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1.
Int J Biol Macromol ; 268(Pt 2): 131972, 2024 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-38697436

RESUMO

Photochromic hydrogels have promising prospects in areas such as wearable device, information encryption technology, optoelectronic display technology, and electronic skin. However, there are strict requirements for the properties of photochromic hydrogels in practical engineering applications, especially in some extreme application environments. The preparation of photochromic hydrogels with high transparency, high toughness, fast response, colour reversibility, excellent electrical conductivity, and anti-freezing property remains a challenge. In this study, a novel photochromic hydrogel (PAAm/SA/NaCl-Mo7) was prepared by loading ammonium molybdate (Mo7) and sodium chloride (NaCl) into a dual-network hydrogel of polyacrylamide (PAAm) and sodium alginate (SA) using a simple one-pot method. PAAm/SA/NaCl-Mo7 hydrogel has excellent conductivity (175.9 S/cm), water retention capacity and anti-freezing properties, which can work normally at a low temperature of -28.4 °C. In addition, the prepared PAAm/SA/NaCl-Mo7 hydrogel exhibits fast response (<15 s), high transparency (>70 %), good toughness (maximum elongation up to 1500 %), good cyclic compression properties at high compressive strains (60 %), good biocompatibility (78.5 %), stable reversible discolouration and excellent sensing properties, which can be used for photoelectric display, information storage and motion monitoring. This work provides a new inspiration for the development of flexible electronic skin devices.

3.
Gels ; 10(4)2024 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-38667677

RESUMO

Hydrogels with excellent flexibility, conductivity, and controllable mechanical properties are the current research hotspots in the field of biomaterial sensors. However, it is difficult for hydrogel sensors to regain their original function after being damaged, which limits their practical applications. Herein, a composite hydrogel (named SPBC) of poly(vinyl alcohol) (PVA)/sodium alginate (SA)/cellulose nanofibers (CNFs)/sodium borate tetrahydrate was synthesized, which has good self-healing, electrical conductivity, and excellent mechanical properties. The SPBC0.3 hydrogel demonstrates rapid self-healing (<30 s) and achieves mechanical properties of 33.92 kPa. Additionally, it exhibits high tensile strain performance (4000%). The abundant internal ions and functional groups of SPBC hydrogels provide support for the good electrical conductivity (0.62 S/cm) and electrical response properties. In addition, the SPBC hydrogel can be attached to surfaces such as fingers and wrists to monitor human movements in real time, and its good rheological property supports three-dimensional (3D) printing molding methods. In summary, this study successfully prepared a self-healing, conductive, printable, and mechanically superior SPBC hydrogel. Its suitability for 3D-printing personalized fabrication and outstanding sensor properties makes it a useful reference for hydrogels in wearable devices and human motion monitoring.

4.
Org Lett ; 26(15): 2982-2986, 2024 Apr 19.
Artigo em Inglês | MEDLINE | ID: mdl-38602341

RESUMO

Pd(OAc)2/Nixantphos or CoI2/Nixantphos catalyzed allylic substitutions with weakly acidic C(sp)3-H bonds of azaarylmethylamines are described. This method facilitates access to various kinds of heteroaryl rings containing homoallylamines (39 examples, 30-98% yields) with excellent functional group tolerance and diastereoselectivity. Compared with the Pd/Nixantphos complex, the Co/Nixantphos catalysis could obtain the cyclic products with good to excellent diastereoselectivities. Importantly, the CoI2/(R,R)-Me-Duphos catalyzed reactions exhibit moderate enantioselectivity. Additionally, the scalability of this transformation is successfully demonstrated.

5.
Polymers (Basel) ; 16(8)2024 Apr 12.
Artigo em Inglês | MEDLINE | ID: mdl-38675005

RESUMO

The flexibility and adaptability of soft robots enable them to perform various tasks in changing environments, such as flower picking, fruit harvesting, in vivo targeted treatment, and information feedback. However, these fulfilled functions are discrepant, based on the varied working environments, driving methods, and materials. To further understand the working principle and research emphasis of soft robots, this paper summarized the current research status of soft robots from the aspects of actuating methods (e.g., humidity, temperature, PH, electricity, pressure, magnetic field, light, biological, and hybrid drive), materials (like hydrogels, shape-memory materials, and other flexible materials) and application areas (camouflage, medical devices, electrical equipment, and grippers, etc.). Finally, we provided some opinions on the technical difficulties and challenges of soft robots to comprehensively comprehend soft robots, lucubrate their applications, and improve the quality of our lives.

6.
J Agric Food Chem ; 72(14): 7727-7734, 2024 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-38530940

RESUMO

To discover novel transketolase (TKL, EC 2.2.1.1) inhibitors with potential herbicidal applications, a series of pyrazole acyl thiourea derivatives were designed based on a previously obtained pyrazolamide acyl lead compound, employing a scaffold hopping strategy. The compounds were synthesized, their structures were characterized, and they were evaluated for herbicidal activities. The results indicate that 7a exhibited exceptional herbicidal activity against Digitaria sanguinalis and Amaranthus retroflexus at a dosage of 90 g ai/ha, using the foliar spray method in a greenhouse. This performance is comparable to that of commercial products, such as nicosulfuron and mesotrione. Moreover, 7a showed moderate growth inhibitory activity against the young root and stem of A. retroflexus at 200 mg/L in the small cup method, similar to that of nicosulfuron and mesotrione. Subsequent mode-of-action verification experiments revealed that 7a and 7e inhibited Setaria viridis TKL (SvTKL) enzyme activity, with IC50 values of 0.740 and 0.474 mg/L, respectively. Furthermore, they exhibited inhibitory effects on the Brassica napus acetohydroxyacid synthase enzyme activity. Molecular docking predicted potential interactions between these (7a and 7e) and SvTKL. A greenhouse experiment demonstrated that 7a exhibited favorable crop safety at 150 g ai/ha. Therefore, 7a is a promising herbicidal candidate that is worthy of further development.


Assuntos
Cicloexanonas , Herbicidas , Piridinas , Compostos de Sulfonilureia , Herbicidas/farmacologia , Herbicidas/química , Relação Estrutura-Atividade , Simulação de Acoplamento Molecular , Esqueleto , Pirazóis/farmacologia , Pirazóis/química , Tioureia
7.
J Agric Food Chem ; 72(7): 3334-3341, 2024 Feb 21.
Artigo em Inglês | MEDLINE | ID: mdl-38346337

RESUMO

The design and synthesis of new herbicidal active compounds based on a new target are of great significance for the development of new herbicides. Transketolase (TK) plays a key role in the Calvin cycle of plant photosynthesis and has been confirmed as a potential candidate target to develop and discover new herbicides. To obtain compounds with ultraefficient targeting of TK, a series of pyrazole amide derivatives were designed and synthesized through structural optimization for lead compound 4u based on TK as the new target. The bioassay results showed that compounds 6ba and 6bj displayed a highly inhibitory effect with the root inhibition of about 90% against Digitaria sanguinalis (DS) and 80% against Amaranthus retroflexus (AR) and Setaria viridis (SV) by the small cup method, which was better than the positive control mesotrione and nicosulfuron. Furthermore, compounds 6ba and 6bj exhibited an excellent inhibitory effect with the inhibition of about 80% (against DS) and over 80% (against SV) at the dosage of 150 g of active ingredient/ha by the foliar spray method. The TK enzyme activity inhibition test showed that the inhibition effect of target compounds against TK was consistent with the results of herbicidal activities. Also, molecular docking analysis showed that compounds 6ba and 6bj went deep into the active cavity of TK, bound to TK by a strong interaction, and might act on the enzyme TK. Above of all, compounds 6ba and 6bj are promising herbicide lead compounds targeting TK. Hence, they could be developed into more efficient herbicides by further structural optimization.


Assuntos
Herbicidas , Herbicidas/química , Relação Estrutura-Atividade , Transcetolase , Amidas , Simulação de Acoplamento Molecular , Pirazóis/farmacologia , Pirazóis/química , Inibidores Enzimáticos/farmacologia
8.
Int J Biol Macromol ; 259(Pt 2): 129201, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38191110

RESUMO

Medical stents, artificial teeth, and grafts are just some of the many applications for additive manufacturing techniques like bio-degradable polylactic acid 3D printing. However, there are drawbacks associated with fused filament fabrication-fabricated objects, including poor surface quality, insufficient mechanical strength, and a lengthy construction time for even a relatively small object. Thus, this study aims to identify the finest polylactic acid 3D printing parameters to maximize print quality while minimizing energy use, print time, flexural and tensile strengths, average surface roughness, and print time, respectively. Specifically, the infill density, printing speed, and layer thickness are all variables that were selected. A full-central-composite design generated 20 samples to test the prediction models' experimental procedures. Validation trial tests were used to show that the experimental findings agreed with the predictions, and analysis of variance was used to verify the importance of the performance characteristics (ANOVA). At layer thickness = 0.26 mm, infill density = 84 %, and print speed = 68.87 mm/s, the following optimized values were measured for PLA: flexural strength = 70.1 MPa, tensile strength = 39.2 MPa, minimum surface roughness = 7.8 µm, print time = 47 min, and print energy = 0.18 kwh. Firms and clinicians may benefit from utilizing the developed, model to better predict the required surface characteristic for various aspects afore trials.


Assuntos
Citoesqueleto , Poliésteres , Fenômenos Físicos , Impressão Tridimensional
9.
Org Lett ; 25(51): 9153-9157, 2023 Dec 29.
Artigo em Inglês | MEDLINE | ID: mdl-38096429

RESUMO

A nickel-catalyzed cross-electrophile coupling of aryl iodides with α-bromo sulfoxide to access a diverse array of aryl benzyl sulfoxides has been discovered. These reactions occurred under mild conditions with excellent functional group tolerance so that optically enriched sulfoxides could be coupled with aryl iodides, generating corresponding sulfoxides with excellent stereochemical integrity. Furthermore, the scalability of this transformation was demonstrated. Initial mechanistic studies revealed that the reaction undergoes a radical pathway.

10.
Chem Commun (Camb) ; 59(89): 13355-13358, 2023 Nov 07.
Artigo em Inglês | MEDLINE | ID: mdl-37873615

RESUMO

The first dual nickel/photoredox-catalyzed enantioselective reductive cross-coupling of racemic α-chloro thioesters with aryl iodides has been developed. This strategy avoids the need for organometallic reagents or stoichiometric metal reductants. This reaction could tolerate a wide range of substrate scope with excellent reactivity and high enantioselectivities (up to 91% ee) to access a variety of chiral α-aryl thioesters. The synthetic utility of the corresponding α-aryl thioesters is demonstrated. Furthermore, we explored the mechanism of such an enantioselective radical cross-coupling process.

11.
Org Lett ; 25(41): 7557-7561, 2023 Oct 20.
Artigo em Inglês | MEDLINE | ID: mdl-37818792

RESUMO

A tandem Madelung indole synthesis by the reaction of methyl benzoate and N-methyl-o-toluidine has been discovered. The combination of LiN(SiMe3)2 with CsF is the key factor, which secures the high efficiency of such tandem transformations. Simply combining methyl benzoate, N-methyl-o-toluidine LiN(SiMe3)2, and CsF generated a diverse array of N-methyl-2-phenylindoles (31 examples, 50-90% yields). Furthermore, the scalability and the poststructural modifications of this indole synthesis were demonstrated.

13.
ACS Biomater Sci Eng ; 9(6): 3032-3057, 2023 06 12.
Artigo em Inglês | MEDLINE | ID: mdl-37264613

RESUMO

In recent years, bioactive ceramic bone scaffolds have drawn remarkable attention as an alternative method for treating and repairing bone defects. Vat photopolymerization (VP) is a promising additive manufacturing (AM) technique that enables the efficient and accurate fabrication of bioactive ceramic bone scaffolds. This review systematically reviews the research progress of VP-printed bioactive ceramic bone scaffolds. First, a summary and comparison of commonly used bioactive ceramics and different VP techniques are provided. This is followed by a detailed introduction to the preparation of ceramic suspensions and optimization of printing and heat treatment processes. The mechanical strength and biological performance of the VP-printed bioactive ceramic scaffolds are then discussed. Finally, current challenges and future research directions in this field are highlighted.


Assuntos
Osso e Ossos , Alicerces Teciduais , Cerâmica/uso terapêutico
14.
J Org Chem ; 88(11): 7362-7372, 2023 Jun 02.
Artigo em Inglês | MEDLINE | ID: mdl-37213086

RESUMO

The deprotonation of allylbenzene was successfully demonstrated with a catalytic alkali amide base (NaN(SiMe3)2). The deprotonated allyl anion could be trapped by in situ generated N-(trimethylsilyl) aldimines to provide value-added homoallylic amines (39 examples, 68-98% yields) in a one-pot manner with excellent liner selectivity. Compared with the previously reported method for the synthesis of homoallylic amines, this method does not need to use the preinstalled protection groups on the imines, which need to be removed after the reaction to obtain the N-H free homoallylic amine derivatives.

15.
Materials (Basel) ; 16(9)2023 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-37176273

RESUMO

Professionals in industries are making progress in creating predictive techniques for evaluating critical characteristics and reactions of engineered materials. The objective of this investigation is to determine the optimal settings for a 3D printer made of acrylonitrile butadiene styrene (ABS) in terms of its conflicting responses (flexural strength (FS), tensile strength (TS), average surface roughness (Ra), print time (T), and energy consumption (E)). Layer thickness (LT), printing speed (PS), and infill density (ID) are all quantifiable characteristics that were chosen. For the experimental methods of the prediction models, twenty samples were created using a full central composite design (CCD). The models were verified by proving that the experimental results were consistent with the predictions using validation trial tests, and the significance of the performance parameters was confirmed using analysis of variance (ANOVA). The most crucial element in obtaining the desired Ra and T was LT, whereas ID was the most crucial in attaining the desired mechanical characteristics. Numerical multi-objective optimization was used to achieve the following parameters: LT = 0.27 mm, ID = 84 percent, and PS = 51.1 mm/s; FS = 58.01 MPa; TS = 35.8 MPa; lowest Ra = 8.01 m; lowest T = 58 min; and E = 0.21 kwh. Manufacturers and practitioners may profit from using the produced numerically optimized model to forecast the necessary surface quality for different aspects before undertaking trials.

16.
Gels ; 9(4)2023 Mar 23.
Artigo em Inglês | MEDLINE | ID: mdl-37102875

RESUMO

Hydrogels and hydrophilic polymer networks play an important role in biomedical engineering due to their good biocompatibility, biodegradability, hydrophilicity, and mechanical properties, similarly to some soft tissues [...].

17.
J Agric Food Chem ; 71(13): 5136-5142, 2023 Apr 05.
Artigo em Inglês | MEDLINE | ID: mdl-36972477

RESUMO

4-Hydroxyphenylpyruvate dioxygenase (EC 1.13.11.27; HPPD) represents a potential target for novel herbicide development. To discover the more promising HPPD inhibitor, we designed and synthesized a series of bis-5-cyclopropylisoxazole-4-carboxamides with different linkers using a multitarget pesticide design strategy. Among them, compounds b9 and b10 displayed excellent herbicidal activities versus Digitaria sanguinalis (DS) and Amaranthus retroflexus (AR) with the inhibition of about 90% at the concentration of 100 mg/L in vitro, which was better than that of isoxaflutole (IFT). Furthermore, compounds b9 and b10 displayed the best inhibitory effect versus DS and AR with the inhibition of about 90 and 85% at 90 g (ai)/ha in the greenhouse, respectively. The structure-activity relationship study showed that the flexible linker (6 carbon atoms) is responsible for increasing their herbicidal activity. The molecular docking analyses showed that compounds b9 and b10 could more closely bind to the active site of HPPD and thus exhibited a better inhibitory effect. Altogether, these results indicated that compounds b9 and b10 could be used as potential herbicide candidates targeting HPPD.


Assuntos
4-Hidroxifenilpiruvato Dioxigenase , Amaranthus , Herbicidas , 4-Hidroxifenilpiruvato Dioxigenase/química , Inibidores Enzimáticos/farmacologia , Inibidores Enzimáticos/química , Herbicidas/farmacologia , Herbicidas/química , Simulação de Acoplamento Molecular , Estrutura Molecular , Relação Estrutura-Atividade , Isoxazóis/química , Isoxazóis/farmacologia
18.
Gels ; 9(2)2023 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-36826325

RESUMO

The use of flexible, self-healing conductive hydrogels as a type of typical electronic skin with the function of transmitting sensory signals has attracted wide attention in the field of biomaterials. In this study, composite hydrogels based on polyvinyl alcohol (PVA), gelatin (GEL), oxidized sodium alginate (OSA), graphene oxide (GO), and single-walled carbon nanotubes (SWNTs) were successfully prepared. The hydrogen and imine bonding of the composite hydrogels gives them excellent self-healing properties. Their self-healing properties restore 68% of their breaking strength and over 95% of their electrical conductivity. The addition of GO and SWNTs enables the PGO-GS hydrogels to achieve a compressive modulus and conductivity of 42.2 kPa and 29.6 mS/m, which is 8.2 times and 1.5 times that of pure PGO, respectively. Furthermore, the PGO-GS hydrogels can produce profound feedback signals in response to deformation caused by external forces and human movements such as finger flexion and speech. In addition, the PGO-GS hydrogels exhibit superior biocompatibility compared to PGO. All of these results indicate that the PGO-GS hydrogels have great potential with respect to future applications in the field of electronic skin.

19.
J Hazard Mater ; 443(Pt B): 130265, 2023 02 05.
Artigo em Inglês | MEDLINE | ID: mdl-36327847

RESUMO

Herbicide residues in the environment threaten high-quality agriculture and human health. Consequently, in situ remediation of herbicide contamination is vital. We synthesized a novel self-catalyzed nanozyme, ultrasmall (2-3 nm) copper peroxide nanodots modified by citric acid (CP@CA) for this purpose, which can break down into H2O2 and Cu2+ in water or soil. Ubiquitous glutathione reduces Cu2+ into Cu+, which promotes the decomposition of H2O2 into •OH through a Fenton-like reaction under mild acid conditions created by the presence of citric acid. The generated •OH efficiently degrade nicosulfuron in water and soil, and the maximum degradation efficiency could be achieved at 97.58% in water at 56 min. The possible degradation mechanisms of nicosulfuron were proposed through the 25 intermediates detected. The overall ecotoxicity of the nicosulfuron system was significantly reduced after CP@CA treatment. Furthermore, CP@CA had little impact on active components of soil bacterial community. Moreover, CP@CA nanozyme could effectively remove seven other sulfonylurea herbicides from the water. In this paper, a high-efficiency method for herbicide degradation was proposed, which provides a new reference for the in situ remediation of herbicide pollution.


Assuntos
Herbicidas , Humanos , Herbicidas/metabolismo , Cobre/toxicidade , Ácido Cítrico , Peróxido de Hidrogênio/metabolismo , Peróxidos , Compostos de Sulfonilureia/toxicidade , Compostos de Sulfonilureia/metabolismo , Solo/química , Água
20.
J Org Chem ; 87(24): 16567-16577, 2022 12 16.
Artigo em Inglês | MEDLINE | ID: mdl-36455282

RESUMO

The nickel-catalyzed cross-electrophile coupling of 1,2,3-benzotriazin-4(3H)-ones with aryl bromides to generate a diverse array of ortho-arylated benzamide derivatives has been developed. The reaction displayed good functional group tolerance with Zn as the reductant. The key to this transformation is the ring opening of benzotriazinones, which undergo a denitrogenative process to obtain various benzamide derivatives (29 examples, 42-93% yield). The scalability of this transformation was demonstrated.


Assuntos
Brometos , Níquel , Catálise , Benzamidas
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