised mechanical properties, thereby restricting their application. Here, inspired from nacre, layered composite paper with excellent mechanical strength, electrical insulation and UV-resistance properties was fabricated through vacuum assisted self-assembly using CNF, PVA and basalt scales (BS). Unlike the conventional blending strategy, the pre-mixed PVA and BS suspension facilitates the formation of Al-O-C bond, thereby enhancing the interfacial bonding between BS and CNF. Consequently, the composite paper (BS@PVA/PVA/CNF) containing 60 wt% BS demonstrates higher mechanical strength-approximately 140 % higher than that of BS/CNF composite paper, achieving a strength of 33.5 MPa. Additionally, it demonstrates enhanced dielectric properties, surpassing those of CNF paper by up to 107 %. Moreover, it exhibits robust ultraviolet-resistant aging performance, retaining ~87 % of its tensile strength after undergoing a simulated two-year aging period. As a result, this work presents a simple and innovative design strategy for enhancing interfacial bonding and optimizing layer structure, providing essential guidelines for large-scale production of high-performance insulation and aging-resistant composite paper.
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Nacre , Cellulose , SilicatesABSTRACT
Although microstructure optimization is an effective strategy to improve and regulate electromagnetic wave (EMW) absorption properties, preparing microwave absorbents with enhanced EMW absorbing performance and tuned absorption band by a simple method remains challenging. Herein, ZnIn2S4/reduced graphene oxide (rGO) composites with flower-like and cloud-like morphologies were fabricated by a convenient hydrothermal method. The ZnIn2S4/rGO composites with different morphologies realize efficient EMW absorption and tunable absorption bands, covering a wide frequency range. The flower-like structure has an optimal reflection loss (RL) of up to -49.2 dB with a maximum effective absorption bandwidth (EAB) of 5.7 GHz, and its main absorption peaks are concentrated in the C and Ku bands. The minimal RL of the cloud-like structure can reach -36.3 dB, and the absorption peak shifts to the junction of X and Ku bands. The distinguished EMW absorption capacity originates from the uniquely optimized microstructure, complementary effect of ZnIn2S4 and rGO in dielectric constant, and synergy of various loss mechanisms, such as interfacial polarization, dipole polarization, conductive loss, and multiple reflections. This study proposes a guide for the structural optimization of an ideal EMW absorber to achieve efficient and tunable EMW absorption performance.
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Background: No interventional study has been conducted in China to assess efficacy and safety of perampanel in treating Chinese patients with epilepsy, nor has there been any study on perampanel early add-on therapy in China. This interventional study aimed to assess efficacy and safety of perampanel as an early add-on treatment of focal-onset seizures (FOS) with or without focal-to-bilateral tonic-clonic seizures (FBTCS) in Chinese patients. Methods: In this multicenter, open-label, single-arm, phase 4 interventional study, Chinese patients ≥ 12 years old with FOS with or without FBTCS who failed anti-seizure medication (ASM) monotherapy from 15 hospitals in China were enrolled and treated with perampanel add-on therapy (8-week titration followed by 24-week maintenance). The primary endpoint was 50% responder rate. Secondary endpoints included seizure-freedom rate and changes in seizure frequency from baseline. Treatment-emergent adverse events (TEAEs) and drug-related TEAEs were recorded. Results: The full analysis set included 150 patients. The mean maintenance perampanel dose was 5.9 ± 1.5 mg/day and the 8-month retention rate was 72%. The 50% responder rate and seizure-freedom rate for all patients during maintenance were 67.9 and 30.5%, respectively. Patients with FBTCS had higher 50% responder rate (96.0%) and seizure-freedom rate (76.0%) during maintenance. Patients on concomitant sodium valproate had a significantly higher seizure-freedom rate than those on concomitant oxcarbazepine. Eight-six (55.1%) patients experienced treatment-related TEAEs, and the most common TEAEs were dizziness (36.5%), hypersomnia (11.5%), headache (3.9%), somnolence (3.2%), and irritability (3.2%). Withdrawal due to TEAEs occurred to 14.7% of the patients. Conclusion: Perampanel early add-on was effective and safe in treating Chinese patients≥12 years old with FOS with or without FBTCS.Clinical trial registrationwww.chictr.org.cn, Identifier ChiCTR2000039510.
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Background: There is great scope for improving the quality of pain management. Although pain prevalence has been investigated in several countries, few studies have comparatively assessed changes in pain prevalence and management over a span of multiple years. Aim: This work was aimed at determining the pain prevalence and evaluating the condition of pain management in a Chinese general hospital in 2021 and comparing them with corresponding data from 10 years ago. Methods: Repeated single-center cross-sectional studies were initiated on June 14th, 2011, and September 2nd, 2021, in the same tertiary grade A Chinese general hospital. The same structured questionnaire was used to collect inpatient data on pain intensity and classification and pain management outcomes. We performed statistical analyses to compare categorical variables to assess changes over time. Results: The sample sizes for the investigations in 2011 and 2021 were 2323 and 4454, respectively. In 2021, 24.34% of patients experienced pain; this percentage was significantly lower than that in 2011. Meanwhile, the prevalence of moderate and severe pain decreased from 14.73% in 2011 to 4.98% in 2021. The other six indicators of pain management outcomes also improved significantly. The percentages of patients using painkillers, opioid analgesics, and multiple analgesics increased from 44.61 to 51.38%, 24.01% to 44.61%, and 6.82% to 14.11%, respectively. Furthermore, the percentages of patients who received pain information and who actively reported pain increased from 27.56% to 96.5% and from 85.54% to 98.71%, respectively. The percentage of patients qualified to accurately use the Numerical Rating Scale increased from 10.5% to 79.98%. Conclusion: The quality and outcomes of pain management improved greatly after the establishment and implementation of the pain management system. Nonetheless, pain of different intensities is common after major surgeries, and it is recommended that hospitals popularize and implement perioperative multimodal analgesia strategies to reduce the incidence of postoperative pain.
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The rapid development of modern electrical equipment has led to urgent demands for electrical insulating materials with mechanical reliability and excellent dielectric properties. Herein, basalt nanosheets (BSNs) with high aspect ratios (≈780.1) are first exfoliated from basalt scales (BS) through a reliable chemical/mechanical approach. Meanwhile, inspired by the layered architecture of natural nacre, nacre-mimetic composite nanopapers are reported containing a 3D aramid nanofibers (ANF) framework as a matrix and BSNs as ideal building blocks through vacuum-assisted filtration. The as-prepared ANF-BSNs composite nanopapers exhibit considerably enhanced mechanical properties with ultralow BSNs content. These superiorities are wonderfully integrated with exceptional dielectric breakdown strength, prominent volume resistivity, and extremely low dielectric constant and loss, which are far superior to conventional nacre-mimetic composite nanopapers. Notably, the tensile strength and breakdown strength of ANF-BSNs composite nanopapers with a mere 1.0 wt% BSNs reach 269.40 MPa and 77.91 kV mm-1 , respectively, representing an 87% and 133% increase compared to those of the control ANF nanopaper. Their properties are superior to those of previously reported nacre-mimetic composite nanopapers and commercial insulating micropapers, indicating that ANF-BSNs composite nanopapers are a highly promising electrical insulating material for miniaturized high-power electrical equipment.
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OBJECTIVE: To explore changes in the alpha rhythm wavelength of background electroencephalography in Alzheimer's disease patients with different degrees of dementia in a resting state; examine their correlation with the degree of cognitive impairment; determine whether the alpha rhythm wavelength can distinguish mild Alzheimer's disease patients, moderately severe Alzheimer's disease patients, and healthy controls at the individual level; and identify a cut-off value to differentiate Alzheimer's disease patients from healthy controls. METHODS: Quantitative electroencephalography signals of 42 patients with mild Alzheimer's disease, 42 patients with moderately severe Alzheimer's disease, and 40 healthy controls during rest state with eyes closed were analyzed using wavelet transform. Electroencephalography signals were decomposed into different scales, and their segments were superimposed according to the same length (wavelength and amplitude) and phase alignment. Phase averaging was performed to obtain average phase waveforms of the desired scales of each lead. The alpha-band wavelengths corresponding to the ninth scale of the background rhythm of different leads were compared between groups. RESULTS: The average wavelength of the alpha rhythm phase of the whole-brain electroencephalography signals in Alzheimer's disease patients was prolonged and positively correlated with the severity of cognitive dysfunction (P < 0.01). The ninth-scale phase average wavelength of each lead had high diagnostic efficacy for Alzheimer's disease, and the diagnostic efficacy of lead P3 (area under the receiver operating characteristic curve = 0.873) was the highest. CONCLUSION: The average wavelength of the electroencephalography alpha rhythm phase may be used as a quantitative feature for the diagnosis of Alzheimer's disease, and the slowing of the alpha rhythm may be an important neuro-electrophysiological index for disease evaluation.
Subject(s)
Alzheimer Disease , Cognitive Dysfunction , Humans , Alpha Rhythm/physiology , Electroencephalography , BiomarkersABSTRACT
This paper aimed to experimentally clarify the crushing mechanism and performance of expanded polypropylene foam (EPP) and analyze the influence of density and thickness on its mechanical behavior and energy absorption properties under static crushing loadings. Hence, a series of compression tests were carried out on EPP foams with different densities and thicknesses. For foam with a density of 60 kg/m3, the mean crushing strength, energy absorption (Ea), energy absorption efficiency (Ef), specific energy absorption (SEA), and energy absorption per unit volume (w) increased by 245.3%, 187.2%, 42.3%, 54.3%, and 242.8%, respectively, compared to foam with a density of 20 kg/m3. Meanwhile, compared to foam with a thickness of 30 mm, the mean crushing strength, energy absorption (Ea), energy absorption efficiency (Ef), SEA, and energy absorption per unit volume (w) for foam with a thickness of 75 mm increased by 53.3%, 25.2%, -10.8%, -4.7%, and -10.6%, respectively. The results show that foam density has a significantly greater influence on static compressive performance than foam thickness. The microstructures of the EPP foam before and after static compression were compared by observing with a scanning electron microscope (SEM), and the failure mechanism was analyzed. Results showed that the load and energy as well as the deformation and instability processes of its cells were transferred layer by layer. The influence of density on the degree of destruction of the internal cells was obvious. Due to its larger mass and larger internal damping, thicker foams were less damaged, and less deformation was produced. Additionally, the EPP foam exhibited a considerable ability to recover after compression.
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In the practical application of microwave absorbing materials, traditional powder materials need to be mixed with the matrix to fabricate composite coatings. However, the complex preparation process of composite coatings and the uneven dispersion of powders in the matrix limit their application. To solve these problems, two-dimensional (2D) F-WS2/CP composite films were prepared by using carbon paper (CP) as a dispersion matrix and loading flower-like WS2 on its surface through a simple hydrothermal method. The morphology and microwave absorption (MA) performance of the composite films are easily regulated by adjusting the amount of reaction precursors. The combination of WS2 and CP facilitates impedance matching and improves the electromagnetic wave attenuation performance based on the synergistic effect of different loss mechanisms including multiple reflections and scattering, interfacial polarization, dipolar polarization, and conduction loss. At a low filler content (5 wt%), the maximum reflection loss (RL) of the composite film is up to -50 dB (99.999% energy absorption) at 12.5 GHz with 2.8 mm thickness. Moreover, at a relatively thin 1.8 mm thickness, its maximum RL remains -35 dB (>99.9% energy absorption). The as-prepared composite film shows excellent MA properties at a thinner thickness and lower filling content, providing inspiration for the preparation of light weight and efficient 2D thin-film microwave absorbers in the future.
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Pressure sensors with desirable flexibility, robustness, and versatility are urgently needed for complicated smart wearable devices. However, developing an ideal multifunctional flexible sensor is still challenging. In this work, a composite aerogel film sensor with an internal three-dimensional (3D) microporous and hierarchical structure is successfully fabricated by the self-assembly of aramid nanofiber (ANF) and conductive MXene by vacuum-assisted filtration and ice crystal growth. The resultant MXene/ANF aerogel film with a mass ratio of 3/7 (30% MAAF) presents high robustness with an outstanding tensile strength of 14.1 MPa and a modulus of 455 MPa while retaining appealing flexibility and sensitive characteristics due to the 3D microstructure. Accompanied by superior electric conductivity, the MAAF sensor performs noticeably in human motion and microexpression detection with a fast response time of 100 ms and a high sensitivity of 37.4 kPa-1. In addition, MAAF exhibits considerable thermal shielding performance based on the excellent thermostability. Moreover, it possesses prominent electrothermal property with a wide heating temperature range (32.7-242 °C) in a fast thermal response time (5 s) due to the Joule effect. Additionally, a hydrophobic SiO2 coating is introduced on the surface of MAAF to further broaden the sensing application, and the obtained MAAF@SiO2 sensor shows distinguished sensing capability underwater, which can be accurately applied to swimming monitoring. Therefore, this work provides a highly flexible, lightweight, robust, and multifunctional aerogel film sensor, showing promising potential in smart wearable sensing and healthcare devices, intelligent robots, and underwater detection.
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Epidemiological evidence of the effects of PM2.5 elements on lung function and DNA methylation is limited. We conducted a longitudinal panel study of 76 healthy older adults aged 60-69 years in Jinan, China, from September 2018 to January 2019. We periodically measured individual 72 h PM2.5 and element concentrations, lung function, and DNA methylation levels of eight inflammation-related genes. We used linear mixed-effect models to investigate the effects of exposure to personal PM2.5 elements on the lung function and DNA methylation. Mediation analysis was used to investigate the underlying effect mechanism. Negative changes in the ratio of forced expiratory volume in 1 s to forced vital capacity, ranging from -1.23% [95% confidence interval (CI): -2.11%, -0.35%] to -0.77% (95% CI: -1.49%, -0.04%), were significantly associated with interquartile range (IQR) increases in personal PM2.5 at different lag periods (7-12, 13-24, 25-48, 0-24, 0-48, and 0-72 h). Arsenic (As), nickel, rubidium (Rb), selenium, and vanadium were significantly associated with at least three lung function parameters, and IQR increases in these elements led to 0.12-5.66% reductions in these parameters. PM2.5 elements were significantly associated with DNA methylation levels. DNA methylation mediated 7.28-13.02% of the As- and Rb-related reduced lung function. The findings indicate that exposure to elements in personal PM2.5 contributes to reduced lung function through DNA methylation.
Subject(s)
Air Pollutants , Air Pollution , Humans , Aged , Particulate Matter/analysis , Air Pollutants/analysis , Environmental Exposure/analysis , DNA Methylation , Inflammation/genetics , Lung , China , Air Pollution/analysisABSTRACT
Aramid nanofibers (ANFs) have important applications in many fields, including electrical insulation and battery separators. However, a few limitations seriously restrict the application of ANFs currently, such as low preparation efficiency and the unclear preparation mechanism. To overcome these limitations, the present work proposes a new view-point from the perspective of reaction kinetics. The preparation efficiency was proven to essentially rely on the effective c(OH-). With a simple pre-treatment, a kinetic advantage was created and the preparation time of ANFs was reduced from multiple hours to 10 minutes, which was a considerable step towards practical applications. Moreover, the resultant ANF membranes still exhibited excellent properties in terms of mechanical strength (tensile strength > 160 MPa), thermal stability, light transmittance, and electrical insulation (above 90 kV mm-1). This work not only presents an ultrafast method to produce ANFs but also provides new insights into the mechanism that will benefit the subsequent development of ANF-based materials.
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Moisture-trigged electricity generator (MEG) that can convert ubiquitous moisture into electricity are highly desirable for developing renewable energy supply and ameliorating the crisis in energy. Constructing an asymmetric ordered, namely gradient ordered porous membrane has great potential in MEG. Herein, a series of cellulose acetate (CA)-based membranes with ordered asymmetric honeycomb membranes were fabricated by Breath Figure method, along with silver nanowires (AgNWs) coating. The asymmetric gradient honeycomb pores were achieved by graft modification of lauroyl chloride and adjustment of relative humidity, which not only endowed the MEG with sensitive sensing signals transport under tension and humidity fluctuations but also enhanced voltages generation speed under flowing moisture. The current study provides a facile and scalable strategy for constructing asymmetric gradient ordered porous materials and creates more possibilities for MEG self-powered flexible wearable electronic devices.
Subject(s)
Nanowires , Wearable Electronic Devices , Cellulose , Electricity , HumidityABSTRACT
Mineral fillers hinder cellulosic fiber bonding and thus limit the increase of filler content in paper. Herein, precipitated calcium carbonate (PCC)/cellulose nanofibrils (CNF) composites were fabricated by a facile and efficient strategy, i.e., co-refining process (CRP). During this process, CNF and PCC were activated by mechanochemical effect and formed encapsulation structure by calcium ion coordination and hydrogen bonding. The encapsulation structure and H-bond/ionic coordination interactions not only endowed the composite with excellent size stability but also enhanced interfacial interaction between composite fillers and cellulosic fibers. Compare with the paper filled with only PCC, PCC + CNF mixture, the tensile index of the cellulosic paper containing PCC/CNF composite was increased by 44.48% and 12.14%, respectively. These results not only provide a facile and scalable approach to increase interaction between cellulosic fiber and mineral filler but also create more possibilities for special paper-based materials with requiring high content of inorganic materials.
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Cellulose , Nanofibers , Calcium Carbonate/chemistry , Cellulose/chemistry , Ions , Minerals , Nanofibers/chemistryABSTRACT
Activation of molecular oxygen plays a crucial role in natural organisms and the modern chemical industry. Herein, we report a Mn-Co dual-single-atom catalyst that exerts a specific synergy in boosting O2 activation by collaboration between two distinct types of activation sites. Taking the oxidative esterification of the biomass platform 5-hydroxymethylfurfural (HMF) as the model reaction, the activation of O2 is demonstrated through transforming O2 into a reactive superoxide anion radical (O2â¢-) on Co-N4 sites and, meanwhile, by reversible consumption and supplement of coordinated surface oxygen as a new type of reactive oxygen species (ROS) on N,O-coordinated single-atom Mn sites (Mn-NxOy). EXAFS analysis results show a longer average Mn-O bond distance at near 2.19 Å, which makes the breaking and formation of surface Mn-O bonds easier to cycle. Control experiments support that such Mn-O bonding conditions could facilitate H-elimination of C-H in HMF. The co-existence of two types of ROS effectively matches the oxidation of hydroxyl and aldehyde groups, and thus, the overall reaction is boosted in excellent yield of diester (95.8%) with an extremely high carbon balance. This study represents a rare example of taking advantage of the synergy of the diatomic catalyst for activating O2 by two types of activation pathways.