Surfaces, interfaces and grain boundaries are classically known to be sinks of defects generated within the bulk lattice. Here, we report an inverse case by which the defects generated at the ...particle surface are continuously pumped into the bulk lattice. We show that, during operation of a rechargeable battery, oxygen vacancies produced at the surfaces of lithium-rich layered cathode particles migrate towards the inside lattice. This process is associated with a high cutoff voltage at which an anionic redox process is activated. First-principle calculations reveal that triggering of this redox process leads to a sharp decrease of both the formation energy of oxygen vacancies and the migration barrier of oxidized oxide ions, therefore enabling the migration of oxygen vacancies into the bulk lattice of the cathode. This work unveils a coupled redox dynamic that needs to be taken into account when designing high-capacity layered cathode materials for high-voltage lithium-ion batteries.
Poor oxygen diffusion at multiphase interfaces in an air cathode suppresses the energy densities of zinc–air batteries (ZABs). Developing effective strategies to tackle the issue is of great ...significance for overcoming the performance bottleneck. Herein, inspired by the bionics of diving flies, a polytetrafluoroethylene layer was coated on the surfaces of Co3O4 nanosheets (NSs) grown on carbon cloth (CC) to create a hydrophobic surface to enable the formation of more three‐phase reaction interfaces and promoted oxygen diffusion, rendering the hydrophobic‐Co3O4 NSs/CC electrode a higher limiting current density (214 mA cm−2 at 0.3 V) than that (10 mA cm−2) of untreated‐Co3O4 NSs/CC electrode. Consequently, the assembled ZAB employing hydrophobic‐Co3O4 NSs/CC cathode acquired a higher power density (171 mW cm−2) than that (102 mW cm−2) utilizing untreated‐Co3O4 NSs/CC cathode, proving the enhanced interfacial reaction kinetics on air cathode benefiting from the hydrophobization engineering.
A bionic‐inspired hydrophobization engineering of electrocatalysts is developed to enable the formation of more three‐phase reaction interfaces and promoted oxygen diffusion on an air cathode, achieving enhanced electrocatalytic efficiency toward zinc–air battery with higher energy density in comparison with that employing the air cathode without hydrophobic surface design.
Heteroatom (N or S)‐doped graphene with high surface area is successfully synthesized via thermal reaction between graphene oxide and guest gases (NH3 or H2S) on the basis of ultrathin graphene ...oxide‐porous silica sheets at high temperatures. It is found that both N and S‐doping can occur at annealing temperatures from 500 to 1000 °C to form the different binding configurations at the edges or on the planes of the graphene, such as pyridinic‐N, pyrrolic‐N, and graphitic‐N for N‐doped graphene, thiophene‐like S, and oxidized S for S‐doped graphene. Moreover, the resulting N and S‐doped graphene sheets exhibit good electrocatalytic activity, long durability, and high selectivity when they are employed as metal‐free catalysts for oxygen reduction reactions. This approach may provide an efficient platform for the synthesis of a series of heteroatom‐doped graphenes for different applications.
Heteroatom (N or S)‐doped graphenes are synthesized via thermal reaction between graphene oxide and guest gases (NH3 or H2S) on ultrathin graphene oxide‐porous silica sheets at high temperatures. It is found that both N and S‐doping can occur to form the different binding configurations in the graphene and both N and S‐doped graphene sheets exhibit excellent electrocatalytic properties for oxygen reduction reaction.
Demonstrated here is the correlation between atomic configuration induced electronic density of single‐atom Co active sites and oxygen reduction reaction (ORR) performance by combining ...density‐functional theory (DFT) calculations and electrochemical analysis. Guided by DFT calculations, a MOF‐derived Co single‐atom catalyst with the optimal Co1‐N3PS active moiety incorporated in a hollow carbon polyhedron (Co1‐N3PS/HC) was designed and synthesized. Co1‐N3PS/HC exhibits outstanding alkaline ORR activity with a half‐wave potential of 0.920 V and superior ORR kinetics with record‐level kinetic current density and an ultralow Tafel slope of 31 mV dec−1, exceeding that of Pt/C and almost all non‐precious ORR electrocatalysts. In acidic media the ORR kinetics of Co1‐N3PS/HC still surpasses that of Pt/C. This work offers atomic‐level insight into the relationship between electronic density of the active site and catalytic properties, promoting rational design of efficient catalysts.
The correlation between atomic configuration induced electronic density of single‐atom Co active sites and oxygen reduction reaction (ORR) performance has been established by combining density‐functional theory calculations and electrochemical analysis. A metal–organic framework derived single‐atom Co catalyst, comprising an optimal Co1‐N3PS active moiety supported on hollow carbon polyhedron (Co1‐N3PS/HC), was synthesized, and it exhibits superior alkaline and acidic ORR performance.
Sexually transmitted diseases (STDs) are a serious issue worldwide. With the popularity of the internet, online health information-seeking behavior (OHISB) has been widely adopted to improve health ...and prevent disease.
This study aimed to investigate the short-term and long-term effects of different types of OHISBs on STDs, including syphilis, gonorrhea, and AIDS due to HIV, based on the Baidu index.
Multisource big data were collected, including case numbers of STDs, search queries based on the Baidu index, provincial total population, male-female ratio, the proportion of the population older than 65 years, gross regional domestic product (GRDP), and health institution number data in 2011-2018 in mainland China. We categorized OHISBs into 4 types: concept, symptoms, treatment, and prevention. Before and after controlling for socioeconomic and medical conditions, we applied multiple linear regression to analyze associations between the Baidu search index (BSI) and Baidu search rate (BSR) and STD case numbers. In addition, we compared the effects of 4 types of OHISBs and performed time lag cross-correlation analyses to investigate the long-term effect of OHISB.
The distributions of both STD case numbers and OHISBs presented variability. For case number, syphilis, and gonorrhea, cases were mainly distributed in southeastern and northwestern areas of China, while HIV/AIDS cases were mostly distributed in southwestern areas. For the search query, the eastern region had the highest BSI and BSR, while the western region had the lowest ones. For 4 types of OHISB for 3 diseases, the BSI was positively related to the case number, while the BSR was significantly negatively related to the case number (P<.05). Different categories of OHISB have different effects on STD case numbers. Searches for prevention tended to have a larger impact, while searches for treatment tended to have a smaller impact. Besides, due to the time lag effect, those impacts would increase over time.
Our study validated the significant associations between 4 types of OHISBs and STD case numbers, and the impact of OHISBs on STDs became stronger over time. It may provide insights into how to use internet big data to better achieve disease surveillance and prevention goals.
Celotno besedilo
Dostopno za:
DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, UILJ, UKNU, UL, UM, UPUK
To identify a robust panel of microRNA (miRNA) signatures that can distinguish renal cell carcinoma (RCC) from normal kidney using miRNA expression levels. We performed a comprehensive meta-analysis ...of 29 published studies that compared the miRNA expression profiles of RCC tissues and adjacent normal tissues (NT) to determine candidate miRNAs as prognostic biomarkers for RCC. Using vote-counting strategy and robust rank aggregation method, we identified a statistically significant miRNA meta-signature of two upregulated (miR-21, miR-210) and three downregulated (miR-141, miR-200c and miR-429) miRNAs. X-tile plot was used to generate the optimum cut-off point for the 15 different deregulated miRNAs and Kaplan-Meier method was used to calculate CSS. In a cohort of 45 patients, the high expression of miR-21 (HR: 5.46, 95%CI: 2.02-53.39) and miR-210 (HR: 6.85, 95%CI: 2.13-43.36), the low expression of miR-141 (HR: 0.16, 95%CI: 0.004-0.18), miR-200c (HR: 0.08, 95%CI: 0.01-0.43) and miR-429 (HR: 0.18, 95%CI: 0.02-0.50) were associated with poor cancer-specific survival (CSS) following RCC resection. We also constructed a five-miRNAs-based classifier as a reliable prognostic and predictive tool for CSS in patients with RCC, especially in clear cell RCC (ccRCC) (HR: 5.46, 95% CI: 1.51-19.66). This method might facilitate patient counselling and individualise management of RCC.
Similar to their optic counterparts, acoustic components are anticipated to flexibly tailor the propagation of sound. However, the practical applications, e.g. for audible sound with large ...wavelengths, are frequently hampered by the issue of device thickness. Here we present an effective design of metasurface structures that can deflect the transmitted airborne sound in an anomalous way. This flat lens, made of spatially varied coiling-slit subunits, has a thickness of deep subwavelength. By elaborately optimizing its microstructures, the proposed lens exhibits high performance in steering sound wavefronts. Good agreement has been demonstrated experimentally by a sample around the frequency 2.55 kHz, incident with a Gaussian beam at normal or oblique incidence. This study may open new avenues for numerous daily life applications, such as controlling indoor sound effects by decorating rooms with light metasurface walls.
Rechargeable magnesium (Mg) metal batteries are a promising candidate for “post‐Li‐ion batteries” due to their high capacity, high abundance, and most importantly, highly reversible and dendrite‐free ...Mg metal anode. However, the formation of passivating surface film rather than Mg2+‐conducting solid electrolyte interphase (SEI) on Mg anode surface has always restricted the development of rechargeable Mg batteries. A stable SEI is constructed on the surface of Mg metal anode by the partial decomposition of a pristine Li electrolyte in the electrochemical process. This Li electrolyte is easily prepared by dissolving lithium tetrakis(hexafluoroisopropyloxy)borate (LiB(hfip)4) in dimethoxyethane. It is noteworthy that Mg2+ can be directly introduced into this Li electrolyte during the initial electrochemical cycles for in situ forming a hybrid Mg2+/Li+ electrolyte, and then the cycled electrolyte can conduct Mg‐ion smoothly. The existence of this as‐formed SEI blocks the further parasitic reaction of Mg metal anode with electrolyte and enables this electrolyte enduring long‐term electrochemical cycles stably. This approach of constructing superior SEI on Mg anode surface and exploiting novel Mg electrolyte provides a new avenue for practical application of high‐performance rechargeable Mg batteries.
A stable Li‐species‐containing solid electrolyte interphase is constructed on the surface of a Mg metal anode by the partial decomposition of a pristine Li electrolyte in the electrochemical process. The existence of this as‐formed solid electrolyte interphase blocks the further parasitic reaction of the Mg metal anode with the electrolyte and allows this electrolyte to endure long‐term electrochemical cycles stably.
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