Materials Advances最新文献

In this work, for the first time, a fast and novel assembly of morpholinium-based zwitterionic materials (ZMs) is reported, with benzosultone 2 as the key component in the synthesis of zwitterionic smart materials. The developed materials exhibited LCST phase separation in water, and their structural engineering enabled the development of novel ZMs with attractive T_c values (ZM 2d, T_c = 15 °C) for proof-of-concept applications in biomolecules. Furthermore, to evaluate the potential health risks of the newly developed ZMs, experiments were conducted on both human normal gastric epithelial cells and human normal colon epithelial cells. Neither the thermo-responsive ZMs, such as ZM 2d, nor its untethered, non-thermo-responsive ionic salt IS 1, caused a decrease in cell viability in these two cell lines at concentrations as high as 2000 μM. To the best of our knowledge, this is the first report on morpholinium-based, small-molecule ZMs as non-toxic smart materials, with their temperature-triggered miscibility and immiscibility with water being fully reversible.

Urinary catheters are commonly used in medical practice to drain and monitor urine of patients. However, urinary catheterisation is associated with the risk of developing catheter-associated urinary tract infections (CAUTIs), which can result in life-threatening sepsis that requires antibiotics for treatment. Using the layer-by-layer (LbL) technique, we assembled a multilayer catheter comprising nine quadruple layers (9QL) of alginate, chlorhexidine (CHX), alginate and poly(β-amino ester) (PBAE) built upon an amino-functionalised silicone. The prepared catheter materials were tested for pre-packaged storage conditions and sterilisation techniques. The daily release of CHX was measured at pH 7.4 and pH 5 and simulated urine at 37 °C, which was used to determine the antimicrobial affect. CHX release was detected for a minimum of 14 days in PBS (pH 7.4), pH 5 release media, and simulated urine for the samples tested against storage conditions and sterilisation techniques. Incubation of the prepared material with bacterial cultures for 24 hours restricted bacterial growth compared to incubation with the standard material. The minimum inhibition concentration of CHX for clinically isolated urinary tract infection (UTI) bacterial strains was in the range of 19.4–77.4 µM, at which the released CHX could indirectly prevent bacterial growth for up to 14 days. Based on the daily CHX release from the samples, the hydrolysis of PBAE at pH 5 was gradual, resulting in a greater number of days of preventing bacterial growth, followed by pH 7.4 and then simulated urine. To the best of our knowledge, this is the first report on the use of PBAE in association with a urinary catheter material for the release of an antimicrobial drug.

Cobalt-based catalysts containing Ce, La and Al were prepared via solution combustion synthesis (SCS) and used in dry reforming of methane (DRM). Combustion temperature for the highest active 20Co–10La–20Al catalyst measured during the combustion process was 861 °C, explaining the formation of CoAl₂O₄, which was active for DRM in the present work. No graphite structure was defined from the XRD pattern and TPO profiles of the spent Co–La–Al catalyst, while other catalysts contained this phase. In addition, only 10 wt% of carbon was identified in Co–La–Al, according to CHNS results. All catalysts were well dispersed, and the metal particle size varied between 19 and 28 nm. TPR analyses showed that doping of rare-earth metals leads to easier reduction due to oxygen vacancies, which suppress coking. The highest CH₄ transformation rate and space-time yield of hydrogen were observed for CoLaAl, which exhibited a metal particle size of 23 nm, giving the lowest carbon content in the spent catalysts after temperature cycling experiments in DRM. This catalyst containing metallic cobalt and an active CoAl₂O₄ spinel demonstrated stable formation of hydrogen and CO during 50 h time-on-stream. The spinel phase was, however, decomposed during the DRM. The best catalyst also contained a perovskite-type mixed oxide, LaCo_xAl_1−xO₃, which was already formed during synthesis through an SCS method. This phase was not, however, stable in long-term experiments.

Multielement combinations either as high entropy alloys or as nanocomposites are highly effective electrocatalysts for key reactions such as the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER). Both these reactions are crucial for generation of green hydrogen from water splitting. In this work we demonstrate the concept of using an electrical double layer to modulate the formation of these multielement catalysts. A one-pot, room temperature synthesis method is used to prepare dual functional HER and OER catalysts. The nanocomposite catalyst (NAC) forms chain-like structures composed of Au nanoparticle (AuNP) cores with a shell structure of Pt, Ni, Cu, Co and V that form a combination of metallic and amorphous composite heterostructures on a nanoscale, tailored using the electrical double layer. The NAC achieves low HER and OER overpotentials in 0.1 M KOH with fast kinetics for both reactions.

Aqueous sodium batteries and capacitors offer a low-cost and sustainable alternative to lithium-based energy storage systems, with their performance crucially dependant on the choice of electrode materials. Among the candidates commonly used in sodium-ion devices, various phase modifications of presodiated manganese oxide are considered promising. In this work, we synthesized biphasic (orthorhombic/monoclinic) NaMnO₂ using a cost-effective sol–gel technique and investigated its performance as an electrode material for aqueous sodium electrochemical systems. The performance was evaluated through cyclic voltammetry and galvanostatic charge–discharge measurements. The results demonstrated that NaMnO₂ electrodes were highly suitable for high-power energy devices, exhibiting a specific capacity of 103 mA h g⁻¹ and high capacity retention, even under high current conditions (82% capacity retention as the current increased from 1C to 20C). The superior electrochemical performance, especially under high discharge current conditions, was attributed to the optimal combination of different pseudocapacitive mechanisms associated with the biphasic monoclinic-orthorhombic phase structure, which ensured both high capacity and stability during cycling, as well as the morphology of the samples. These results paved the way for the development of high-power, stable, and cost-effective aqueous sodium-ion storage devices.

Dental caries is a biofilm-mediated dynamic disease associated with imbalance in teeth mineralization. In this study, a facile and dual-functional hybrid polydopamine@proanthocyanidin (PDA@PC) coating was designed to inhibit cariogenic biofilm formation and remineralize demineralized dental hard tissues. PDA@PC exhibited excellent antibiofilm ability with a lower cariogenic bacterial biofilm biomass (0.15 ± 0.03 OD_595nm) than that (1.45 ± 0.16 OD_595nm) exhibited by the control group. In addition, a dense mineral layer was observed on the surface of demineralized enamel. The microhardness of etched enamel with the PDA@PC coating reached 329.28 ± 10.16 HV after incubation with artificial saliva, which was similar to the healthy enamel (368.5 ± 17.18 HV). Furthermore, the in vivo rat dental caries model showed that the PDA@PC coating effectively slowed down the progression of caries, with only superficial demineralization and low dental caries scores. The total score was 3–4 times lower than that of the control group. The successful construction of the dual-functional hybrid PDA@PC coating provides a novel approach for dental caries treatment.

This work systematically investigates the stability and electronic and thermoelectric characteristics of newly discovered 2D Janus monolayers BiYZ (Y ≠ Z = Te, Se and S) according to the first-principles theory. Janus BiYZ monolayers are stable based on the AIMD simulations, positive phonon spectra plots and the evaluation of elastic strain tensor. These monolayers show a high carrier mobility (∼10³ cm² V⁻¹ s⁻¹) and an indirect bandgap nature. The Janus monolayers BiTeSe, BiTeS and BiSeS show an ultralow lattice thermal conductivity of 0.04 W m⁻¹ K⁻¹, 0.20 W m⁻¹ K⁻¹ and 0.02 W m⁻¹ K⁻¹, respectively, at room temperature. Low lattice thermal conductivity is obtained due to a small phonon group velocity, high Grüneisen parameter, small phonon relaxation time and significantly reduced phonon transport. The maximum ZT values at 500 K reach up to 0.97, 0.60 and 1.78 for BiTeSe, BiSeS, and BiTeS monolayers, respectively. Our results suggest Janus BiYZ monolayers to be promising thermoelectric candidates due to their superior thermal and electrical transport characteristics and subsequent strong thermoelectric performance.

Despite significant progress in the diagnosis of acute myocardial infarction (AMI), its morbidity and mortality rates are still high, indicating the necessity of developing easy-to-use diagnostic tests with timely and reliable point-of-care (POC) detection capability. Aiming to address this need, we introduce here for the first time the development of a fluorescence lateral flow immunoassay (LFIA) based on antibody labeled ZIF-8@BSA Au/Ag nanoclusters for the quantitative detection of cardiac troponin I (cTnI) as the major biomarker of AMI. A portable IoT-enabled optoelectronic reader was also fabricated to quantify the fluorescence signals of the developed LFIA, enabling easy, precise, and smart on-site quantitative analysis of cTnI. The developed smart LFIA demonstrated desirable assay performance for cTn1 in a linear concentration range of 10 pg mL⁻¹ to 150 pg mL⁻¹ with an appropriate sensitivity (with a detection limit of 9 pg mL⁻¹) compared to the enzyme-linked immunosorbent assay (ELISA) and other reported assays. The fascinating results of our developed smart LFIA for easy, rapid (∼10 min), and highly sensitive and specific detection of cTnI in serum and whole blood samples make it a very promising biosensor capable of being exploited for smart, reliable, and early diagnosis of AMI at the POC.

The constant demands for the better performance of consumer electronics have led to shorter usage lifespans, resulting in a significant increase in electronic waste (e-waste). Developing electronics that can be easily broken down and recycled is a promising strategy to tackle this growing e-waste challenge. Herein, we report a biocompatible and degradable organic thin film transistor (OTFT) utilizing a biocompatible semiconductor with a biodegradable dielectric and substrate. We present the first OTFT based on bispentafluorophenoxy silicon phthalocyanine (F₁₀-SiPc) integrated with a polyvinyl alcohol (PVA) and poly(caprolactone) (PCL) bilayer as the dielectric, leading to a drop in threshold voltage (V_T) from 12.7 V to −0.97 V, versus using SiO₂ while maintaining similar mobility values. We demonstrate the importance of the annealing temperature on PLA substrate roughness and gate electrode surface chemistry for the fabrication of working OTFT devices. We then demonstrate that the bendable OTFTs could easily be dissolved in phosphate buffer saline (PBS) solution at room temperature in less than a month, which is a crucial aspect for ensuring eco-sustainability in electronic devices. Finally, incubation of the degradation products with fibroblastic cells did not affect cell viability, suggesting that they are non-cytotoxic. These cytocompatible disintegrable OTFTs with low operating voltages will find applications in bioresorbable electronics and constitute a step towards minimizing e-waste.

Sensor research based on biometal performance and health parameter detection attracts significant global interest in the biosensing community. In this study, an electrochemical biosensor has been developed for the detection of lactic acid (LA) in artificial saliva, and in this context, the screen-printed electrode was functionalized using a composite of silver nanoparticles (AgNPs) and silver nanoparticles–polyaniline (AgNPs–PANI). The cyclic voltammetry responses were recorded for non-enzymatic LA sensing. In this process, the electro-polymerization method has been used to generate a film of Ag–PANI on a screen-printed electrode (SPE). Several analytical techniques, including Fourier transform infrared spectroscopy (FTIR), ultraviolet-visible spectroscopy (UV-visible), field emission scanning electron microscopy (FESEM), atomic force microscopy (AFM), and RAMAN spectroscopy, were employed to analyze the film of AgNPs and AgNPs–PANI that was used to change the surface morphology of the screen-printed electrode (SPE). The various important parameters of effectiveness viz., limit of detection (LOD) and limit of quantification (LOQ) for AgNPs–SPE and AgNPs–PANI–SPE were investigated and were found to be in the range of 5.3 mM, 16 mM and 2.5 mM, 7.4 mM, respectively, in PBS solution. Meanwhile, for the artificial saliva samples, the sensitivity of the AgNPs–PANI–SPE was obtained up to 0.00176 mA μM⁻¹ cm⁻² with an LOD of 0.76 mM. Furthermore, DFT results are used to examine the physical and electrical properties of the prepared functional films. The computing results show the functionalization of carbon with AgNP and AgNP–PANI, enabling a stable and reactive structure. The current research offers a non-enzymatic technique for precisely detecting LA biomolecules for medical applications.