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1.
Sensors (Basel) ; 24(7)2024 Apr 08.
Artículo en Inglés | MEDLINE | ID: mdl-38610589

RESUMEN

Functional electrical stimulation (FES) devices are widely employed for clinical treatment, rehabilitation, and sports training. However, existing FES devices are inadequate in terms of wearability and cannot recognize a user's intention to move or muscle fatigue. These issues impede the user's ability to incorporate FES devices into their daily life. In response to these issues, this paper introduces a novel wearable FES system based on customized textile electrodes. The system is driven by surface electromyography (sEMG) movement intention. A parallel structured deep learning model based on a wearable FES device is used, which enables the identification of both the type of motion and muscle fatigue status without being affected by electrical stimulation. Five subjects took part in an experiment to test the proposed system, and the results showed that our method achieved a high level of accuracy for lower limb motion recognition and muscle fatigue status detection. The preliminary results presented here prove the effectiveness of the novel wearable FES system in terms of recognizing lower limb motions and muscle fatigue status.


Asunto(s)
Fatiga Muscular , Dispositivos Electrónicos Vestibles , Humanos , Electromiografía , Estimulación Eléctrica , Extremidad Inferior
2.
Angew Chem Int Ed Engl ; 63(2): e202312465, 2024 Jan 08.
Artículo en Inglés | MEDLINE | ID: mdl-37997539

RESUMEN

Herein, we report that bulky alkylphosphines such as PtBu3 can switch the roles from actor to spectator ligands to promote the FeCl2 -catalyzed N-amidation reaction of arylamines with dioxazolones, giving hydrazides in high efficiency and chemoselectivity. Mechanistic studies indicated that the phosphine ligands could facilitate the decarboxylation of dioxazolones on the Fe center, and the hydrogen bonding interactions between the arylamines and the ligands on Fe nitrenoid intermediates might play a role in modulating the delicate interplay between the phosphine ligand, arylamine, and acyl nitrene N, favoring N-N coupling over N-P coupling. The new ligand-promoted N-amidation protocols offer a convenient way to access various challenging triazane compounds via double or sequential N-amidation of primary arylamines.

3.
Org Lett ; 26(1): 94-99, 2024 Jan 12.
Artículo en Inglés | MEDLINE | ID: mdl-38149595

RESUMEN

8-Aminoquinoline (AQ) has proven to be a highly effective bidentate directing group for palladium-catalyzed C-H functionalization reactions. However, enantiocontrol of AQ-directed C(sp3)-H functionalization reactions has been challenging. Herein, a new protocol is presented for the Pd-catalyzed enantioselective arylation of unactivated ß C(sp3)-H bonds of alkyl carboxamides with aryl iodides using a C5-iodinated 8-aminoquinolines (IQ) auxiliary in conjugation with a BINOL ligand. Additionally, a C5-aryl substituted 8-aminoquinoline auxiliary can facilitate enantioselective alkenylation and alkynylation of benzylic C(sp3)-H bonds of 3-arylpropanamides with the corresponding bromide reagents under similar conditions.

4.
ACS Appl Mater Interfaces ; 15(47): 55009-55021, 2023 Nov 29.
Artículo en Inglés | MEDLINE | ID: mdl-37922204

RESUMEN

The advancement of smart textiles has resulted in significant development in wearable textile sensors and offers novel interfaces to sense physical movements in daily life. Knitting, as a traditional textile fabrication method, is being used in promising ways to realize fully seamless fabrication and unobtrusive sensing in wearable textile applications. However, current flat-knitted sensors can sense strain only in the horizontal plane. This research presents a novel fully machine-knitted spacer piezoresistive sensor structure with a three-directional sensing ability that can detect both the pressure in the vertical direction and the strain in the warp/weft direction. Besides, it can sense the pressure under 1 kPa, which is critical in comfortable on-body interaction, one-piece integration, and wearable applications. Three sizes spacer-knitted sensors are evaluated in terms of their mechanical performance, stability cycles, and reaction to external factors such as sweat, laundering, etc. Then, the effect of material choice on sensor performance is evaluated and the rationale behind the use of different materials is summarized. Specifically, this research presents a detailed evaluation of the applications with both a single sensor and multiple sensor arrays for fine and gross motion sensing in several scenarios. The testing results demonstrate a fully machine-knitted piezoresistive sensor that can detect multidirectional motions (vertical, warp, and weft directions). In addition, this knitted sensor is scalable and can be facilely and seamlessly integrated into any garment piece. This universal knitted sensor structure could be made with a wide variety of materials for high sensitivity for multidirectional strain/pressure sensing, making it a high-compatibility sensor structure for wearable applications.

5.
Nat Commun ; 13(1): 6445, 2022 10 28.
Artículo en Inglés | MEDLINE | ID: mdl-36307408

RESUMEN

Sulfur-heteroatom bonds such as S-S and S-N are found in a variety of natural products and often play important roles in biological processes. Despite their widespread applications, the synthesis of sulfenamides, which feature S-N bonds that may be cleaved under mild conditions, remains underdeveloped. Here, we report a method for synthesis of N-acyl sulfenamides via copper-catalyzed nitrene-mediated S-amidation reaction of thiols with dioxazolones. This method is efficient, convenient, and broadly applicable. Moreover, the resulting N-acetyl sulfenamides are highly effective S-sulfenylation reagents for the synthesis of unsymmetrical disulfides under mild conditions. The S-sulfenylation protocol enables facile access to sterically demanding disulfides that are difficult to synthesize by other means.


Asunto(s)
Cobre , Compuestos de Sulfhidrilo , Compuestos de Sulfhidrilo/química , Cobre/química , Indicadores y Reactivos , Estructura Molecular , Catálisis , Disulfuros/química
6.
ACS Sens ; 7(4): 929-950, 2022 04 22.
Artículo en Inglés | MEDLINE | ID: mdl-35322661

RESUMEN

Textile-based sensors in the form of a wearable computing device that can be attached to or worn on the human body not only can transmit information but also can be used as a smart sensing device to access the mobile internet. These sensors represent a potential platform for the next generation of human-computer interfaces. The continuous emergence of new conductive materials is one of the driving forces for the development of textile sensors. Recently, a two-dimensional (2D) MXene material with excellent performance has received extensive attention due to its high conductivity, processability, and mechanical stability. In this paper, the synthesis of MXene materials, the fabrication of conductive textiles, the structural design of textile sensors, and the application of MXene-based textile sensors in the wearable field are reviewed. Furthermore, from the perspective of MXene preparation, wearability, stability, and evaluation standards, the difficulties and challenges of MXene-based textile sensors in the field of wearable applications are summarized and prospected. This review attempts to strengthen the connection between wearable smart textiles and MXene materials and promote the rapid development of wearable MXene-based textile sensors.


Asunto(s)
Textiles , Dispositivos Electrónicos Vestibles , Conductividad Eléctrica , Humanos
7.
Nat Chem ; 13(4): 378-385, 2021 04.
Artículo en Inglés | MEDLINE | ID: mdl-33753917

RESUMEN

N-N linkages are found in many natural compounds and endow fascinating structural and functional properties. In comparison to the myriad methods for the construction of C-N bonds, chemistry for N-N coupling, especially in an intermolecular fashion, remains underdeveloped. Here, we report a nitrene-mediated intermolecular N-N coupling of dioxazolones and arylamines under iridium or iron catalysis. These reactions offer a simple and efficient method for the synthesis of various hydrazides from readily available carboxylic acid and amine precursors. Although the Ir-catalysed conditions usually give higher N-N coupling yield than the Fe-catalysed conditions, the reactions of sterically more demanding dioxazolones derived from α-substituted carboxylic acids work much better under the Fe-catalysed conditions. Mechanistic studies revealed that the nitrogen atom of Ir acyl nitrene intermediates has strong electrophilicity and can undergo nucleophilic attack with arylamines with the assistance of Cl···HN hydrogen bonding to form the N-N bond with high efficiency and chemoselectivity.

8.
J Am Chem Soc ; 141(17): 7194-7201, 2019 05 01.
Artículo en Inglés | MEDLINE | ID: mdl-30978019

RESUMEN

While remarkable progress has been made over the past decade, new design strategies for chiral catalysts in enantioselective C(sp3)-H functionalization reactions are still highly desirable. In particular, the ability to use attractive noncovalent interactions for rate acceleration and enantiocontrol would significantly expand the current arsenal for asymmetric metal catalysis. Herein, we report the development of a highly enantioselective Ir(III)-catalyzed intramolecular C(sp3)-H amidation reaction of dioxazolone substrates for synthesis of optically enriched γ-lactams using a newly designed α-amino-acid-based chiral ligand. This Ir-catalyzed reaction proceeds with excellent efficiency and with outstanding enantioselectivity for both activated and unactivated alkyl C(sp3)-H bonds under very mild conditions. It offers the first general route for asymmetric synthesis of γ-alkyl γ-lactams. Water was found to be a unique cosolvent to achieve excellent enantioselectivity for γ-aryl lactam production. Mechanistic studies revealed that the ligands form a well-defined groove-type chiral pocket around the Ir center. The hydrophobic effect of this pocket allows facile stereocontrolled binding of substrates in polar or aqueous media. Instead of capitalizing on steric repulsions as in the conventional approaches, this new Ir catalyst operates through an unprecedented enantiocontrol mechanism for intramolecular nitrenoid C-H insertion featuring multiple attractive noncovalent interactions.

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