High-Voltage Na0.76Ni0.25-x/2Mgx/2Mn0.75O2-xFx Cathode Improved by One-Step In Situ MgF2 Doping with Superior Low-Temperature Performance and Extra-Stable Air Stability.

P2-NaxMnO2 has garnered significant attention due to its favorable Na+ conductivity and structural stability for large-scale energy storage fields. However, achieving a balance between high energy density and extended cycling stability remains a challenge due to the Jahn-Teller distortion of Mn3+ and anionic activity above 4.1 V. Herein, we propose a one-step in situ MgF2 strategy to synthesize a P2-Na0.76Ni0.225Mg0.025Mn0.75O1.95F0.05 cathode with improved Na-storage performance and decent water/air stability. By partially substituting cost-effective Mg for Ni and incorporating extra F for O, the optimized material demonstrates both enhanced capacity and structure stability via promoting Ni2+/Ni4+ and oxygen redox activity. It delivers a high capacity of 132.9 mA h g-1 with an elevated working potential of ≈3.48 V and maintains ≈83.0% capacity retention after 150 cycles at 100 mA g-1 within 2-4.3 V, compared to the 114.9 mA h g-1 capacity and 3.32 V discharging potential of the undoped Na0.76Ni0.25Mn0.75O2. While increasing the charging voltage to 4.5 V, 133.1 mA h g-1 capacity and 3.55 V discharging potential (vs Na/Na+) were achieved with 72.8% capacity retention after 100 cycles, far beyond that of the pristine sample (123.7 mA h g-1, 3.45 V, and 43.8%@100 cycles). Moreover, exceptional low-temperature cycling stability is achieved, with 95.0% after 150 cycles. Finally, the Na-storage mechanism of samples employing various doping strategies was investigated using in situ EIS, in situ XRD, and ex situ XPS techniques.

Quantitative Analysis of Resistance to Deformation of the DNA Origami Framework Supported by Struts.

Nanostructures with controlled shapes are of particular interest due to their consistent physical and chemical properties and their potential for assembly into complex superstructures. The use of supporting struts has proven to be effective in the construction of precise DNA polyhedra. However, the influence of struts on the structure of DNA origami frameworks on the nanoscale remains unclear. In this study, we developed a flexible square DNA origami (SDO) framework and enhanced its structural stability by incorporating interarm supporting struts (SDO-s). Comparing the framework with and without such struts, we found that SDO-s demonstrated a significantly improved resistance to deformation. We assessed the deformability of these two DNA origami structures through the statistical analysis of interior angles of polygons based on atomic force microscopy and transmission electron microscopy data. Our results showed that SDO-s exhibited more centralized interior angle distributions compared to SDO, reducing from 30-150° to 60-120°. Furthermore, molecular dynamics simulations indicated that supporting struts significantly decreased the thermodynamic fluctuations of the SDO-s, as described by the root-mean-square fluctuation parameter. Finally, we experimentally demonstrated that the 2D arrays assembled from SDO-s exhibited significantly higher quality than those assembled from SDO. These quantitative analyses provide an understanding of how supporting struts can enhance the structural integrity of DNA origami frameworks.

Twisted DNA Origami-Based Chiral Monolayers for Spin Filtering.

DNA monolayers with inherent chirality play a pivotal role across various domains including biosensors, DNA chips, and bioelectronics. Nonetheless, conventional DNA chiral monolayers, typically constructed from single-stranded DNA (ssDNA) or double-stranded DNA (dsDNA), often lack structural orderliness and design flexibility at the interface. Structural DNA nanotechnology has emerged as a promising solution to tackle these challenges. In this study, we present a strategy for crafting highly adaptable twisted DNA origami-based chiral monolayers. These structures exhibit distinct interfacial assembly characteristics and effectively mitigate the structural disorder of dsDNA monolayers, which is constrained by a limited persistence length of ∼50 nm of dsDNA. We highlight the spin-filtering capabilities of seven representative DNA origami-based chiral monolayers, demonstrating a maximal one-order-of-magnitude increase in spin-filtering efficiency per unit area compared with conventional dsDNA chiral monolayers. Intriguingly, our findings reveal that the higher-order tertiary chiral structure of twisted DNA origami further enhances the spin-filtering efficiency. This work paves the way for the rational design of DNA chiral monolayers.

Spacer-Programmed Two-Dimensional DNA Origami Assembly.

Two-dimensional (2D) DNA origami assembly represents a powerful approach to the programmable design and construction of advanced 2D materials. Within the context of hybridization-mediated 2D DNA origami assembly, DNA spacers play a pivotal role as essential connectors between sticky-end regions and DNA origami units. Here, we demonstrated that programming the spacer length, which determines the binding radius of DNA origami units, could effectively tune sticky-end hybridization reactions to produce distinct 2D DNA origami arrays. Using DNA-PAINT super-resolution imaging, we unveiled the significant impact of spacer length on the hybridization efficiency of sticky ends for assembling square DNA origami (SDO) units. We also found that the assembly efficiency and pattern diversity of 2D DNA origami assemblies were critically dependent on the spacer length. Remarkably, we realized a near-unity yield of ∼98% for the assembly of SDO trimers and tetramers via this spacer-programmed strategy. At last, we revealed that spacer lengths and thermodynamic fluctuations of SDO are positively correlated, using molecular dynamics simulations. Our study thus paves the way for the precision assembly of DNA nanostructures toward higher complexity.

The impact of COVID-19 lockdown on the quality of life of Chinese football referees: the chain mediating role of occupational stress and job burnout.

BACKGROUND: COVID-19 lockdown measures have had a great negative impact on the development of sports competition in China, as well as on the quality of life of football referees. This study aims to explore the impact of lockdown measures implemented in response to the COVID-19 pandemic on the quality of life of football referees in China and its mechanism of action. METHODS: The Impact of Event Scale-Revised (IES-R), the Effort-Reward Imbalance Scale (ERI), the Maslach Burnout Inventory General Survey (MBI-GS), and the World Health Organization Quality of Life Brief Version (WHOQOL-BREF). The scale was used from August to September 2022. Using an online questionnaire, 350 questionnaires were sent out and 338 were returned, for a return rate of 96.57%. Invalid questionnaires were excluded, and 307 football referees with referee grades in 29 provinces registered with the CFA were surveyed. SPSS 24.0 and Mplus 8.0 were used for data analysis and structural equation model testing in this study. RESULTS: The results showed that the COVID-19 lockdown had no significant impact on the quality of life of Chinese football referees. However, the COVID-19 lockdown can affect the quality of life of Chinese football referees through occupational stress or job burnout. Occupational stress and job burnout also play a chain intermediary role between the COVID-19 lockdown and the quality of life of Chinese football referees. In addition, this study further explores the quality of life by dividing it into four dimensions (physical, social, psychological, and environmental). The results show that all four dimensions satisfy the chain mediation model. CONCLUSIONS: Therefore, the quality of life of Chinese football referees can be improved by reducing their occupational stress and job burnout during the COVID-19 lockdown.

Mechanical Properties and Mechanism Analysis of Graphite Tailings Environment-Friendly Concrete.

The development of tailings in concrete technology is not only conducive to the realization of the goal of reducing carbon emissions, but also conducive to the inhibition the occurrence of shortages of sand and gravel supplies. In this study, graphite tailings were used to replace sand in the range of 0~100%, and the mechanical mechanism of graphite tailings concrete was examined through compressive and flexural tests. The mechanical experimental results were evaluated and verified based on concrete macroscopic failure appearance, mesoscopic failure appearance, and physical characteristics of graphite tailings. The results revealed that the concrete strength increases first and then decreases with the increase of the graphite tailings content. Compared to GT00 (GT00 is a specimen with a graphite tailings content of 0%, and so on), GT10~GT60 exhibited better mechanical properties, of which 30% was recommended as the optimal replacement rate. The mechanical properties of GT10 and GT20 had an upward trend, and GT30 had low spalling, with aggregate fragmentation found on the fracture surface. GT30 showed the best resistance to bending and deformation. The mechanical properties of GT40~GT60 had a downward trend. When the graphite tailings content was higher than 70%, the interface defects of the aggregate matrix increased, thus making it easier for cracks to propagate along the interface. Furthermore, the mechanism of graphite tailings replacing sand verified the test results from different perspectives, which provides new analysis ideas for other tailings in environment-friendly concrete.

Overcoming the difficulties of predicting conformational polymorph energetics in molecular crystals via correlated wavefunction methods.

Molecular crystal structure prediction is increasingly being applied to study the solid form landscapes of larger, more flexible pharmaceutical molecules. Despite many successes in crystal structure prediction, van der Waals-inclusive density functional theory (DFT) methods exhibit serious failures predicting the polymorph stabilities for a number of systems exhibiting conformational polymorphism, where changes in intramolecular conformation lead to different intermolecular crystal packings. Here, the stabilities of the conformational polymorphs of o-acetamidobenzamide, ROY, and oxalyl dihydrazide are examined in detail. DFT functionals that have previously been very successful in crystal structure prediction perform poorly in all three systems, due primarily to the poor intramolecular conformational energies, but also due to the intermolecular description in oxalyl dihydrazide. In all three cases, a fragment-based dispersion-corrected second-order Møller-Plesset perturbation theory (MP2D) treatment of the crystals overcomes these difficulties and predicts conformational polymorph stabilities in good agreement with experiment. These results highlight the need for methods which go beyond current-generation DFT functionals to make crystal polymorph stability predictions truly reliable.

[Research Progress on Evaluation Method of Parkinson's Disease Bradykinesia Detection Based on Wearable Device].

Parkinson's Disease (PD) is a neurodegenerative disease that occurs in the middle-aged and elderly population and has dyskinesia as the main clinical symptom. Bradykinesia is a typical dyskinesia symptom of Parkinson's disease. The evaluation of bradykinesia based on wearable devices is an important support for individualized diagnosis and telemedicine. This paper focuses on the bradykinesia, expound the existing detection and evaluation techniques for wearable devices and data analysis methods. This paper also analyzes and discusses some current problems in the field and future research directions.

[Freezing of Gait Detection System for Parkinson's Patients Based on Inertial Measurement Unit].

In order to detect freezing of gait of Parkinson's patients automatically, a system based on inertial measurement unit to detect freezing of gait for Parkinson's patients is established. The two inertial measurement units are respectively fixed on the left and right ankles of the patient to be measured, the freezing index is calculated by windowed Fourier transform, the freezing threshold is calculated based on the freezing index during normal walking, and the freezing index and the freezing threshold are compared to complete the detection of freezing of gait. The experimental results show that the number of freezing of gait occurrences in Parkinson's patients is accurately detected, and it has high sensitivity and specificity, which can assist doctors to objectively assess the patient's condition.