Bionic Spider Web Flexible Strain Sensor Based on CF-L and Machine Learning.

At present, the preparation of laser-induced graphene (LIG) has become an important technology in sensor manufacturing. In the conventional preparation process, the CO2 laser is widely used; however, its experimental period is long and its efficiency needs to be improved. We propose an innovative strategy to improve the experimental efficiency. We use the machine learning method to accurately predict the preparation parameters of LIG, so as to optimize the experimental process. Different structures can lead to different sensor performances. The structure constructed by the CO2 laser is rough and has a large size, which can affect the performance of the sensor. Therefore, we propose for the first time an innovative method for intramembrane structure construction that combines the advantages of the CO2 laser and fiber laser (CF-L). With this CF-L method, we have successfully prepared a biomimetic, flexible strain sensor. This sensor not only maintains a high degree of sensitivity, but also has a more refined and optimized structure. The manufacturing process of the whole sensor is simple, economical, and durable and can be prepared in large quantities and can be used to detect the extension and bending of human joints.

Carbon coated Na3+xV2-xCux(PO4)3@C cathode for high-performance sodium ion batteries.

Na3V2(PO4)3 is considered as one of the most promising cathodes for sodium ion batteries owing to its fast Na+ diffusion, good structural stability and high working potential. However, its practical application is limited by its low intrinsic electronic conductivity. Herein, a carbon coated Cu2+-doped Na3V2(PO4)3 cathode was prepared. The carbon coating not only improve its apparent conductivity, but also inhibit crystal growth and prevent agglomeration of particles. Moreover, Cu2+ doping contributes to an enhanced intrinsic conductivity and decreased Na+ diffusion energy barrier, remarkably boosting its charge transfer kinetics. Based on the structure characterizations, electrochemical performances tests, charge transfer kinetics analyses and theoretical calculations, it's proved that such an elaborate design ensures the excellent rate performances (116.9 mA h g-1 at 0.1C; 92.6 mA h g-1 at 10C) and distinguished cycling lifespan (95.8 % retention after 300 cycles at 1C; 84.8 % retention after 3300 cycles at 10C). Besides, a two-phase reaction mechanism is also confirmed via in-situ XRD. This research is expected to promote the development of Na3V2(PO4)3-based sodium ion batteries with high energy/power density and excellent cycling lifespan.

Fabrication of multi-functional gelatin/deep eutectic solvent/polyacrylonitrile nanofiber membranes via electrospinning.

In this work, gelatin was dissolved in sodium acetate trihydrate/urea deep eutectic solvent (DES) and then mixed with polyacrylonitrile (PAN) spinning solution to prepare composite nanofiber membranes via electrospinning. The rheological properties of gelatin/DES (Gel/DES) solution and gelatin/DES/PAN (GDES/PAN) spinning solution were investigated. Besides, the water vapor transmittance rate, water contact angle, and antistatic and mechanical properties of GDES/PAN nanofiber membranes had also been evaluated and the composition and structure of GDES/PAN nanofiber membranes had also been characterized by SEM, EDS and FTIR further. Due to the introduction of DES components and gelatin, the composite nanofibers presented a smooth surface, small diameter, uniform distribution and good continuity. GDES/PAN nanofiber membranes also exhibited desirable breathable properties, hydrophilicity, antistatic properties and mechanical strength compared with the PAN nanofiber membrane. GDES/PAN nanofiber membranes would provide new opportunities for the application of gelatin and DES in the electrospinning field.

Accurate integrated position measurement system for mobile applications in GPS-denied coal mine.

The automatic positioning of underground mobile applications plays a crucial role in enabling intelligent coal mining. However, due to the diverse kinematics and dynamics of these applications, various positioning methods have been proposed to match different targets. Nonetheless, the accuracy and applicability of these methods still fall short of meeting the requirements for field applications. Based on the vibration characteristics of underground mobile devices, a multi-sensor fusion positioning system is developed to enhance the accuracy of positioning in long and narrow global positioning system denied (GPS-denied) underground coal mine roadways. The system combines inertial navigation (INS), odometer, and ultra wide band (UWB) technologies through extended Kalman filter (EKF) and unscented Kalman filter (UKF). This approach enables accurate positioning by recognizing target carrier vibrations and facilitating fast conversion between multi-sensor fusion modes. The proposed system is tested on both a small unmanned mine vehicle (UMV) and a large roadheader, demonstrating that UKF enhances stability for roadheaders with strong nonlinear vibrations while EKF is more suitable for flexible UMVs. Detailed results confirm that the proposed system achieves an accuracy level of 0.15 m, meeting most coal mine application requirements.

Palladium-Catalyzed Transient Chirality Transfer and Atroposelective C-H Functionalization to Access Quaternary Stereocenters.

Although palladium-catalyzed asymmetric C-H functionalization and Heck reactions represents one of the most important synthetic strategies for the construction of quaternary stereocenters, developing the enantioselective version of PdII -catalyzed carbopalladation-initiated cascade reactions still remains a formidable challenge. Herein, an unprecedent enantioselective [3+2] annulation of oxime ethers and alkynes has been developed, providing both spiro and nonspiro indenes bearing all-carbon quaternary stereocenters in good yields (up to 98 %) with excellent enantioselectivities (up to >99 % ee). This annulation is accomplished by merging the PdII -catalyzed atroposelective C-H activation/double carbopalladation and the transient axial-to-central chirality transfer process, constituting the first successful example of catalytic chirality transfer strategy involving axially chiral styrene intermediate.

3-Alkyl-2-pyridyl Directing Group-Enabled C2 Selective C-H Silylation of Indoles and Pyrroles via an Iridium Catalyst.

An iridium-catalyzed, directing group-enabled site selective intra- and intermolecular silylation of indoles and pyrroles with hydrosilanes has been developed under ligand-free conditions. Fine-tuning of the removable 3-alkyl-2-pyridyl directing group was found to be crucial for achieving high yields for C2-silylated indole and pyrrole products. Moreover, the scalability was demonstrated, and further transformations of the silylation products were achieved.

Atropisomers with Axial and Point Chirality: Synthesis and Applications.

Enantiopure atropisomers have become increasingly important in asymmetric synthesis and catalysis, pharmaceutical science, and material science since the discovery of inherent features of axial chirality originating from rotational restriction. Despite the advances made in this field to date, it remains highly desirable to construct structurally diverse atropisomers with potentially useful functions. We propose superposition to match axial and point chirality as a potentially useful strategy to access structurally complex and diverse building blocks for organic synthesis and pharmaceutical science because merging atropisomeric backbones with one or more extra chiral elements can topologically broaden three-dimensional environments to create complex scaffolds with multiple tunable parameters. Over the past decade, we have successfully implemented a strategic design for the superposition of axial and point chirality to develop a series of enantiopure atropisomers and have utilized the synergistic functions of these molecules to enhance chirality transfer in various catalytic asymmetric transformations.In this Account, we present several novel atropisomers with superposed axial and point chirality developed in our laboratory. In our studies, this superposition strategy was used to design and synthesize both biaryl and non-biaryl atropisomers from commercially available chiral sources. Consequently, these atropisomers were used to demonstrate the importance of the synergetic functions of axial and point chirality in specific enantioselective reactions. For example, aromatic amide-derived atropisomers, simplified as Xing-Phos arrays, were broadly employed in Ag-catalyzed [3 + 2] cycloaddition by a series of reactions of aldiminoesters with activated alkenes and imines, as well as being used as chiral solvating agents for the discrimination of optically active mandelic acid derivatives. Considering the powerful potential of non-biaryl atropisomers for asymmetric catalysis, we also explored the transition-metal-catalyzed enantioselective construction of a novel backbone of non-biaryl atropisomers (Ar-alkene, Ar-N axis) bearing both axial and point chirality for the design and synthesis of chiral ligands and functional molecules.The studies presented herein are expected to stimulate further research efforts on the development of functional atropisomers by superposition of matching axial and point chirality. In addition to tunable electron and stereohindrance effects, the synergy between matching chiral elements of axial/point chirality and functional groups is proven to be a special function that cannot be ignored for promoting reactivity and chirality-transfer efficiency in enantioselective synthesis. Consequently, our novel types of scaffolds with superposed axial and point chirality that are capable of versatile coordination with various metal catalysts in asymmetric catalysis highlight the power of the superposition of matching axial and point chirality for the construction of synthetically useful atropisomers.

Belief in a Just World and Mental Toughness in Adolescent Athletes: The Mediating Mechanism of Meaning in Life.

Mental toughness is an essential component of adolescent athletes' athletic careers and lives. Evidence supports the positive effect of belief in a just world on individual psychological development, but the relationship between belief in a just world and mental toughness of adolescents has not been tested. In order to determine the influencing factors of mental toughness and explore effective strategies for improving adolescent athletes' mental toughness, this study introduced just world and life meaning theories to explore the relationship between belief in a just world, meaning in life (search for meaning/presence of meaning), and mental toughness. Based on the data of 1,544 adolescent athletes from Yantai and Qingdao in Shandong Province, China, we tested a parallel mediation model that considered the search for meaning and presence of meaning as mediators. The results were predicted as follows: there is a significant positive correlation between belief in a just world and mental toughness, while the relationship between belief in a just world and mental toughness was partially mediated by the search for meaning and the presence of meaning in life. Furthermore, it is worth noting that the presence of meaning played a more influential role than the search for meaning. The results suggest that belief in a just world is connected to the mental toughness of adolescent athletes via the meaning in life. Therefore, maintaining and promoting the level of belief in a just world and enhancing the sense of meaning in life may be an effective strategy to develop the mental toughness of adolescent athletes. The findings of this study can help develop the mental toughness of adolescent athletes and help them maintain a high level of subjective and objective performance under the pressure of training and competition, providing practical guidance for coaches and administrators in the training of adolescent athletes.

Influencing factors and characterization methods of nanoparticles regulating amyloid aggregation.

Human disorders associated with amyloid aggregation, such as Alzheimer's disease and Parkinson's disease, afflict the lives of millions worldwide. When peptides and proteins in the body are converted to amyloids, which have a tendency to aggregate, the toxic oligomers produced during the aggregation process can trigger a range of diseases. Nanoparticles (NPs) have been found to possess surface effects that can modulate the amyloid aggregation process and they have potential application value in the treatment of diseases related to amyloid aggregation and fibrillary tangles. In this review, we discuss recent progress relating to studies of nanoparticles that regulate amyloid aggregation. The review focuses on the factors influencing this regulation, which are important as guidelines for the future design of NPs for the treatment of amyloid aggregation. We describe the characterization methods that have been utilized so far in such studies. This review provides research information and characterization methods for the rational design of NPs, which should result in therapeutic strategies for amyloid diseases.

Combined Dynamic Kinetic Resolution and C-H Functionalization for Facile Synthesis of Non-Biaryl-Atropisomer-Type Axially Chiral Organosilanes.

Although asymmetric C-H functionalization has been available for the synthesis of structurally diverse molecules, catalytic dynamic kinetic resolution (DKR) approaches to change racemic stereogenic axes remain synthetic challenges in this field. Here, a concise palladium-catalyzed DKR was combined with C-H functionalization involving olefination and alkynylation for the highly efficient synthesis of non-biaryl-atropisomer-type (NBA) axially chiral oragnosilanes. The chemistry proceeded through two different and distinct DKR: first, an atroposelective C-H olefination or alkynylation produced axially chiral vinylsilanes or alkynylsilanes as a new family of non-biaryl atropisomers (NBA), and second, the extension of this DKR strategy to twofold o,o'-C-H functionalization led to the multifunctional axially chiral organosilicon compounds with up to >99 % ee.

Surface-initiated PET-ATRP and mussel-inspired chemistry for surface engineering of MWCNTs and application in self-healing nanocomposite hydrogels.

A green strategy by integrating surface-initiated metal-free photoinduced electron transfer-atom transfer radical polymerization (PET-ATRP) with mussel-inspired polydopamine (PDA) chemistry, was used to fabricate multi-walled carbon nanotubes (MWCNTs)/poly(4-vinylpyridine) (P4VP) nanocomposites. Self-healing nanocomposite hydrogels were facilely designed with these nanocomposites through dynamic supramolecular interactions. Using mussel-inspired PDA chemistry from MWCNTs, nanocomposites (MWCNTs@PDA-P4VP) were successfully prepared by metal-free PET-ATRP with MWCNTs@PDA-Br as an initiator, rhodamine B as photocatalyst, 4-vinylpyridine (4VP) as monomer, respectively. Importantly, the obtained nanocomposite hydrogels had high mechanical strength (2.9 MPa), prior fracture strain (633.8%) and excellent self-healing property (90.6%). These methodologies will provide opportunities for the design of eco-functional materials or flexible biosensors.

Catalytic asymmetric cycloaddition of unsymmetrical EWG-activated alkenes to fully substituted pyrrolidines bearing three different carbonyl groups.

A unique 1,3-dipolar [3+2] cycloaddition of alkyl 4-oxo-4-arylbut-2-enoates bearing two different electron-withdrawing groups was completed by using the silver/(R)-DTBM-Segphos catalyst system, which gives the corresponding fully substituted pyrrolidines with four stereogenic centers in good yields and with excellent enantioselectivities (up to 98% ee).

PdCl2(CH3CN)2-catalyzed regioselective C-H olefinations of 2-amino biaryls with vinylsilanes as unactivated alkenes.

The first example of palladium-catalyzed chelation-assisted C-H olefination of 2-amino biaryls using readily available vinylsilanes as unactivated olefinating reagents has been developed, affording valuable arylated vinylsilane compounds in moderate to excellent yields and with exclusive (E)-selectivities.

Desymmetrization-Oriented Enantioselective Synthesis of Silicon-Stereogenic Silanes by Palladium-Catalyzed C-H Olefinations.

A palladium-catalyzed chelation-assisted enantioselective C-H olefination of symmetrically diaryl-substituted tetraorganosilicon derivatives was developed, enabling the generation of nitrogen-containing silicon-stereogenic tetraorganosilicon compounds with modest to good yields and good to excellent enantioselectivities (up to 95.5:4.5 e.r.). The Thorpe-Ingold effect exerted by the substituents on silicon was observed to have a profound influence on formation of olefinated products which were further converted into other relevant chiral organosilanes without the loss of enantiomeric purity, thus demonstrating the synthetic utility of the developed enantioselective olefination.

Enantioselective synthesis of axially chiral vinyl arenes through palladium-catalyzed C-H olefination.

A palladium-catalyzed ketoxime-chelation-assisted enantioselective C-H olefination of 2-arylcyclohex-2-enone oxime ether with a wide range of olefins as coupling partners was developed. Employing ketoxime ether as an efficient directing group, a variety of axially chiral vinyl arenes was synthesized by Pd(ii)-catalyzed C-H functionalization with excellent enantioselectivities (96 → 99% ee) under mild conditions.

Ligand-Controlled Inversion of Diastereo- and Enantioselectivity in Silver-Catalyzed Azomethine Ylide-Imine Cycloaddition of Glycine Aldimino Esters with Imines.

A highly diastereo- and enantioselective silver-catalyzed azomethine ylide-imine (AYI) cycloaddition reaction of glycine aldimino esters with imines was developed in which the Xing-Phos-controlled syn-selective or DTBM-Segphos-induced anti-selective AYI cycloaddition reaction could be applied to the synthesis of a variety of stereodivergent 1-alkyl-2,5-substituted imidazolidines with high yields and excellent enantioselectivities (up to 99% ee) as well as good diastereoselectivities (up to 99:1 dr) under mild reaction conditions.

Facile fabrication of CNTs@C@MoSe2@Se hybrids with amorphous structure for high performance anode in lithium-ion batteries.

Amorphous MoSe2 and Se anchored on amorphous carbon coated multiwalled carbon nanotubes (CNTs@C@MoSe2@Se) have been synthesized by a facile solvothermal strategy. The one dimensional CNTs@C@MoSe2@Se can effectively buffer the volume variation, prohibit the aggregation and facilitate electron and ion transport throughout the electrode. Furthermore, the combination of MoSe2 and Se also provides buffer spaces for the volumetric change during cycling. Thus, the obtained CNTs@C@MoSe2@Se hybrids display the enhanced cycle stability and excellent high rate capacity. The reversible capacity of 1010mAhg-1 can be achieved after 100 cycles at the current density of 0.1Ag-1. Even after 500 cycles, a reversible capacity of 508mAhg-1 is still retained at 5Ag-1.

Asymmetric Synthesis of Glutamic Acid Derivatives by Silver-Catalyzed Conjugate Addition-Elimination Reactions.

The enantioselective construction of a family of chiral glycine-derived aldimino esters is described. The asymmetric tandem conjugate addition-elimination procedure is characterized by its exceptional mild reaction conditions and features with an exquisite enantioselectivity profile using commercially available silver/DTBM-SegPhos catalyst, allowing for the facile preparation of a variety of substituted and chiral glutamic acid derivatives (up to 99% ee) bearing Schiff base in a straightforward manner.

Lewis-Base-Mediated Diastereoselective Silylations of Alcohols: Synthesis of Silicon-Stereogenic Dialkoxysilanes Controlled by Chiral Aryl BINMOLs.

In the past years, stereoselective functionalizations of hydroxyl groups of alcohol substrates with chlorosilanes leading to silyl ether formation have evolved from a functional-group protection to an enantioselective synthetic strategy. This work comprises a controlled desymmetrization of dichlorosilanes by using a family of structurally specific chiral diols, chiral 1,1'-binaphthalene-2-α-arylmethanol-2'-ol (Ar-BINMOL). This process led to the facile construction of silicon-stereogenic organosilicon compounds with high yields and good diastereoselectivities. In addition, the diasteroselective silylation of chiral diols might not only be of interest for the development of highly stereoselective nucleophilic silylation, but also shed light on the construction of novel chiral phosphine ligands bearing a silicon-stereogenic center.

Cs2CO3-Initiated Trifluoro-Methylation of Chalcones and Ketones for Practical Synthesis of Trifluoromethylated Tertiary Silyl Ethers.

It was found that 1,2-trifluoromethylation reactions of ketones, enones, and aldehydes were easily accomplished using the Prakash reagent in the presence of catalytic amounts of cesium carbonate, which represents an experimentally convenient, atom-economic process for this anionic trifluoromethylation of non-enolisable aldehydes and ketones.