Stable Radicals with Protective Umbrellas Integrated on the Surface of 2D Layered Materials

Radicals are closely related to human life and health and have been widely used in biology, chemistry, functional materials, etc. However, the high reactivity, disorder, and short half-lives limit their wide applications. Therefore, it remains a great challenge to prepare stable and ordered radicals. Herein, radicals are prepared with protective umbrellas (diethylmethyleneamine, DEMA) that are integrated on the surface of 2D layered materials to isolate water and oxygen and enhance the stability of radicals. Taking 2D black phosphorus (BP) as an example: triethylamine reacts with dichloromethane to form quaternary ammonium salts with further Hoffmann elimination to produce DEMA radicals that could react with one electron of a lone pair electrons in P on the surface of BP to produce P radicals, which shows a prolonged half-life of 21 days at room temperature. First-principle calculations and electron paramagnetic resonance fitting confirm that the steric hindrance constructed by dense DEMA passivation layer acts as a protective umbrella and the 2D coupling of P radicals and other P atoms in 2D BP plane to enhance the stability and strong superexchange interaction of P radicals. Furthermore, it is a general strategy to produce stable radicals integrated on the 2D plane.     

地铁车辆空气制动管路保压试验的改进方案

分析了地铁车辆空气制动管路组装完毕后的保压试验操作过程,识别了其中的问题项点,提出了有针对性的优化改进方案,使保压试验结果准确可靠.     

Structural insights into peptide self-assembly using photo-induced crosslinking experiments and discontinuous molecular dynamics

Determining the structure of the (oligomeric) intermediates that form during the self-assembly of amyloidogenic peptides is challenging because of their heterogeneous and dynamic nature. Thus, there is need for methodology to analyze the underlying molecular structure of these transient species. In this work, a combination of fluorescence quenching, photo-induced crosslinking (PIC) and molecular dynamics simulation was used to study the assembly of a synthetic amyloid-forming peptide, Aβ_16-22. A PIC amino acid containing a trifluormethyldiazirine (TFMD) group—Fmoc(TFMD)Phe—was incorporated into the sequence (Aβ*_16–22). Electrospray ionization ion-mobility spectrometry mass-spectrometry (ESI-IMS-MS) analysis of the PIC products confirmed that Aβ*_16–22 forms assemblies with the monomers arranged as anti-parallel, in-register β-strands at all time points during the aggregation assay. The assembly process was also monitored separately using fluorescence quenching to profile the fibril assembly reaction. The molecular picture resulting from discontinuous molecule dynamics simulations showed that Aβ_16-22 assembles through a single-step nucleation into a β-sheet fibril in agreement with these experimental observations. This study provides detailed structural insights into the Aβ_16-22 self-assembly processes, paving the way to explore the self-assembly mechanism of larger, more complex peptides, including those whose aggregation is responsible for human disease.     

Flash joining of alumina ceramics under a small current density

The ceramic joining using electric field (E-field) has garnered significant research attention due to the decreased joining barrier and enhanced reliability. However, the underlying mechanism of E-field assisted joining remains unclear. Herein, we report the rapid joining of alumina ceramics using a small current. Moreover, the E-field is applied in both perpendicular and parallel directions to the faying surfaces, demonstrating a significant difference in terms of joint strength. These results indicate that the E-field generates defects and promotes the joining process by facilitating ionic diffusion.     

Negative thermal quenching CsPbBr3 glass-ceramic based on intrinsic radiation and vacancy defect co-induced dual-emission

Halide perovskite glass-ceramic has recently moved into the center of the attention of perovskite research due to their potential for temperature sensing. However, quantum dots glass-ceramic with excellent luminescence performance still needs to be combined with rare-earth (RE) ions to accurately measure temperature. In this work, a novel non-RE doped dual-emission (460 nm and 512 nm) CsPbBr₃ quantum dots was obtained in telluride glass via the friction crystallization method, where 512 nm was derived from intrinsic luminescence of quantum dots, and 460 nm was originated from thermally induced bromine vacancy, which can be used for temperature sensing. Fluorescence intensity ratio results indicate that the relative sensitivity of dual-emission could reach 5.6 % K^?1 at 323 K. The discovery of non-RE doped CsPbBr₃ QDs glass-ceramic with negative thermal quenching uncovers a new optional sensing glass material that surpass traditional RE-doped QDs glass by their tunability and sensitivity.     

无黏土相盐水储层钻开液体系构建及其抗污染性能评价

采用NaCl/KCl/HCOONa复配欠饱和盐水作为钻开液的基础液相,自研的聚合物VIS-B作为流型调节剂,可酸溶的改性淀粉STA作为体系的降失水剂,Dua及Jqw作为暂堵材料,构建了一套无黏土相钻开液体系。该体系在密度1.10~1.28 g/cm^3间稳定可调,抗温可达130℃,具有较高的低剪切速率黏度和较好的润滑性能,且能有效抵抗各类储层污染物的污染,满足了Missan油田不同储层段的作业需求。     

High-Throughput Screening for Phase-Change Memory Materials

Phase change memory (PCM) is an emerging non-volatile data storage technology concerned by the semiconductor industry. To improve the performances, previous efforts have mainly focused on partially replacing or doping elements in the flagship Ge-Sb-Te (GST) alloy based on experimental “trial-and-error” methods. Here, the current largest scale PCM materials searching is reported, starting with 124 515 candidate materials, using a rational high-throughput screening strategy consisting of criteria related to PCM characteristics. In the results, there are 158 candidates screened for PCM materials, of which ≈68% are not employed. By further analyses, including cohesive energy, bond angle analyses, and Born effective charge, there are 52 materials with properties similar to the GST system, including Ge₂Bi₂Te₅, GeAs₄Te₇, GeAs₂Te₄, so on and other candidates that have not been reported, such as TlBiTe₂, TlSbTe₂, CdPb₃Se₄, etc. Compared with GST, materials with close cohesive energy include AgBiTe₂, TlSbTe₂, As₂Te₃, TlBiTe₂, etc., indicating possible low power consumption. Through further melt-quenching molecular dynamic calculation and structural/electronic analyses, Ge₂Bi₂Te₅, CdPb₃Se₄, MnBi₂Te₄, and TlBiTe₂ are found suitable for optical/electrical PCM applications, which further verifies the effectiveness of this strategy. The present study will accelerate the exploration and development of advanced PCM materials for current and future big-data applications.     

Lithiation MXene Derivative Skeletons for Wide-Temperature Lithium Metal Anodes

Lithium (Li) metal, as an appealing candidate for the next-generation of high-energy-density batteries, is plagued by its safety issue mainly caused by uncontrolled dendrite growth and infinite volume expansion. Developing new materials that can improve the performance of Li-metal anode is one of the urgent tasks. Herein, a new MXene derivative containing pure rutile TiO₂ and N-doped carbon prepared by heat-treating MXene under a mixing gas, exhibiting high chemical activity in molten Li, is reported. The lithiation MXene derivative with a hybrid of LiTiO₂-Li₃N-C and Li offers outstanding electrochemical properties. The symmetrical cell assembling lithiation MXene derivative hybrid anode exhibits an ultra-long cycle lifespan of 2000 h with an overpotential of ≈30 mV at 1 mA cm⁻², which overwhelms Li-based anodes reported so far. Additionally, long-term operations of 34, 350, and 500 h at 10 mA cm⁻² can be achieved in symmetrical cells at temperatures of −10, 25, and 50 °C, respectively. Both experimental tests and density functional theory calculations confirm that the LiTiO₂-Li₃N-C skeleton serves as a promising host for Li infusion by alleviating volume variation. Simultaneously, the superlithiophilic interphase of Li₃N guides Li deposition along the LiTiO₂-Li₃N-C skeleton to avoid dendrite growth.     

Solution-Synthesized Multifunctional Janus Nanotree Microswimmer

Synthetic active matters are perfect model systems for non-equilibrium thermodynamics and of great potential for novel biomedical and environmental applications. However, most applications are limited by the complicated and low-yield preparation, while a scalable synthesis for highly functional microswimmers is highly desired. In this paper, an all-solution synthesis method is developed where the gold-loaded titania-silica nanotree can be produced as a multi-functional self-propulsion microswimmer. By applying light, heat, and electric field, the Janus nanotree demonstrated multi-mode self-propulsion, including photochemical self-electrophoresis by UV and visible light radiation, thermophoresis by near-infrared light radiation, and induced-charge electrophoresis under AC electric field. Due to the scalable synthesis, the Janus nanotree is further demonstrated as a high-efficiency, low-cost, active adsorbent for water decontamination, where the toxic mercury ions can be reclaimed with enhanced efficiency.