Cross-linked

交联
  • 文章类型: Journal Article
    为了追求高效的钙钛矿太阳能电池,spiro-OMeTAD已经证明了创纪录的功率转换效率(PCE),然而,稳定问题仍然是制约其商业发展的瓶颈之一。在这项研究中,我们成功合成了一种新型的自聚合螺型界面分子,被称为v-spiro。与螺-OMeTAD相比,线性排列的分子表现出较强的分子间相互作用和较高的固有空穴迁移率。重要的是,v-spiro中的乙烯基能够原位聚合,在钙钛矿薄膜表面形成聚合物保护层,这证明在抑制水分降解和离子迁移方面非常有效。利用这些优势,聚-v-spiro基器件实现了24.54%的突出效率,具有1.173V的增强开路电压和81.11%的填充因子,由于缺陷密度降低,能级对齐和高效的界面孔提取。此外,未封装器件的运行稳定性显著增强,即使在约60%湿度下2000小时或在连续AM1.5G阳光照射下1250小时后,初始效率仍保持在90%以上。这项工作提出了一种全面的方法,通过创新的界面设计在PSC中实现高效率和长期稳定性。
    In the pursuit of highly efficient perovskite solar cells, spiro-OMeTAD has demonstrated recorded power conversion efficiencies (PCEs), however, the stability issue remains one of the bottlenecks constraining its commercial development. In this study, we successfully synthesize a novel self-polymerized spiro-type interfacial molecule, termed v-spiro. The linearly arranged molecule exhibits stronger intermolecular interactions and higher intrinsic hole mobility compared to spiro-OMeTAD. Importantly, the vinyl groups in v-spiro enable in situ polymerization, forming a polymeric protective layer on the perovskite film surface, which proves highly effective in suppressing moisture degradation and ion migration. Utilizing these advantages, poly-v-spiro-based device achieves an outstanding efficiency of 24.54 %, with an enhanced open-circuit voltage of 1.173 V and a fill factor of 81.11 %, owing to the reduced defect density, energy level alignment and efficient interfacial hole extraction. Furthermore, the operational stability of unencapsulated devices is significantly enhanced, maintaining initial efficiencies above 90 % even after 2000 hours under approximately 60 % humidity or 1250 hours under continuous AM 1.5G sunlight exposure. This work presents a comprehensive approach to achieving both high efficiency and long-term stability in PSCs through innovative interfacial design.
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  • 文章类型: Journal Article
    由混合组分制成的复合结构的合理制造显示出提高超级电容器能量密度的巨大潜力。在这里,通过分步方法制备了精细的分层MOF衍生的NiCo2S4@Mo掺杂的Co-LDH阵列混合电极。通过利用NiCo2S4纳米线的均匀阵列作为核心和MOF衍生的多孔壳的协同效应,NiCo2S4@Mo掺杂的Co-LDH混合电极在1Ag-1时显示出3049.3Fg-1的特殊比电容。即使在20Ag-1的较高电流密度下,电容仍保持在2458.8Fg-1。此外,电极表现出显著的循环稳定性,在10,000次循环后,初始电容的91%保持在10g-1。此外,基于NiCo2S4@Mo掺杂的Co-LDH电极的制造的非对称超级电容器(ASC)在835.6Wkg-1的功率密度下实现了97.5Whkg-1的令人印象深刻的能量密度。这些发现为混合结构电极的开发提供了一种有希望的方法,实现高能量密度的非对称超级电容器。
    The rational fabrication of composite structures made of mixed components has shown great potential for boosting the energy density of supercapacitors. Herein, an elaborate hierarchical MOF-derived NiCo2S4@Mo-doped Co-LDH arrays hybrid electrode was fabricated through a step-wise method. By leveraging the synergistic effects of a uniform array of NiCo2S4 nanowires as the core and an MOF-derived porous shell, the NiCo2S4@Mo-doped Co-LDH hybrid electrode demonstrates an exceptional specific capacitance of 3049.3 F g-1 at 1 A g-1. Even at a higher current density of 20 A g-1, the capacitance remains high at 2458.8 F g-1. Moreover, the electrode exhibits remarkable cycling stability, with 91% of the initial capacitance maintained after 10,000 cycles at 10 A g-1. Additionally, the as-fabricated asymmetric supercapacitor (ASC) based on the NiCo2S4@Mo-doped Co-LDH electrode achieves an impressive energy density of 97.5 Wh kg-1 at a power density of 835.6 W kg-1. These findings provide a promising approach for the development of hybrid-structured electrodes, enabling the realization of high-energy-density asymmetric supercapacitors.
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  • 文章类型: Journal Article
    开发具有低细胞毒性和高抗微生物活性的涂层材料已被认为是预防医疗器械相关感染的有效方法。在这项研究中,合成了马来酸酐三元共聚物(PPTM)并共价连接到硅橡胶(SR)表面。所形成的涂层可以通过三元共聚物的悬挂硅氧烷基团的自缩合进一步交联(SPM)。在500个弯曲循环和在去离子水中浸泡7天之后,没有观察到SPM的裂纹或分层。用SPM涂覆后,导管的滑动摩擦力降低了50%。SPM涂层不添加任何额外的抗菌试剂可以杀死99.99%的金黄色葡萄球菌和大肠杆菌,并且还可以显着降低细菌覆盖率,而当SPM的马来酸酐基团被胺化或水解时,涂层没有抗微生物活性。重复消毒试验结果表明,SPM涂层SR在5个循环内能保持87.3%的杀菌活性。此外,在共培养36小时后,SPM涂层仅对L929细胞产生轻微的毒性作用(>85%的活力),这优于与抗菌肽E6缀合的胺化SPM的涂层。含有马来酸酐单元的三元共聚物作为抗植入物感染的柔性和耐久涂层具有巨大潜力。
    Developing coating materials with low cytotoxicity and high antimicrobial activity has been recognized as an effective way to prevent medical device-associated infections. In this study, a maleic anhydride terpolymer (PPTM) is synthesized and covalently attached to silicone rubber (SR) surface. The formed coating can be further cross-linked (SPM) through the self-condensation of pendent siloxane groups of terpolymer. No crack or delamination of SPM was observed after 500 cycles of bending and 7 day immersion in deionized water. The sliding friction force of a catheter was reduced by 50% after coating with SPM. The SPM coating without adding any extra antibacterial reagents can kill 99.99% of Staphylococcus aureus and Escherichia coli and also significantly reduce bacterial coverage, while the coating displayed no antimicrobial activity when maleic anhydride groups of SPM were aminated or hydrolyzed. The results of the repeated disinfection tests showed that the SR coated with SPM could maintain 87.3% bactericidal activity within 5 cycles. Furthermore, the SPM coating only imparted slight toxic effect (>85% viability) on L929 cells after 36 h of coculture, which is superior to the coating of aminated SPM conjugated with the antimicrobial peptide E6. The terpolymer containing maleic anhydride units have great potential as a flexible and durable coating against implant infections.
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  • 文章类型: Journal Article
    通过非溶剂诱导的相分离和表面涂层制备了高蛋白质保留聚醚砜(PES)膜,表现出增强的血液相容性和抗氧化应激性能。通过单宁酸(TA)和α-硫辛酸(α-LA)在膜表面构建交联网络,将毛孔控制在合理的尺寸。肝素样基团在膜表面的富集,通过“疏水相互作用”和“点击反应”实现,赋予抗凝血性质;来自TA的大量酚羟基的存在和α-LA的引入允许改性膜干预氧化应激。血液相容性特征包括血浆复钙时间(PRT),活化部分凝血活酶时间(APTT),凝血酶原时间(PT),凝血酶时间(TT)和溶血率(HR)。此外,测试了DPPHABTS自由基清除能力以评估其抗氧化性能。结果表明,改性膜具有出色的蛋白质保留率(99.3%)以及渗透性。此外,PRT延长至341.7s,DPPH·清除能力达到0.74µmol·cm-2。该膜易于制备并具有优异的综合性能。这项工作为制造具有可控孔径的血液透析膜提供了简单而简便的策略。
    A high protein retention polyethersulfone (PES) membrane was prepared by nonsolvent-induced phase separation and surface coating, which exhibited enhanced hemocompatibility and antioxidant stress performance. The cross-linked network was constructed by tannic acid (TA) and alpha-lipoic acid (α-LA) on the surface of the membrane, which controlled the pores to a reasonable size. The enrichment of heparin-like groups on the membrane surface, implemented by \"hydrophobic interaction\" and \"click reaction\", confers anticoagulant properties; the presence of a large number of phenolic hydroxyl groups from TA and the introduction of α-LA allows the modified membranes to intervene in oxidative stress. The hemocompatibility characterizations included plasma recalcification time (PRT), activated partial thromboplastin time (APTT), prothrombin time (PT), thrombin time (TT) and hemolysis rate (HR). Additionally, the DPPH ABTS radical scavenging capacity was tested to evaluate the antioxidant performance. The results show that the modified membrane presents an outstanding protein retention rate (99.3%) along with permeability. In addition, the PRT is prolonged to 341.7 s, and the DPPH• scavenging ability reaches 0.74 µmol•cm-2. The membranes can be easily prepared and present excellent comprehensive performance. This work provides a simple and facile strategy for the fabrication of hemodialysis membranes with controllable pore sizes.
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  • 文章类型: Journal Article
    壳聚糖是一种丰富的天然多糖,含有大量的氨基和羟基。由于其低毒性,在生物医学应用中具有巨大的潜力,生物可降解性和低成本。在这里,通过六氯环三磷腈(HCCP)的亲核取代,设计并合成了一种新型的壳聚糖基荧光共聚物(WS-CS-TPA),水溶性壳聚糖(WS-CS)和聚集诱导发射(AIE)荧光原(AIEgen)三苯胺衍生物(TPA-NH2)。在超声波处理下,1.16gTPA-NH2和1.1gWS-CS可以在室温下通过0.7gHCCP缀合。所得共聚物表现出两亲性,可组装成粒径约为100nm的纳米颗粒。自组装后,TPA-NH2聚集在核心,因此,在水性介质中表现出极好的AIE特征,具有强烈的绿色荧光发射。另一方面,亲水性WS-CS被包覆在纳米粒子表面,赋予其高的水分散性。初步的生物学实验结果表明,WS-CS-TPA可以被细胞内化并表现出低的细胞毒性,表明它们在生物成像和细胞内药物递送方面的巨大潜力。
    Chitosan is an abundant natural polysaccharide that contains a lot of amino and hydroxyl groups. It possesses great potential for biomedical applications owing to its low toxicity, biodegradability and low cost. Herein, a novel chitosan-based fluorescent copolymer (WS-CS-TPA) was designed and synthesized via nucleophilic substitution of hexachlorocyclotriphosphazene (HCCP), water-soluble chitosan (WS-CS) and an aggregation-induced emission (AIE) fluorogen (AIEgen) triphenylamine derivative (TPA-NH2). Under ultrasonic treatment, 1.16 g TPA-NH2 and 1.1 g WS-CS can be conjugated by 0.7 g HCCP at room temperature. The obtained copolymer shows amphiphilic property and could assemble into nanoparticles with size about 100 nm. After self-assembly, TPA-NH2 was aggregated in the core, thus exhibiting superb AIE feature with intense green fluorescence emission in aqueous media. On the other hand, hydrophilic WS-CS was coated on the surface of nanoparticles and endowed their high water dispersibility. Results from preliminary biological assays suggested that WS-CS-TPA can be internalized by cells and exhibits low cytotoxicity, suggesting their great potential for biological imaging and intracellular drug delivery.
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  • 文章类型: Journal Article
    Despite the high specific capacity of silicon as a promising anode material for the next-generation high-capacity Li-ion batteries (LIBs), its practical applications are impeded by the rapid capacity decay during cycling. To tackle the issue, herein, a binder-grafting strategy is proposed to construct a covalently cross-linked binder [carboxymethyl cellulose/phytic acid (CMC/PA)], which builds a robust branched network with more contact points, allowing stronger bonds with Si nanoparticles by hydrogen bonding. Benefitting from the enhanced mechanical reliability, the resulting Si-CMC/PA electrodes exhibit a high reversible capacity with improved long-term cycling stability. Moreover, an assembled full cell consisting of the as-obtained Si-CMC/PA anode and commercial LiFePO4 cathode also exhibits excellent cycling performance (120.4 mA h g-1 at 1 C for over 100 cycles with 88.4% capacity retention). In situ transmission electron microscopy was employed to visualize the binding effect of CMC/PA, which, unlike the conventional CMC binder, can effectively prevent the lithiated Si anodes from cracking. Furthermore, the combined ex situ microscopy and X-ray photoelectron spectroscopy analysis unveils the origin of the superior Li-ion storage performance of the Si-CMC/PA electrode, which arises from its excellent structural integrity and the stabilized solid-electrolyte interphase films during cycling. This work presents a facile and efficient binder-engineering strategy for significantly improving the performance of Si anodes for next-generation LIBs.
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  • 文章类型: Journal Article
    硅(Si)被认为是下一代锂离子电池最有前途的负极材料,由于其较高的理论能力,安全,和高自然丰度。然而,硅阳极的商业应用受到其巨大体积膨胀的阻碍,导电性差,库仑效率低。对于阳极制造,粘合剂起着粘合硅材料的重要作用,电流收集器,和导电剂,粘结剂结构会显著影响机械耐久性,附着力,离子/电子电导率,和硅阳极的固体电解质界面(SEI)稳定性。此外,许多交联粘合剂有效地减轻硅纳米尺寸甚至微米尺寸的阳极材料的体积膨胀,同时保持阳极完整性和稳定的电化学性能。这个迷你评论根据其结构全面总结了各种粘合剂,包括线性,分支,三维(3D)交联,导电聚合物,和其他混合粘合剂。各种粘结剂结构影响硅阳极性能的机理,的局限性,并讨论了不同混合粘结剂的发展前景。这篇小型评论可以帮助设计混合聚合物粘合剂,并促进具有高电化学活性和长期稳定性的硅基阳极的实际应用。
    Silicon (Si) has been counted as the most promising anode material for next-generation lithium-ion batteries, owing to its high theoretical specific capacity, safety, and high natural abundance. However, the commercial application of silicon anodes is hindered by its huge volume expansions, poor conductivity, and low coulombic efficiency. For the anode manufacture, binders play an important role of binding silicon materials, current collectors, and conductive agents, and the binder structure can significantly affect the mechanical durability, adhesion, ionic/electronic conductivities, and solid electrolyte interface (SEI) stability of the silicon anodes. Moreover, many cross-linked binders are effective in alleviating the volume expansions of silicon nanosized even microsized anodic materials along with maintaining the anode integrity and stable electrochemical performances. This mini review comprehensively summarizes various binders based on their structures, including the linear, branched, three-dimensional (3D) cross-linked, conductive polymer, and other hybrid binders. The mechanisms how various binder structures influence the performances of the silicon anodes, the limitations, and prospects of different hybrid binders are also discussed. This mini review can help in designing hybrid polymer binders and facilitating the practical application of silicon-based anodes with high electrochemical activity and long-term stability.
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  • 文章类型: Journal Article
    Based on carboxylated multi-walled carbon nanotubes (MWCNTs-COOH), a MWCNTs/PVDF conductive membrane was prepared by a vacuum filtration cross-linking method. The surface compositions and morphology of conductive membranes were studied by X-ray photoelectron spectroscopy and high-resolution field emission scanning electron microscopy, respectively. The effects of cross-linked polymeric polyvinyl alcohol (PVA) on the conductive membrane properties such as the porosity, pore size distribution, pure water flux, conductivity, hydrophilicity, stability and antifouling properties were investigated. Results showed that the addition of PVA to the MWCNTs/PVDF conductive membrane decreased the pure water flux, porosity and the conductivity. However, the hydrophilicity of the modified MWCNTs/PVDF conductive membrane was greatly improved, and the contact angle of pure water was reduced from 70.18° to 25.48° with the addition of PVA contents from 0 wt% to 0.05 wt%. Meanwhile, the conductive membranes with higher content had a relatively higher stability. It was found that the conductive functional layer of the conductive membrane had an average mass loss rate of 1.22% in the 30 min ultrasonic oscillation experiment. The tensile intensity and break elongation ratio of the conductive membrane are improved by the addition of PVA, and the durability of the conductive membrane with PVA was superior to that without PVA added. The electric assisted anti-fouling experiments of modified conductive membrane indicated that compared with the condition without electric field, the average flux attenuation of the conductive membrane was reduced by 11.2%, and the membrane flux recovery rate reached 97.05%. Moreover, the addition of PVA could accelerate the clean of the conductive membranes.
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  • 文章类型: Journal Article
    The unique two-dimensional structure and chemical properties of graphene oxide (GO) provide a convenient method for preparing novel membranes. In this study, GO membranes were prepared through filtration by a pressure-assisted self-assembly method involving the cross-linking of three diamine monomers on a polyethersulfone (PES) support. The different small molecular diamines, ethylenediamine, butanediamine, and p-phenylenediamine, were introduced as cross-linking agents to investigate the effect of diamine on the properties of GO membranes. The hydrophobic substances ibuprofen, gemfibrozil, and triclosan were selected as target pharmaceuticals and personal care products (PPCPs). The adsorption and molecular sieving activities of PPCPs by cross-linked GO membranes at a pH of 3 were investigated. The permeate water was analyzed for dissolved organic carbon, ultraviolet absorption at 254 nm, molecular weight distribution, and fluorescence excitation-emission matrices. The results showed that the removal of hydrophobic PPCPs by GO membranes was mainly due to their adsorption and molecular sieving activities. Adsorption was mainly determined by the hydrophilic and hydrophobic properties of the membranes and PPCPs. The interception effect was mainly determined by the interlayer spacing between the GO membranes and the molecular weight and steric hindrance of the PPCPs. A smaller spacing of the GO membrane layers resulted in greater steric hindrance and a higher removal rate.
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  • 文章类型: Journal Article
    生物膜感染负责至少65%的人类细菌感染。这些生物膜对常规抗生素是难处理的,导致慢性感染和伤口不愈合。植物衍生的抗生素(植物化学物质)是具有抗微生物特性的有前途的替代抗微生物治疗。然而,它们在水性介质中的溶解性差限制了它们在治疗生物膜感染中的应用。将植物化学物质掺入交联聚合物纳米复合材料“海绵”中,用于处理细菌生物膜。结果表明,包封低logP植物化学物质有效地消除了生物膜,同时表现出对哺乳动物成纤维细胞的低细胞毒性。
    Biofilm infections are responsible for at least 65% of human bacterial infections. These biofilms are refractory to conventional antibiotics, leading to chronic infections and nonhealing wounds. Plant-derived antibiotics (phytochemicals) are promising alternative antimicrobial treatments featuring antimicrobial properties. However, their poor solubility in aqueous media limits their application in treating biofilm infections. Phytochemicals were incorporated into cross-linked polymer nanocomposite \"sponges\" for the treatment of bacterial biofilms. The results indicated encapsulating low log P phytochemicals effectively eliminated biofilms while demonstrating low cytotoxicity against mammalian fibroblast cells.
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