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1.
Angew Chem Int Ed Engl ; : e202407491, 2024 May 12.
Article in English | MEDLINE | ID: mdl-38735853

ABSTRACT

Ion-selective nanochannel membranes assembled from two-dimensional (2D) nanosheets hold immense promise for power conversion using salinity gradient. However, they face challenges stemming from insufficient surface charge density, which impairs both permselectivity and durability. Herein, we present a novel vacancy-engineered, oxygen-deficient NiCo layered double hydroxide (NiCoLDH)/cellulose nanofibers-wrapped carbon nanotubes (VOLDH/CNF-CNT) composite membrane. This membrane, featuring abundant angstrom-scale, cation-selective nanochannels, is designed and fabricated through a synergistic combination of vacancy engineering and interfacial super-assembly. The membrane shows interlayer free-spacing of ~3.62 Å, which validates the membrane size exclusion selectivity.This strategy, validated by DFT calculations and experimental data, improves hydrophilicity and surface charge density, leading to the strong interaction with K+ ions to benefit the low ion transport resistance and exceptional charge selectivity. When employed in an artificial river water|seawater salinity gradient power generator, it delivers a high-power density of 5.35 W/m2 with long-term durability (20,000s), which is almost 400% higher than that of the pristine NiCoLDH membrane. Furthermore, it displays both pH- and temperature-sensitive ion transport behavior, offering additional opportunities for optimization. This work establishes a basis for high-performance salinity gradient power conversion and underscores the potential of vacancy engineering and super-assembly in customizing 2D nanomaterials for diverse advanced nanofluidic energy devices.

2.
Adv Healthc Mater ; : e2400707, 2024 Apr 02.
Article in English | MEDLINE | ID: mdl-38563114

ABSTRACT

Existing artificial periostea face many challenges, including difficult-to-replicate anisotropy in mechanics and structure, poor tissue adhesion, and neglected synergistic angiogenesis and osteogenesis. Here, inspired by natural wood (NW), a wood-derived elastic artificial periosteum is developed to mimic the structure and functions of natural periosteum, which combines an elastic wood (EW) skeleton, a polydopamine (PDA) binder layer, and layer-by-layer (LBL) biofunctional layers. Specifically, EW derived from NW is utilized as the anisotropic skeleton of artificial periosteum to guide cell directional behaviors, moreover, it also shows a similar elastic modulus and flexibility to natural periosteum. To further enhance its synergistic angiogenesis and osteogenesis, surface LBL biofunctional layers are designed to serve as spatiotemporal release platforms to achieve sequential and long-term release of pamidronate disodium (PDS) and deferoxamine (DFO), which are pre-encapsulated in chitosan (CS) and hyaluronic acid (HA) solutions, respectively. Furthermore, the combined effect of PDA coating and LBL biofunctional layers enables the periosteum to tightly adhere to damaged bone tissue. More importantly, this novel artificial periosteum can boost angiogenesis and bone formation in vitro and in vivo. This study opens up a new path for biomimetic design of artificial periosteum, and provides a feasible clinical strategy for bone repair.

3.
Int J Biol Macromol ; 267(Pt 2): 131651, 2024 May.
Article in English | MEDLINE | ID: mdl-38636746

ABSTRACT

The plastics derived from fossil fuels for food packaging results in serious environmental problems. Developing environment-friendly materials for food packaging is urgent and essential. In this study, polylactic acid (PLA) composite nanofibers membranes were prepared with good biocompatibility and antibacterial property. Cu2+ loaded in the natural halloysite nanotubes (HNTs) was used for the antibacterial agent. Cu2+ was loaded in the HNTs and was confirmed by the X-ray photoelectron spectroscopy (XPS). PLA nanofibers with different HNTs-Cu content were continuous nanofibers with the nanoscale range. HNTs-Cu entered into the nanofiber successfully. Thermal analysis results showed composite nanofibers had good thermal stability. Composite nanofiber membranes had the good hydrophobic property. HNTs-Cu improved the mechanical property of composite nanofibers than pure PLA nanofibers. Tensile strength and elasticity modulus of composite nanofibers with 4 % HNTs-Cu content were the most outstanding. L929 cells were cultured on the nanofiber membranes for biocompatibility evaluation. Cell viability of nanofiber membranes was above the 90 %. Cell live/dead staining results showed L929 cells was seldom dead on the nanofiber membranes. PLA/HNTs-Cu nanofiber membranes exhibited excellent antibacterial effects on S. aureus and E. coli. The inhibitory rates against S. aureus and E. coli were 98.31 % and 97.80 % respectively. The fresh-keeping effects of nanofiber membranes were evaluated by the strawberry preservation. Strawberries covered by nanofiber membranes exhibited better appearance, lower weight loss and higher firmness than control, PLA and PLA/HNTs groups. It promised that PLA/HNTs-Cu composite nanofiber membranes have the significant potential application for active food packaging.


Subject(s)
Anti-Bacterial Agents , Clay , Copper , Food Packaging , Nanofibers , Nanotubes , Polyesters , Staphylococcus aureus , Copper/chemistry , Copper/pharmacology , Nanofibers/chemistry , Polyesters/chemistry , Nanotubes/chemistry , Food Packaging/methods , Clay/chemistry , Anti-Bacterial Agents/pharmacology , Anti-Bacterial Agents/chemistry , Staphylococcus aureus/drug effects , Escherichia coli/drug effects , Mice , Membranes, Artificial , Animals , Cell Line , Tensile Strength , Cell Survival/drug effects
4.
Small ; : e2400774, 2024 Apr 15.
Article in English | MEDLINE | ID: mdl-38616778

ABSTRACT

Capacitive carbon cathodes deliver great potential for zinc-ion hybrid capacitors (ZHCs) due to their resource abundance and structural versatility. However, the dimension mismatch between the micropores of carbons and hydrated Zn2+ ions often results in unsatisfactory charge storage capability. Here well-arranged heterodiatomic carbon superstructures are reported with compatible pore dimensions for activating Zn2+ ions, initiated by the supramolecular self-assembly of 1,3,5-triazine-2,4,6-triamine and cyanuric acid via in-plane hydrogen-bonds and out-of-plane π-π interactions. Flower-shaped carbon superstructures expose more surface-active motifs, continuous charge-transport routes, and more importantly, well-developed pores. The primary subnanopores of 0.82 nm are size-exclusively accessible for solvated Zn2+ ions (0.86 nm) to maximize spatial charge storage, while rich mesopores (1-3 nm) allow for high-kinetics ion migration with a low activation energy. Such favorable superstructure cathodes contribute to all-round performance improvement for ZHCs, including high energy density (158 Wh kg-1), fast-charging ability (50 A g-1), and excellent cyclic lifespan (100 000 cycles). An anion-cation hybrid charge storage mechanism is elucidated for superstructure cathode, which entails alternate physical uptake of Zn2+/CF3SO3 - at electroactive pores and bipedal chemical binding of Zn2+ to electronegative carbonyl/pyridine motifs. This work expands the design landscape of carbon superstructures for advanced energy storage.

5.
ACS Appl Mater Interfaces ; 16(12): 15177-15192, 2024 Mar 27.
Article in English | MEDLINE | ID: mdl-38471076

ABSTRACT

Halloysite nanotubes (HNTs) are one-dimensional clay nanomaterials featuring distinct tubular structures and unique surface charges. HNTs can readily form ordered assembly structures under specific conditions, which shows significant potential applications in optical and biological fields. In this study, sodium hexametaphosphate (SHMP) was employed as a stabilizer to prepare polymer spherulite-like patterns via the evaporation-induced self-assembly (EISA) technique. The incorporation of SHMP enhanced the repulsion force among the nanotubes and the surface potential, which facilitated the orderly deposition of HNTs. The influence of HNT concentration, SHMP concentration, drying temperature, and substrate on the polymer spherulites-like pattern has been investigated in detail. The optimal conditions were 10 wt % HNT dispersion, 0.6 wt % SHMP concentration, 30 °C as drying temperature, and glass substrates. In addition, by changing the droplet volume and shape of the three-phase contact line, patterns of different sizes and shapes can be achieved. Bovine serum albumin or metal salt compounds were incorporated into the dispersion of SHMP-modified HNTs, which altered the charge and the self-assembled patterns with different area ratios. Thus, this technology can be utilized for the analysis and comparison of protein and metal ion concentration accurately. This study creates the correlation between the structural parameters and the preparation process involved in creating polymer spherulite-like patterns of modified HNTs and offers fresh insights into potential applications for the self-assembly of HNT droplets in the realms of anticounterfeiting and solution concentration analysis.

6.
Sci Technol Adv Mater ; 25(1): 2327276, 2024.
Article in English | MEDLINE | ID: mdl-38532983

ABSTRACT

Micropatterning of biological surfaces performed via assembly of nano-blocks is an efficient design method for functional materials with complex organic-inorganic architecture. Halloysite clay nanotubes with high aspect ratios and empty lumens have attracted widespread interest for aligned biocompatible composite production. Here, we give our vision of advances in interfacial self-assembly techniques for these natural nanotubes. Highly ordered micropatterns of halloysite, such as coffee rings, regular strips, and concentric circles, can be obtained through high-temperature evaporation-induced self-assembly in a confined space and shear-force brush-induced orientation. Assembly of these clay nanotubes on biological surfaces, including the coating of human or animal hair, wool, and cotton, was generalized with the indication of common features. Halloysite-coated microfibers promise new approaches in cotton and hair dyeing, medical hemostasis, and flame-retardant tissue applications. An interfacial halloysite assembly on oil microdroplets (Pickering emulsion) and its core-shell structure (functionalization with quantum dots) was described in comparison with microfiber nanoclay coatings. In addition to being abundantly available in nature, halloysite is also biosafe, which makes its spontaneous surface micropatterning prospective for high-performance materials, and it is a promising technique with potential for an industrial scale-up.


This international group of authors unites researchers who pioneered halloysite clay nanotubes for biomaterials, and discloses a new strategy for this nanoclay composite design through interfacial architecture. These results confirm Dr. K. Ariga concept of nanoarchitectonics, and demonstrate promising applications. Assembly of the clay nanotubes on biosurfaces, including the coating of human or animal hair, wool, and cotton, was generalized for the process optimization. Halloysite-coated microfibers promise new approaches in cotton and hair dyeing, and medical hemostasis and flame-retardant tissue applications. Related techniques of interfacial halloysite assembly on oil microdroplets (Pickering emulsion) and its quantum dots core­shell structure for cell imaging are also described. Contrary to many other synthetic nanomaterials, described natural halloysite nanotubes are environmentally safe and abundantly available, thus allowing for scale up of the suggested functional biocomposites.

7.
Chem Sci ; 15(12): 4322-4330, 2024 Mar 20.
Article in English | MEDLINE | ID: mdl-38516081

ABSTRACT

Dendrite growth and parasitic reactions of a Zn metal anode in aqueous media hinder the development of up-and-coming Zn-ion batteries. Optimizing the crystal growth after Zn nucleation is promising to enable stable cyclic performance of the anode, but directly regulating specific crystal plane growth for homogenized Zn electrodeposition remains highly challenging. Herein, a perfluoropolymer (Nafion) is introduced into an aqueous electrolyte to activate a thermodynamically ultrastable Zn/electrolyte interface for long-term Zn-ion batteries. The low adsorption energy (-2.09 eV) of Nafion molecules on Zn metal ensures the in situ formation of a Nafion-nanofilm during the first charge process. This ultrathin artificial solid electrolyte interface with zincophilic -SO3- groups guides the directional Zn2+ electrodeposition along the (002) crystal surface even at high current density, yielding a dendrite-free Zn anode. The synergic Zn/electrolyte interphase electrochemistry contributes an average coulombic efficiency of 99.71% after 4500 cycles for Zn‖Cu cells, and Zn‖Zn cells achieve an ultralong lifespan of over 7000 h at 5 mA cm-2. Besides, Zn‖MnO2 cells operate well over 3000 cycles. Even at -40 °C, Zn‖Zn cells achieve stable Zn2+ plating/stripping for 1200 h.

8.
Adv Sci (Weinh) ; 11(19): e2310319, 2024 May.
Article in English | MEDLINE | ID: mdl-38477446

ABSTRACT

Zinc-organic batteries (ZOBs) are receiving widespread attention as up-and-coming energy-storage systems due to their sustainability, operational safety and low cost. Charge carrier is one of the critical factors affecting the redox kinetics and electrochemical performances of ZOBs. Compared with conventional large-sized and sluggish Zn2+ storage, non-metallic charge carriers with small hydrated size and light weight show accelerated interfacial dehydration and fast reaction kinetics, enabling superior electrochemical metrics for ZOBs. Thus, it is valuable and ongoing works to build better ZOBs with non-metallic ion storage. In this review, versatile non-metallic cationic (H+, NH4 +) and anionic (Cl-, OH-, CF3SO3 -, SO4 2-) charge carriers of ZOBs are first categorized with a brief comparison of their respective physicochemical properties and chemical interactions with redox-active organic materials. Furthermore, this work highlights the implementation effectiveness of non-metallic ions in ZOBs, giving insights into the impact of ion types on the metrics (capacity, rate capability, operation voltage, and cycle life) of organic cathodes. Finally, the challenges and perspectives of non-metal-ion-based ZOBs are outlined to guild the future development of next-generation energy communities.

9.
Carbohydr Polym ; 332: 121927, 2024 May 15.
Article in English | MEDLINE | ID: mdl-38431420

ABSTRACT

Natural bone exhibits a complex anisotropic and micro-nano hierarchical structure, more importantly, bone extracellular matrix (ECM) presents liquid crystal (LC) phase and viscoelastic characteristics, providing a unique microenvironment for guiding cell behavior and regulating osteogenesis. However, in bone tissue engineering scaffolds, the construction of bone-like ECM microenvironment with exquisite microstructure is still a great challenge. Here, we developed a novel polysaccharide LC hydrogel supported 3D printed poly(l-lactide) (PLLA) scaffold with bone-like ECM microenvironment and micro-nano aligned structure. First, we prepared a chitin whisker/chitosan polysaccharide LC precursor, and then infuse it into the pores of 3D printed PLLA scaffold, which was previously surface modified with a polydopamine layer. Next, the LC precursor was chemical cross-linked by genipin to form a hydrogel network with bone-like ECM viscoelasticity and LC phase in the scaffold. Subsequently, we performed directional freeze-casting on the composite scaffold to create oriented channels in the LC hydrogel. Finally, we soaked the composite scaffold in phytic acid to further physical cross-link the LC hydrogel through electrostatic interactions and impart antibacterial effects to the scaffold. The resultant biomimetic scaffold displays osteogenic activity, vascularization ability and antibacterial effect, and is expected to be a promising candidate for bone repair.


Subject(s)
Chitosan , Liquid Crystals , Animals , Chitosan/chemistry , Hydrogels/pharmacology , Hydrogels/metabolism , Chitin/pharmacology , Chitin/metabolism , Vibrissae , Tissue Scaffolds/chemistry , Bone Regeneration , Tissue Engineering , Osteogenesis , Extracellular Matrix/metabolism , Anti-Bacterial Agents/pharmacology
10.
Angew Chem Int Ed Engl ; 63(16): e202401049, 2024 Apr 15.
Article in English | MEDLINE | ID: mdl-38372434

ABSTRACT

Bipolar organics fuse the merits of n/p-type redox reactions for better Zn-organic batteries (ZOBs), but face the capacity plafond due to low density of active units and single-electron reactions. Here we report multielectron redox-bipolar tetranitroporphyrin (TNP) with quadruple two-electron-accepting n-type nitro motifs and dual-electron-donating p-type amine moieties towards high-capacity-voltage ZOBs. TNP cathode initiates high-kinetics, hybrid anion-cation 10e- charge storage involving four nitro sites coordinating with Zn2+ ions at low potential and two amine species coupling with SO4 2- ions at high potential. Consequently, Zn||TNP battery harvests high capacity (338 mAh g-1), boosted average voltage (1.08 V), and outstanding energy density (365 Wh kg-1 TNP). Moreover, the extended π-conjugated TNP macrocycle achieves anti-dissolution in electrolytes, prolonging the battery life to 50,000 cycles at 10 A g-1 with 71.6 % capacity retention. This work expands the chemical landscape of multielectron redox-bipolar organics for state-of-the-art ZOBs.

11.
Angew Chem Int Ed Engl ; 63(13): e202315122, 2024 Mar 22.
Article in English | MEDLINE | ID: mdl-38311601

ABSTRACT

Dendrites growth and unstable interfacial Li+ transport hinder the practical application of lithium metal batteries (LMBs). Herein, we report an active layer of 2,4,6-trihydroxy benzene sulfonyl fluorine on copper substrate that induces oriented Li+ deposition and generates highly crystalline solid-electrolyte interphase (SEI) to achieve high-performance LMBs. The lithiophilic -SO2 - groups of highly crystalline SEI accept the rapidly transported Li+ ions and form a dense inner layer of LiF and Li3 N, which regulate Li+ plating morphology along the (110) crystal surface toward dendrite-free Li anode. Thus, Li||Cu cells with lithiophilic SEI achieve an average deposition efficiency of 99.8 % after 700 cycles, and Li||Li cells operate well for 1100 h. Besides, Li||LiNi0.8 Co0.1 Mn0.1 O2 cells with modified SEI exhibit a capacity retention that is 14 times than that of conventional SEI. Even at -60 °C, Li||Cu cells reach stable deposition efficiency of 83.2 % after 100 cycles.

12.
Carbohydr Polym ; 328: 121728, 2024 Mar 15.
Article in English | MEDLINE | ID: mdl-38220327

ABSTRACT

Conductive hydrogels show extensive applications in flexible electronics and biomedical areas, but it is a challenge to simultaneously achieve high mechanical properties, satisfied electrical conductivity, good biocompatibility, self-recovery and anti-freezing properties through a simple preparation method. Herein, chitin nanocrystals (ChNCs) were employed to encapsulate liquid metal nanoparticles (LMNPs) to ensure the dispersion stability of LMNPs in a hydrogel system composed of polyacrylamide (PAM) and polyvinyl alcohol (PVA). The synergistic effect of ChNCs-stabilized LMNPs imparts remarkable conductivity to the hydrogel, making it an effective strain sensor for human motion. With 1 % LMNPs, the composite hydrogel stretches up to 2100 %, showing excellent stretchability. Under 10 cycles of 200 % strain, hysteresis loop curves overlap, indicating outstanding fatigue resistance. The hydrogel exhibits remarkable self-recovery, enduring 1400 % deformation without rupture. In addition, its effective antifreeze properties result from immersion in a glycerol-water solvent. Even at -20 °C and 60 °C, the hydrogel maintains stable, reproducible resistance changes at 150 % tensile strain. Therefore, the high-performance conductive hydrogel containing ChNCs stabilized LM has promising applications in flexible wearable sensing devices.

13.
Bioresour Technol ; 395: 130284, 2024 Mar.
Article in English | MEDLINE | ID: mdl-38219925

ABSTRACT

The role of metal organic framework (MOF) modified cathode in promoting long chain fatty acid (LCFA) methanation was identified in microbial electrolysis cell coupled anaerobic digestion (MEC-AD) system. The maximum methane production rate of MEC-AD-MOF achieved 49.8 ± 3.4 mL/d, which increased by 41 % compared to MEC-AD-C. The analysis of bio-cathode biofilm revealed that microbial activity, distribution, population, and protein secretion prompted by MOF cathode, which in turn led to an acceleration of electron transfer between the cathode and microbes. Specifically, the relative abundance of acetate-oxidizing bacterium (Mesotoga) in MEC-AD-MOF was 1.5-3.6 times higher than that in MEC-AD-C, with a co-metabolized enrichment of Methanobacterium. Moreover, MOF cathode reinforced LCFA methanation by raising the relative abundance of genes coded key enzymes involved in CO2-reducing pathway, and elevating the tolerance of microbes to LCFA inhibition. These results indicate that MOF can enhance biofilm construction in MEC-AD, thereby improving the treatment performance of lipid wastewater.


Subject(s)
Metal-Organic Frameworks , Anaerobiosis , Bioreactors , Methane , Fatty Acids , Electron Transport , Electrolysis , Electrodes
14.
Angew Chem Int Ed Engl ; 63(3): e202316835, 2024 Jan 15.
Article in English | MEDLINE | ID: mdl-38010854

ABSTRACT

Compared with Zn2+ storage, non-metallic charge carrier with small hydrated size and light weight shows fast dehydration and diffusion kinetics for Zn-organic batteries. Here we first report NH4 + /H+ co-storage in self-assembled organic superstructures (OSs) by intermolecular interactions of p-benzoquinone (BQ) and 2, 6-diaminoanthraquinone (DQ) polymer through H-bonding and π-π stacking. BQ-DQ OSs exhibit exposed quadruple-active carbonyl motifs and super electron delocalization routes, which are redox-exclusively coupled with high-kinetics NH4 + /H+ but exclude sluggish and rigid Zn2+ ions. A unique 4e- NH4 + /H+ co-coordination mechanism is unravelled, giving BQ-DQ cathode high capacity (299 mAh g-1 at 1 A g-1 ), large-current tolerance (100 A g-1 ) and ultralong life (50,000 cycles). This strategy further boosts the capacity to 358 mAh g-1 by modulating redox-active building units, giving new insights into ultra-fast and stable NH4 + /H+ storage in organic materials for better Zn batteries.

15.
J Colloid Interface Sci ; 658: 856-864, 2024 Mar 15.
Article in English | MEDLINE | ID: mdl-38157610

ABSTRACT

Understanding the self-stacking interactions in precursors can facilitate the preparation of high-performance carbon materials and promote the commercial application of zinc ion hybrid capacitors (ZIHCs). Here, a π-conjugated molecule mediated pyrolysis strategy is presented to prepare carbon materials. Taking intermolecular force simulation (reduced density gradient plots) as a guide, the relationship between the self-stacking interactions in π-conjugated molecules and the structural parameters of carbon materials can be extrapolated. The resultant self-doped hierarchical porous carbons (NHPCs) derived from 1, 8, 4, 5-naphthalenetetracarboxdiimide with suitable self-stacking interactions empower the highest specific surface areas (2038 m2/g) and surface opening macropores. The NHPCs-based ZIHCs deliver a high capacity of 220 mAh/g, a high energy density of 149.5 Wh kg-1 and a super-stable cycle lifespan with 93.2 % capacity retention after 200, 000 cycles. The excellent electrochemical performance roots in the superior hierarchical porous structure with surface opening macropores, which guarantees the structural stability of carbon cathodes upon repeated rounds. Meanwhile, the heteroatom doping further relieves the kinetics concern of Zn2+ uptake/removal to enhance O-Zn-N binding particularly at high discharge currents. Besides, the proton-assisted Zn2+ dual-ion storage mechanism plays an essential role in the energy storage process. This work demonstrates a facile synthesis method and advances the fundamental understanding of its dual-ion storage mechanism.

16.
Nanotechnology ; 35(15)2024 Jan 23.
Article in English | MEDLINE | ID: mdl-38150723

ABSTRACT

Smart energy storage systems, such as electrochromic supercapacitor (ECSC) integrated technology, have drawn a lot of attention recently, and numerous developments have been made owing to their reliable performance. Developing novel electrode materials for ECSCs that embed two different technologies in a material is an exciting and emerging field of research. To date, the research into ECSC electrode materials has been ongoing with excellent efforts, which need to be systematically reviewed so that they can be used to develop more efficient ECSCs. This mini-review provides a general composition, main evaluation parameters and future perspectives for electrode materials of ECSCs as well as a brief overview of the published reports on ECSCs and performance statistics on the existing literature in this field.

17.
Bioresour Technol ; 394: 130203, 2024 Feb.
Article in English | MEDLINE | ID: mdl-38109977

ABSTRACT

Excessive ammonia stresses anaerobic digestion (AD) significantly. Although there has been progress in understanding AD under ammonia exposure, investigations on AD liberated from ammonia exposure are limited. Here, the recovery capability of AD from ammonia stress was evaluated, by examining specific methanogenic activity, energy-conserving capability, microbial community succession, and metabolic pathway reconstruction. The findings demonstrated that ammonia stress relief resulted in < 50% methane recovery, with propionate conversion identified as the critical impediment to AD reactivation. Energy generation could not recovered either. Efforts to mitigate ammonia stress failed to restore acetoclastic methanogens, e.g., Methanothrix soehngenii, and proved futile in awakening propionate oxidizers, e.g., Desulfobulbus. Interestingly, a symbiotic metabolism emerged, prevailing in stress-relieved AD due to its energy-conserving advantage. This study underscores the importance of targeted interventions, including stimulating acetoclastic methanogenesis, propionate oxidation, and energy generation, as priorities for AD recovery following ammonia stress, rather than focusing solely on ammonia level management.


Subject(s)
Euryarchaeota , Propionates , Anaerobiosis , Ammonia/metabolism , Bioreactors , Euryarchaeota/metabolism , Methane
18.
ACS Appl Mater Interfaces ; 15(50): 58196-58211, 2023 Dec 20.
Article in English | MEDLINE | ID: mdl-38079497

ABSTRACT

Tissue-engineered poly(l-lactide) (PLLA) scaffolds have been widely used to treat bone defects; however, poor biological activities have always been key challenges for its further application. To address this issue, introducing bioactive drugs or factors is the most commonly used method, but there are often many problems such as high cost, uncontrollable and monotonous drug activity, and poor bioavailability. Here, a drug-free 3D printing PLLA scaffold with a triple-effect combination induced by surface-modified copper-doped layered double hydroxides (Cu-LDHs) is proposed. In the early stage of scaffold implantation, Cu-LDHs exert a photothermal therapy (PTT) effect to generate high temperature to effectively prevent bacterial infection. In the later stage, Cu-LDHs can further have a mild hyperthermia (MHT) effect to stimulate angiogenesis and osteogenic differentiation, demonstrating excellent vascularization and osteogenic activity. More importantly, with the degradation of Cu-LDHs, the released Cu2+ and Mg2+ provide an ion microenvironment effect and further synergize with the MHT effect to stimulate angiogenesis and osteogenic differentiation, thus more effectively promoting the healing of bone tissue. This triple-effect combined scaffold exhibits outstanding antibacterial, osteogenic, and angiogenic activities, as well as the advantages of low cost, convenient procedure, and long-term efficacy, and is expected to provide a promising strategy for clinical repair of bone defects.


Subject(s)
Osteogenesis , Tissue Scaffolds , Copper/pharmacology , Bone Regeneration , Hydroxides/pharmacology , Printing, Three-Dimensional
19.
Carbohydr Polym ; 321: 121292, 2023 Dec 01.
Article in English | MEDLINE | ID: mdl-37739527

ABSTRACT

Inspired by the similarity of anisotropic channels in wood to the canals of bone, the elastic wood-derived (EW) scaffolds with anisotropic channels were prepared via simple delignification treatment of natural wood (NW). We hypothesize that the degree of delignification will lead to differences in mechanical properties of scaffolds, which in turn directly affect the behaviors and fate of stem cells. The delignification process did not destroy the anisotropic channel structure of the scaffolds, but endowed the scaffolds with good elasticity and rapid stress relaxation. Interestingly, the micron-scale anisotropic channels of the scaffolds can highly promote the polarization of cells along the direction of channels. We also found that the alkaline phosphatase of EW scaffold can reach to about 13.1 U/gprot, which was about double that of NW scaffold. Moreover, the longer the delignification time, the better the osteogenic activity of the EW scaffolds. We further hypothesize that the osteogenic activity of scaffolds is related to the stress relaxation properties. The immunofluorescence staining showed that when the stress relaxation time of scaffold was shortened to about 10 s, the nuclear ratio of YAP of scaffold increased to 0.22, which well supports our hypothesis.


Subject(s)
Cues , Osteogenesis , Alkaline Phosphatase , Anisotropy , Cell Differentiation
20.
J Colloid Interface Sci ; 651: 714-725, 2023 Dec.
Article in English | MEDLINE | ID: mdl-37567115

ABSTRACT

Preparing complex non-spherical assemblies of elongated nanoparticles and exploring their topological conformations is a challenge due to liquid crystals' mobility and elastic distortion. Here, we fabricated a variety of non-spherical liquid crystal assemblies of chitin nanocrystals (ChNCs) in a coagulation bath containing sodium triphosphate (STP) by drop impact assembly method, and the forming mechanism and internal topology were systematically investigated. The collection height, ChNCs concentration, and STP concentration have significant influence on the shape and size of the assembled structures. Long-range ordered structures and long-lived topological textures of the ChNCs liquid crystal can be obtained since a molecular interaction of hydrogen bonding and electrostatic attractions between ChNCs and STP occur during the impact assembly. Rheological and kinetic analysis suggested the shear thinning behavior of the ChNCs liquid crystals and the rapid gelation phenomenon of ChNCs induced by STP. Morphology results showed that the rod-like ChNCs in the non-spherical assemblies were orderly and closely arranged with periodic repetition and layered structure. The non-spherical assemblies of ChNCs liquid crystals can be used as carriers of carbon nanotubes, magnetic Fe3O4 nanoparticles, synthesized polymers, and anticancer drugs for functional composite applications. The drop impact assembly method of ChNCs liquid crystal structure is highly controllable on the composition, morphology, and function, which shows promising applications in energy, environmental-friendly, and bioactive materials.

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