Well-ordered Structure Research Articles

In-situ gelation of fibrin gel encapsulating platelet-rich plasma-derived exosomes promotes rotator cuff healing

Although platelet-rich plasma-derived exosomes (PRP-Exos) hold significant repair potential, their efficacy in treating rotator cuff tear (RCT) remains unknown. In light of the potential for clinical translation of fibrin gel and PRP-Exos, we evaluated their combined impact on RCT healing and explored suitable gel implantation techniques. In vitro experiments demonstrated that PRP-Exos effectively enhanced key phenotypes changes in tendon stem/progenitor cells. Multi-modality imaging, including conventional ultrasound, shear wave elastography ultrasound, and micro-computed tomography, and histopathological assessments were performed to collectively evaluate the regenerative effects on RCT. The regenerated tendons exhibited a well-ordered structure, while bone and cartilage regeneration were significantly improved. PRP-Exos participated in the healing process of RCT. In-situ gelation of fibrin gel-encapsulated PRP-Exos at the bone-tendon interface during surgery proved to be a feasible gel implantation method that benefits the healing outcome. Comprehensive multi-modality postoperative evaluations were necessary, providing a reliable foundation for post-injury repair.

Directional and Orderly Arranged Ni0.9Mn0.1(OH)2 Enables the Synthesis of Single-Crystal Ni-Rich Co-Free LiNi0.9Mn0.1O2 with Enhanced Internal Structural Stability.

In this paper, the effect of the structure characteristics of the precursor on the electrochemical properties of a single-crystal cobalt-free high-nickel LiNi0.9Mn0.1O2 cathode is systematically studied. Precursors with different morphologies are synthesized by adjusting the coprecipitation reaction conditions. The results of SEM and XRD show that with the increase in the orderly stacking arrangement of internal primary nanosheets of Ni0.9Mn0.1(OH)2, the exposed active {010} planes at the surface increase. The prepared cathode materials finally inherit the structural features of the precursor, and the single-crystal Co-free Ni-rich LiNi0.9Mn0.1O2 cathode with highly exposed active {010} planes shows a well-ordered crystal structure and low Li+/Ni2+ cation mixing. The characterization results reveal that the high percentage of {010} planes will improve the Li+ transportation kinetics, decrease electrochemical impedance, and significantly alleviate the accumulation of rock-salt phases. Therefore, the material with this structure shows good electrochemical performance.

Mesoporous Silica MCM-41 from Fly Ash as a Support of Bimetallic Cu/Mn Catalysts for Toluene Combustion.

The main outcome of this research was to demonstrate the opportunity to obtain a stable and well-ordered structure of MCM-41 synthesized from fly ash. A series of bimetallic (Cu/Mn) catalysts supported at MCM-41 were prepared via grinding method and investigated in catalytic toluene combustion reaction to show the material's potential application. It was proved, that the Cu/Mn ratio had a crucial effect on the catalytic activity of prepared materials. The best catalytic performance was achieved with sample Cu/Mn(2.5/2.5), for which the temperature of 50% toluene conversion was found to be 300 °C. This value remains in line with the literature reports, for which comparable catalytic activity was attained for 3-fold higher metal loadings. Time-on-stream experiment proved the thermal stability of the investigated catalyst Cu/Mn(2.5/2.5). The obtained results bring a valuable background in the field of fly ash utilization, where fly ash-derived MCM-41 can be considered as efficient and stable support for dispersion of active phase for catalyst preparation.

Sensing of heavy metal Pb2+ ions in water utilizing the photonic structure of highly controlled hexagonal TiON/TiO2 nanotubes

The detection of heavy metals in water, especially Pb2+ ions, is important due to their severe hazardous effects. To address this issue, a highly controlled hexagonal TiON/TiO2 heterostructure has been synthesized in this study. The fabrication process involved the utilization of atomic layer deposition and direct current sputtering techniques to deposit TiO2 and TiON layers onto a porous Al2O3 membrane used as a template. The resulting heterostructure exhibits a well-ordered hollow tube structure with a diameter of 345 nm and a length of 1.2 µm. The electrochemical sensing of Pb2+ ions in water is carried out using a cyclic voltammetry technique under both light and dark conditions. The concentration range for the Pb2+ ions ranges from 10–5 to 10–1 M. The sensitivity values obtained for the sensor are 1.0 × 10–6 in dark conditions and 1.0 × 10–4 in light conditions. The remarkable enhancement in sensitivity under light illumination can be attributed to the increased activity and electron transfer facilitated by the presence of light. The sensor demonstrates excellent reproducibility, highlighting its reliability and consistency. These findings suggest that the proposed sensor holds great promise for the detection of Pb2+ ions in water, thereby facilitating environmental monitoring, water quality assessment, and safety regulation across various industries. Furthermore, the eco-friendly and straightforward preparation techniques employed in its fabrication provide a significant advantage for practical and scalable implementation.

Enhancing the Inhibition of Corneal Neovascularization Efficacy by Self-Assembled into Supramolecular Hydrogel of Anti-Angiogenic Peptide.

Corneal neovascularization (CNV) is a common eye disease that leads to blindness. New treatment strategies are urgently needed due to the limitations of current treatment methods. We report the synthesis of peptide Nap-FFEEPCAIWF ( Comp.3 ) via chemical conjugation of Nap-FFEE ( Comp.2 ) to antiangiogenic peptide PCAIWF (Comp.1). Comp.3 self-assembled into a hydrogel ( gel of 3 ) composed of nanofibers, which enhanced the antiangiogenic function of the epitope. We developed a novel peptide with an amphiphilic framework, Comp.3 , which could self-assemble into a supramolecular hydrogel with a well-ordered nanofiber structure. The nanofibers exhibited good biocompatibility with corneal epithelial cells, presenting a promising strategy to enhance the efficacy of free peptide-based drugs in the treatment of ocular vascular diseases, such as CNV and other angiogenesis-related diseases. Nap-FFEEPCAIWF nanofibers provide an alternative approach to enhancing the therapeutic efficiency of free peptide-based drugs against ocular vascular diseases.

Beyond acid treatment of PEDOT:PSS: decoding mechanisms of electrical conductivity enhancement

Coupling the acid post-treatment and hot-pressing processes can exponentially improve the electrical conductivity of PEDOT:PSS (3360 S cm−1) by providing a densely packed and well-ordered structure of PEDOT lamella along the edge-on direction.

Covalent Organic Frameworks for the Purification of Recombinant Enzymes and Heterogeneous Biocatalysis.

Recombinant enzymes have gained prominence due to their diverse functionalities and specificity and are often a greener alternative in biocatalysis. This context makes purifying recombinant enzymes from host cells and other impurities crucial. The primary goal is to isolate the pure enzyme of interest and ensure its stability under ambient conditions. Covalent organic frameworks (COFs), renowned for their well-ordered structure and permeability, offer a promising approach for purifying histidine-tagged (His-tagged) enzymes. Furthermore, immobilizing enzymes within COFs represents a growing field in heterogeneous biocatalysis. In this study, we have developed a flow-based technology utilizing a nickel-infused covalent organic framework (Ni-TpBpy COF) to combine two distinct processes: the purification of His-tagged enzymes and the immobilization of enzymes simultaneously. Our work primarily focuses on the purification of three His-tagged enzymes β-glucosidase, cellobiohydrolase, and endoglucanase as well as two proteins with varying molecular weights, namely, green fluorescent protein (27 kDa) and BG Rho (88 kDa). We employed Ni-TpBpy as a column matrix to showcase the versatility of our system. Additionally, we successfully obtained a Ni-TpBpy COF immobilized with enzymes, which can serve as a heterogeneous catalyst for the hydrolysis of p-nitrophenyl-β-d-glucopyranoside and carboxymethylcellulose. These immobilized enzymes demonstrated catalytic activity comparable to that of their free counterparts, with the added advantages of recyclability and enhanced stability under ambient conditions for an extended period, ranging from 60 to 90 days. This contrasts with the free enzymes, which do not maintain their activity as effectively over time.

An Ultrasmall Ordered High-Entropy Intermetallic with Multiple Active Sites for the Oxygen Reduction Reaction.

Controlling multimetallic ensembles at the atomic level is significantly challenging, particularly for high-entropy alloys with more than five elements. Herein, we report an innovative ultrasmall (∼2 nm) PtFeCoNiCuZn high-entropy intermetallic (PFCNCZ-HEI) with a well-ordered structure synthesized by using the space-confined strategy. By exploiting these combined metals, the PFCNCZ-HEI nanoparticles achieve an ultrahigh mass activity of 2.403 A mgPt-1 at 0.90 V vs reversible hydrogen electrode for the oxygen reduction reaction, which is up to 19-fold higher than that of state-of-the-art commercial Pt/C. A proton exchange membrane fuel cell assembled with PFCNCZ-HEI as the cathode (0.03 mgPt cm-2) exhibits a power density of 1.4 W cm-2 and a high mass-normalized rated power of 45 W mgPt-1. Furthermore, theoretical calculations reveal that the outer electrons of the non-noble-metal atoms on the surface of the PFCNCZ-HEI nanoparticle are modulated to show characteristics of multiple active centers. This work offers a promising catalyst design direction for developing highly ordered HEI nanoparticles for electrocatalysis.

Analysis of the properties of a novel natural fibre extracted from pumpkin plant stalks: A sustainable alternative for lightweight applications

This study explores the characterization and potential applications of cellulose fibre extracted from pumpkin stems by the water retting process. X-ray diffraction (XRD) analysis revealed distinct diffraction peaks at 13.2° and 16.8° (2θ), indicating a well-ordered crystalline structure with a crystallinity index of 24.3 %. Fourier-transform infrared (FTIR) spectroscopy identified characteristic peaks at 1430 cm−1 (O-H stretching), 1510 cm−1 (C-H stretching), 1630 cm−1 (C = O stretching), and 1055 cm−1 (C-O-C glycosidic linkage vibrations) confirming the presence of cellulose with vital functional groups. Scanning Electron Microscopy (SEM), analysis revealed a fibrous and porous structure with smooth, cylindrical fibres. The study also assessed the antibacterial properties of pumpkin cellulose fibre against Staphylococcus aureus and Enterococcus faecalis, demonstrating significant inhibitory effects. These findings suggest its potential in healthcare applications, including wound dressings and lightweight structural and medical textiles.

Enhancing Osteoblastic Cell Cultures with Gelatin Methacryloyl, Bovine Lactoferrin, and Bioactive Mesoporous Glass Scaffolds Loaded with Distinct Parsley Extracts.

The increasing interest in innovative solutions for addressing bone defects has driven research into the use of Bioactive Mesoporous Glasses (MBGs). These materials, distinguished by their well-ordered mesoporous structure, possess the capability to accommodate plant extracts with well-established osteogenic properties, including bovine lactoferrin (bLF), as part of their 3D scaffold composition. This harmonizes seamlessly with the ongoing advancements in the field of biomedicine. In this study, we fabricated 3D scaffolds utilizing MBGs loaded with extracts from parsley leaves (PL) and embryogenic cultures (EC), rich in bioactive compounds such as apigenin and kaempferol, which hold potential benefits for bone metabolism. Gelatin Methacryloyl (GelMa) served as the polymer, and bLF was included in the formulation. Cytocompatibility, Runx2 gene expression, ALP enzyme activity, and biomineralization were assessed in preosteoblastic MC3T3-E1 cell cultures. MBGs effectively integrated PL and EC extracts with loadings between 22.6 ± 0.1 and 43.6 ± 0.3 µM for PL and 26.3 ± 0.3 and 46.8 ± 0.4 µM for EC, ensuring cell viability through a release percentage between 28.3% and 59.9%. The incorporation of bLF in the 3D scaffold formulation showed significant differences compared to the control in all assays, even at concentrations below 0.2 µM. Combinations, especially PL + bLF at 0.19 µM, demonstrated additive potential, with superior biomineralization compared to EC. In summary, this study highlights the effectiveness of MBGs in incorporating PL and EC extracts, along with bLF, into 3D scaffolds. The results underscore cytocompatibility, osteogenic activity, and biomineralization, offering exciting potential for future in vivo applications.

Paving the way for electrochemical recycling of spent lithium-ion batteries: Targeting the direct regeneration of de-lithiated materials

The recycling of spent lithium-ion batteries has become an urgent imperative. Electrochemical technology is emerging as an environmentally friendly approach for selectively extracting lithium from discarded cathode materials, garnering significant attention. However, the lack of a clear understanding of the structural evolution during the de-lithiation process, and the re-lithiation mechanism of transition-metal oxides after lithium extraction, hinder the direct regeneration of de-lithiated materials into battery-worthy materials. This limitation also impeds the further advancement of this promising technology. Here, for the first time the structural transformation associated with water-molecule intercalation during the electrochemical process of spent layer material (LiNi0.55Co0.15Mn0.3O2) is demonstrated. X-ray diffraction technique monitors the structural evolution upon de-lithiation, revealing an unusual phase transformation from H3 to “H4” driven by water-molecule intercalation. This transformation triggers significant lattice expansion along c-axis and introduces notable lattice distortion in de-lithiated material. These characteristics render direct calcination for material regeneration impractical, due to lattice collapse from dehydration, obstructing lithium intercalation at high temperatures. Interestingly, low-temperature calcination can endow resynthesized materials with a well-ordered layer structure after creating a lithium-water-balance layer structure for de-lithiated materials by hydrothermal process. Consequently, the regenerated material delivers a capacity of 132.5 mAh/g at 5C.

Structural, Physical, Magnetic, and Dielectric Study of Glassy and Crystalline Bismuth Zinc Silicates

AbstractThe current study aims to thoroughly analyze the optical, magnetic, and dielectric properties of the glass and glass-ceramics in the system Bi2O3.ZnO.SiO2 with stoichiometric composition xBi12SiO20.(100-x)Zn2SiO4(x = 0, 10, 30, 50, 70, 90, and 100). The systematic dependence on density, Bi2O3, and the presence of interphases was studied. Fourier transform infrared (FTIR) spectra of the glass-ceramic samples certify the changes occurring in structure from amorphous to crystalline form where more intense, sharp, narrow bands were observed. Both 10B and 30B samples display more ultraviolet (UV) absorbance than the remaining samples. Upon introducing Bi2O3, the glass sample's color gradually changed from brown to pale yellow. In the vibrating sample magnetometer (VSM) study, the highest (9.22 × 10-7 emu/g) and lowest (4.53 × 10-7 emu/g) magnetic susceptibility were noticed for 30B and 70B samples, respectively. Further, all glass ceramics display diamagnetic properties due to the existence of Bi ions. The glass-ceramic samples showed better dielectric properties than glass samples due to changes from the amorphous nature of the glassy phase (high dielectric loss) to the well-ordered structure of the corresponding glass-ceramic (low dielectric loss). The glass ceramic sample of 100B attained much lower dielectric loss values (0.002, f = 106 Hz) than the corresponding glass sample (0.01, f = 106Hz) which could be helpful for electric storage devices, i.e. capacitors, supercapacitors, batteries, etc. Besides, the high-quality factor (Q = 2758) of the same glass-ceramic sample makes it promising in Radio Frequency (RF) circuits or other high- frequency applications.

High performance broadband photodetector in two-dimensional metal dichalcogenides mediated by topologically protected surface state

Carrier scattering in photodetectors employing 2D dichalcogenide as an absorber impedes carrier transport. As scattering at the interface between the semiconductor and the electrode restricts carrier transport, it is essential to develop alternative electrode materials to achieve high photoresponsivity. A carrier can effectively move through a topologically protected Dirac surface state without scattering: i.e., alternatives such as topological insulators (TI) containing the surface state can effectively reduce scattering at the interface between the semiconductor and the electrode. In this stucy, TI Bi2Se3 with a well-ordered interfacial structure was used as a carrier transport layer (CTL) to effectively employ the topological surface state (TSS) for improving WSe2 photoresponsivity. At 520 nm, the Bi2Se3 TI-CTL photodetector has a photoresponsivity of up to 11.47 AW−1, 100 times higher than the photodevice using only Au electrodes. The photoresponsivity and time-resolved photoluminescence as a function of thickness indicate that TSS contributes to improved carrier separation with high carrier transfer efficiency, thereby affecting photocurrent generation. The fast carrier transfer through TSS helps efficiently separate electron-hole pairs and suppress recombination at the interface, generating ultra-fast and high-efficiency photocurrents in the broadband region (450–1550 nm). Therefore, TSS based on carrier dynamics can lead to further applications of next-generation optoelectronic devices.

Direct observation of radiation-induced graft polymerization on a polyethylene film

Radiation-induced graft polymerization is widely used in the synthesis of polymeric materials with various functionalities; however, the details of the reaction mechanism are still unresolved. Herein, the initial stage of the graft polymerization reaction was investigated through atomic force microscopy (AFM). We used glycidyl methacrylate (GMA) in methanol (monomer solution) and a high-density polyethylene (HDPE) film with a well-ordered lamellar structure as the substrate. Using polymer film surfaces with a maximum grafting degree of 0.5%, AFM can distinguish between crystalline and amorphous polyethylene (PE) phases as well as a grafted polymer GMA (PGMA) phase. The graft polymerization reaction started from the interface between the crystalline and amorphous PE phases. As the reaction proceeded, the PGMA covered the crystalline PE phase: i.e., the entire surface of the PE film were covered by the PGMA. Further, the crystalline lamellae of the PE film eventually became a scaffold for the formation of aggregates comprising grafted polymer chains alone. The graft polymerization reaction mechanism was explained by comparing the solubility parameters of the monomer solution, substrate, and grafted polymer chains. Understanding the reaction mechanism at a low grafting degree obtained in this study may contribute to enhancing the efficiency of the graft polymerization reaction on any polymeric material.

Enhanced heat transfer using wafer-scale crack-free well-ordered porous structure surface

Boiling heat transfer through porous medium is one of the prevalent cooling strategies in electronic thermal management due to its superior heat transfer capability. However, multiple optimization goals generally have conflicting requirements for the physical design of surface structure during boiling heat transfer. In order to reveal the potential mechanism, the boiling characteristics of a heated surface composed of three-dimensional ordered porous inverse opal (IO) structure were studied. From a numerical perspective, the change in critical heat flux does not always have a linear relationship with the thickness of the structure. When the thickness approaches 4.1 μm, the maximum critical heat flux (CHF) of 122 W/cm2 was obtained at a lower superheat (<15 K). Compared with smooth surfaces, the heat transfer performance of IO structure was largely enhanced with a maximum heat transfer coefficient (HTC) improvement of 945%. For IO structures with the thickness of 3.3 μm, the simulated CHF value is 102 W/cm2 which is in close agreement with the experimental value of 103 W/cm2. Due to its uniform porous structure and high capillary capacity, it can persistently maintain small bubbles before approaching CHF, thereby improving heat transfer performance. This high-performance IO structure provides an alternative thermal dissipation method for electronics.

Synergistic mesoporous bimetallic gold-silver nanoparticles: Synthesis, structure, and superior electrocatalytic activity

Mesoporous bimetallic nanoparticles have gained immense interest due to their unique properties and applications in various fields. In this study, we report a novel and straightforward one-pot chemical reduction method for the synthesis of mesoporous AuAg nanoparticles, featuring a substantial mesopore size (>10 nm) and a well-defined structure. The synthetic route involves employing L-cysteine as a ligand to form thiolate-metal(I) complexes and co-reduction of metal precursors around sacrificial templates of polymeric micelles. The resulting nanoparticles exhibit remarkable uniformity in size and possess a well-ordered mesoporous structure. Structural analyses confirm the formation of an alloy system containing Au and Ag without any distinct phases. By adjusting the initial precursor composition, precise control over the Au:Ag ratios in the final products is achievable. The electrocatalytic activity of mesoporous AuAg nanoparticles in the electrooxidation of small molecules surpasses that of mesoporous Au nanoparticles, owing to the synergistic effect arising from both the alterations in the electronic structure and the benefits offered by the porous architecture. This synthetic approach provides a promising avenue for developing efficient and cost-effective mesoporous Au-based nanoparticles for a diverse range of applications.

Acrylic-grafted nanocellulose hybrid double-network hydrogel with super-high toughness for water shutoff treatments

Hydrogels with high strength are strongly needed to perform such operations as fluid plugging and water shutoff in the oil & gas industry. In this work, a new type of tough hydrogel consisting of the acrylic acid grafted nanocellulose network and the copolymer (AA-co-AM) network was synthesized via one-pot free-radical polymerization, and further cross-linked by using Al3+. The prepared dual-crosslinked double network hydrogel (DN-Poly-X-CNF-g-AA) showed the high compressive strength and toughness at low concentrations of nanocellulose (within 0.2 wt%), i.e., the maximum compressive strength was 2.5 MPa at strains of 90% and the recovery rates exceeded to 90% after 10 compressive cycles. Meanwhile, the grafted nanocellulose endowed the double-network hydrogels with the strong intermolecular forces and the well-ordered hierarchical structure, which exhibited a high thermal decomposition temperature, solid-like elastic behavior and a swelling suppression. Finally, the sand-pack plugging experiments showed that the double-network hydrogels could effectively plug the porous media with different permeability, in which the breakthrough pressure gradient was between 4.9 and 104.63 MPa/m. The results demonstrated that the obtained tough hydrogel has a great potential to be applied as soft materials for water shutoff and conformance control in reservoirs.

An Evaluation of the Usability of Argon Plasma-Treated Bacterial Cellulose as a Carrier for Controlled Releases of Glycoside Hydrolases PelAh and PslGh, Which Are Able to Eradicate Biofilm

Bacterial cellulose is a unique biopolymer that has found numerous biomedical applications, such as being an excellent wound-dressing material or a carrier for delivering active compounds. The purpose of this study was to analyze the ability of modified bacterial cellulose (BC) using low-pressure Ar plasma to control the release of glycoside hydrolases with antibiofilm activity, namely PelAh and PslGh, from Pseudomonas aeruginosa. The chemical composition and morphology of the BC surfaces were characterized using photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), and scanning electron microscopy (SEM). The analyses revealed significant changes in the chemical composition of the BC surface due to the introduction of charged functional groups and the conversion of its well-ordered structure into a more amorphous form. The release profiles of enzymes from both forms of the carrier were different and depended on their structural properties. However, a significant impact of BC modification on protein release behavior from the carrier was observed only for PslGh. Both enzymes, when immobilized on pristine and argon plasma-modified BC, retained their ability to effectively reduce biofilm levels, similarly to their soluble form. Ar plasma-modified BC with immobilized specific hydrolases can be used as an effective tool for inhibiting P. aeruginosa biofilm development.

Infrared and Raman Spectroscopy of Mullite Ceramics Synthesized from Fly Ash and Kaolin

Infrared spectroscopy and Raman spectroscopy were used to characterize mullite ceramics prepared from fly ash and kaolin by annealing at 1000 °C, 1100 °C, 1200 °C, and 1300 °C. IR spectroscopy confirmed the presence of SiO4 tetrahedra and AlO6 octahedra in samples. The presence of mullite has been confirmed at all temperatures. The presence of quartz has been confirmed up to a temperature of 1100 °C, and the presence of an amorphous form of SiO2 has been confirmed at temperatures of 1200 °C and 1300 °C. The transformation of quartz into the amorphous form of SiO2 at temperatures above 1100 °C is assumed. Transformation was performed on the percentage intensity decrease of the bending vibration of Si-O-Si (at about 450 cm−1) and Al-O-Si (at about 550 cm−1). Raman spectroscopy confirmed the presence of mullite at different stages of structural ordering (a well-ordered structure at a temperature of 1100 °C and a disordered structure at a temperature of 1300 °C).

Electrochemical performance optimization of NMC811 through the structure design of its precursor

This paper presents a study on the effect of the precursor structure on NMC811 electrochemical properties. The influence of different parameters, such as morphology and crystallinity of the precursor, Ni0.8Mn0.1Co0.1(OH)2, on the final electrochemical performance of NMC811 are analyzed. To ensure a correct and fast mixing of the precursor reactants and prepare the Ni0.8Co0.1Mn0.1(OH)2, a novel approach is used employing a micromixer, thus enabling the collection of the precipitated metal hydroxide within a few seconds after its precipitation. Then the precursor is calcinated together with a Li source to obtain the NMC811 cathode material. When analyzing the aging time of the precursor, between collection and calcination, it is observed that the primary particles of the precursor grow and become more crystalline, adopting a lamellar shape, while the secondary particles turn more compact, when increasing the aging time. The NMC materials synthesized from the aged precursors have smoother primary particles, exposing clearer crystalline planes. This change in morphology is also evidenced in the crystalline structure where an increase in the aging time produces better layered materials with a lower cation mixing index. The well-ordered structure impacts the electrochemical characteristics; indeed, the aged precursor produces NMC with higher specific capacity, better cyclability and lower capacity fade.