Multifunctional DNA nanomaterials: a new frontier in rheumatoid arthritis diagnosis and treatment
Rheumatoid arthritis (RA) remains a challenging autoimmune disease due to its complex and heterogeneous pathophysiology, which complicates therapeutic and diagnostic efforts. Advances in DNA nanotechnology have introduced DNA nanomaterials as promising tools to overcome these barriers. This review focuses on three primary categories of DNA nanomaterials applied in RA: DNA nanostructures, DNA aptamers, and DNA-modified nanoparticles. DNA nanostructures, such as tetrahedral framework nucleic acids (tFNAs) and DNA origami, demonstrate anti-inflammatory properties and facilitate precise, controlled drug delivery. DNA aptamers, functioning as molecular recognition ligands, surpass traditional antibodies with their high specificity, low immunogenicity, and thermal stability, offering significant potential in biomarker detection and therapeutic interventions. While DNA-modified nanoparticles, which integrate DNA with materials like gold or lipids, have shown significant progress in bioimaging and drug delivery in other fields, their application in RA remains limited and warrants further exploration. Furthermore, advancements in stimulus-responsive systems are being explored to enable controlled drug release, which could significantly improve the specificity and efficiency of DNA nanomaterials in therapeutic applications. Despite their immense potential, challenges such as stability under physiological conditions, safety concerns, and clinical regulatory complexities persist. Overcoming these limitations is essential. This review highlights how DNA nanomaterials, beyond serving as delivery platforms, are poised to redefine RA treatment and diagnosis, opening the door to more personalized and effective approaches.
Preparation of novel lithiated high-entropy spinel-type oxyhalides and their electrochemical performance in Li-ion batteries
Compositionally complex doping of spinel oxides toward high-entropy oxides is expected to enhance their electrochemical performance substantially. We successfully prepared high-entropy compounds, the oxide (ZnMgCoCu)FeO (HEOFe), lithiated oxyfluoride Li(ZnMgCoCu)FeOF (LiHEOFeF), and lithiated oxychloride Li(ZnMgCoCu)FeOCl (LiHEOFeCl) with a spinel-based cubic structure by ball milling and subsequent heat treatment. The products exhibit particles with sizes from 50 to 200 nm with a homogeneous atomic distribution. The average elemental composition of the samples is close to the nominal value. Fe Mössbauer spectroscopy revealed that incorporating Li and F or Cl and forming oxygen defects do not influence the redistribution of Fe cations over the spinel lattice sites and result in their preferred octahedral coordination. Electrochemical measurements carried out using 2032-coin cells with a Li-metal anode have shown voltammetric charge capacities of 450, 694, and 593 mA h g for HEOFe, LiHEOFeCl, and LiHEOFeF, respectively. The best electrochemical performance of LiHEOFeCl was ascribed to its smallest particle size. Galvanostatic chronopotentiometry at 1C rate confirmed high initial charge capacities for all the samples but galvanostatic curves exhibited capacity decay over 100 charging/discharging cycles. Raman spectroelectrochemical analysis conducted on the LiHEOFeF sample proved the reversibility of the electrochemical process for initial charging/discharging cycles. Electrochemical impedance spectroscopy revealed the lowest initial charge transfer resistance for LiHEOFeCl and its gradual decrease both for LiHEOFeCl and LiHEOFeF during galvanostatic cycling, whereas the charge transfer resistance of HEOFe slightly increases over 100 galvanostatic cycles due to the different mechanism of the electrochemical reduction.
Rational design of stable carbon nitride monolayer membranes for highly controllable CO capture and separation from CH and CH
CO capture and separation from natural and fuel gas are important industrial issues that refer to the control of CO emissions and the purification of target gases. Here, a novel non-planar g-CN monolayer that could be synthesized the supramolecular self-assembly strategy was identified using DFT calculations. The cohesive energy, phonon spectrum, BOMD, and mechanical stability criteria confirm the stability of the g-CN monolayer. Our DFT calculations and MD simulations designate the g-CN monolayer to perform as a superior CO separation membrane from CH and CH gas owing to the high CO permeability and selectivity. Specifically, the CO permeability ranges from 1.21 × 10 to 1.53 × 10 GPU, while the selectivity of CO/CH and CO/CH is 3.03 × 10 and 3.10 × 10 at 300 K, respectively, much higher than the Robeson upper bound and most of the reported 2D membranes, and even at high temperatures, the g-CN monolayer-based CO separation membranes could operate with high performance. Further, at room temperature, the permeated CO gas can adsorb on the g-CN surface with moderate adsorption energy and high capacity. These results indicate that the g-CN membrane exhibits high performance for controlling CO capture and separation, which inevitably injects a new alternative of novel 2D membranes for CO separation and capture from CH and CH in light of further experimental and theoretical research.
Excitation wavelength-dependent quantum yield in water-soluble CdTe quantum dots
The quantum yield (QY) of semiconductor quantum dots (QDs) is severely hampered by the inherent fluorescence intermittency. The QY of QDs typically increases with an increase in the excitation wavelength. Here, we present a distinctive behavior, where the QY is found to decrease with an increase in the excitation wavelength in water-soluble CdTe QDs (CQDs). Single-particle level measurements highlight the increase in permanent single dark particles at longer wavelengths that comprehend the overall QY of the CQDs in bulk solution. Fluorescence correlation spectroscopy further revealed an increase in the number of dark particles at longer wavelengths. As confirmed by DO/HO exchange, the presence of H ions in water plays an important role in creating variable permanently dark states in the CQDs. This observation was further supported by the cell internalization study of the CQDs, where a much brighter image at a shorter wavelength than at a longer wavelength was observed. A study of the excitation wavelength-dependent QY in QDs may reveal new insights into the applicability of QDs in different device fabrication cases.
Exfoliation of triazole-based CN, CN, and CN nanosheets for efficient photocatalytic ammonia production
Atomically thin two-dimensional nanosheets of nitrogen-rich CN, CN, and CN are synthesized by sonochemical process. Despite their high nitrogen content, their triazole-based crystal structures remain intact after exfoliation. Among the present materials, the nitrogen-richest CN nanosheets display the highest photocatalytic activity for ammonia production, highlighting the synergetic effect of composition control and exfoliation.
Superparamagnetic nanoparticles as potential systems for the treatment of Duchenne muscular dystrophy
This study aims to use superparamagnetic iron oxide nanoparticles (SPIONs), specifically magnetite (FeO), to deliver deflazacort (DFZ) and ibuprofen (IBU) to Duchenne muscular dystrophy-affected (DMD) mouse muscles using an external magnetic field. The SPIONs are synthesized by the co-precipitation method, and their surfaces are functionalized with L-cysteine to anchor the drugs, considering that the cysteine on the surface of the SPIONs in the solid state dimerizes to form the cystine molecule, creating the FeO-(Cys)-DFZ and FeO-(Cys)-IBU systems for tests. The FeO nanoparticles (NPs) were characterized by Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, powder X-ray diffraction (PXRD), transmission electron microscopy (TEM), dynamic light scattering (DLS), and magnetic measurements. The results show that the SPIONs have an average crystallite size of about 8 nm in the solid state and a hydrodynamic size of about 120 nm, which is suitable for biological applications in aqueous dispersion. The nanoparticles exhibit superparamagnetic behavior at room temperature and spherical-close morphology. In addition, vibrational modes characteristic of the functional groups of the molecules anchored to the surface of the SPIONs are identified. Data from blood tests of mice after seven consecutive days of treatment with nanoparticles confirm the non-toxic nature of the system and show an improvement in DMD, with normal levels of liver and kidney enzymes and a decrease in creatine kinase protein.
Platinum single atoms on titania aid dye photodegradation whereas platinum nanoparticles do not
The photocatalytic degradation of unwanted organic species has been investigated for decades using modified and non-modified titania nanostructures. In the present study, we investigate the co-catalytic effect of single atoms (SAs) of Pt and Pt nanoparticles on titania substrates on the degradation of the two typical photodegradation model pollutants: Acid Orange 7 (AO7) and Rhodamine B (RhB). For this, we use highly defined sputter deposited anatase layers and load them with Pt SAs at different loading densities or alternatively with Pt nanoparticles. We find that the Pt SAs have strong accelerating effects (already for a low loading density of ∼10 SAs μm) on the photodegradation of AO7, whereas Pt nanoparticles do hardly have an effect on the decay kinetics. The main beneficial effect of SA Pt is facilitated superoxide formation, which for SAs is significantly enhanced. Overall, the work demonstrates that Pt SA co-catalysts can have a beneficial effect not only for the well-studied use of H generation, but also in the photocatalytic degradation of pollutants-this is particularly the case if the degradation is dominated by a conduction band electron transfer to dissolved O in the solution.
An all-vanadium-based lithium-ion full battery with hierarchical yolk-shell structure electrodes
An all-vanadium-based lithium-ion full battery is successfully assembled with hierarchical micro-nano yolk-shell structures VO and VO as the cathode and anode, which were obtained through a facile solvothermal method with heat treatment under different atmospheres. When used as the cathode of the lithium-ion battery, the hierarchical micro-nano yolk-shell VO demonstrated higher capacities than bulk VO, commercial LiFePO, and LiNiCoMnO cathodes at various current densities. The all-vanadium-based lithium-ion full battery shows good cycle performance at 0.1C and stable charge/discharge abilities at large current densities. The electrochemical performance of the full battery results from the low impedance and pseudocapacitance-dominated lithium storage mechanism derived from the micro-nano yolk-shell structure.
Correction: Relieving immunosuppression during long-term anti-angiogenesis therapy using photodynamic therapy and oxygen delivery
Correction for 'Relieving immunosuppression during long-term anti-angiogenesis therapy using photodynamic therapy and oxygen delivery' by Qianyuan He , , 2020, , 14788-14800, https://doi.org/10.1039/D0NR02750B.
Stacked meshes with super-wettability atmospheric plasma for efficient emulsion separation
Common filter membranes for emulsion separation often require time-intensive preparation and extensive use of chemicals, necessitating a fast-processing and eco-friendly alternative. This study introduces a 2-layer stacked nylon mesh treated with surface diffuse atmospheric plasma (SDAP) for rapid and efficient emulsion separation. Commercial nylon mesh exhibited durable super-wetting properties after just 30 s of SDAP treatment, which was sufficient for effective emulsion separation. Multi-layer stacking further enhanced the oil-blocking capacity, with pre-wetted 2-layer meshes achieving over 98% separation efficiency, a flux exceeding 56 000 L m h bar and excellent anti-aging performance, demonstrating applicability across various emulsions simultaneously. The emulsion droplet dynamics within the filter cake revealed high efficiency, offering valuable insights into membrane fouling issues. Furthermore, this work develops SDAP as a promising approach for material treatment, owing to its fast and environmentally friendly processing, scalable set-up and effectiveness under atmospheric conditions.
Multifunctional iron-cobalt heterostructure (FeCoHS) electrocatalysts: accelerating sustainable hydrogen generation through efficient water electrolysis and urea oxidation
The urgent need to address escalating environmental pollution and energy management challenges has underscored the importance of developing efficient, cost-effective, and multifunctional electrocatalysts. To address these issues, we developed an eco-friendly, cost-effective, and multifunctional electrocatalyst a solvothermal synthesis approach. Due to the merits of the ideal synthesis procedure, the FeCoHS@NF electrocatalyst exhibited multifunctional activities, like OER, HER, OWS, UOR, OUS, and overall alkaline seawater splitting, with required potentials of 1.48, 0.130, 1.59, 1.23, 1.40, and 1.54 V @ 10 mA cm, respectively. Moreover, electrolysers required only 1.40 V at 10 mA cm for energy-saving urea-assisted hydrogen production, which was 190 mV lower than that of the alkaline water electrolyser. The alkaline sewage and seawater purification setup combined with the FeCoHS@NF electrolyzer led to a novel approach of producing pure green hydrogen and water. The ultrastability of the FeCoHS@NF electrocatalyst for industrial applications was confirmed using chronopotentiometry at 10 and 100 mA cm over 110 h for OER, HER, UOR, and overall water splitting. The production of hydrogen using the FeCoHS@NF electrocatalyst in alkaline sewage water and seawater offers multiple benefits, including generation of renewable hydrogen energy, purification of wastewater, reduction of environmental pollutants, and low cost and low electricity consumption of the electrolyser system.
Emerging devices based on chiral nanomaterials
As advanced materials, chiral nanomaterials have recently gained vast attention due to their special geometry-based physical and chemical properties. The fast development of the related science and technology means that various devices involving polarization-based information encryption, photoelectronic and spintronic devices, 3D displays, biomedical sensors and measurement, photonic engineering, electronic engineering, solar devices, , been explored extensively. These fields are at their beginning, and much effort needs to be made, including improving the optical, electronic, and magnetic properties of advanced chiral nanomaterials, precisely designing materials, and developing more efficient construction methods. This review tries to offer a whole picture of these state-of-the-art conditions in these fields and offers perspectives on future development.
Recent advances in mRNA-based therapeutics for neurodegenerative diseases and brain tumors
Messenger RNA (mRNA) therapy is an innovative approach that delivers specific protein-coding information. By promoting the ribosomal synthesis of target proteins within cells, it supplements functional or antigenic proteins to treat diseases. Unlike traditional gene therapy, mRNA does not need to enter the cell nucleus, reducing the risks associated with gene integration. Moreover, protein expression levels can be regulated by adjusting the dosage and degradation rates of mRNA. As a new generation gene therapy strategy, mRNA therapy represents the latest advancements and trends in the field. It offers advantages such as precision, safety, and ease of modification. It has been widely used in the prevention of COVID-19. Unlike acute conditions such as cerebral hemorrhage and stroke that often require immediate surgical or interventional treatments, neurodegenerative diseases (NDs) and brain tumors progress relatively slowly and face challenges such as the blood-brain barrier and complex pathogenesis. These characteristics make them particularly suitable for mRNA therapy. With continued research, mRNA-based therapeutics are expected to play a significant role in the prevention and treatment of NDs and brain tumors. This paper reviews the preparation and delivery of mRNA drugs and summarizes the research progress of mRNA gene therapy in treating NDs and brain tumors. It also discusses the current challenges, providing a theoretical basis and reference for future research in this field.
Advances and applications of dynamic surface-enhanced Raman spectroscopy (SERS) for single molecule studies
Dynamic surface-enhanced Raman spectroscopy (SERS) is nowadays one of the most interesting applications of SERS, in particular for single molecule studies. In fact, it enables the study of real-time processes at the molecular level. This review summarizes the latest developments in dynamic SERS techniques and their applications, focusing on new instrumentation, data analysis methods, temporal resolution and sensitivity improvements, and novel substrates. We highlight the progress and applications of single-molecule dynamic SERS in monitoring chemical reactions, catalysis, biomolecular interactions, conformational dynamics, and real-time sensing and detection. We aim to provide a comprehensive review on its advancements, applications as well as its current challenges and development frontiers.
Liquid-crystal-imprinted synthesis of chiral polypyrroles without a chiral centre using a two-step method of spark-discharge oligomerisation-electrochemical polymerisation
Pyrrole in a cholesteric liquid crystal was discharged using a Tesla coil to generate pyrrole radicals, affording linear-shaped nano-ordered pyrrole oligomers. Subsequently, the electrochemical polymerisation of a pre-oriented pyrrole oligomer having good affinity for liquid crystals was performed to achieve polypyrrole-imprinted asymmetry from the cholesteric liquid crystal structure. The resultant polymers were analysed using polarising optical microscopy observations, scanning electron microscopy, electrochemistry, optical spectroscopy, and electron spin resonance. The combination of spark discharge and electrochemical polymerisation is useful for conveniently transferring the liquid crystal structure to the main chain of polymers.
Strain-tunable optoelectronic and photocatalytic properties of 2D GaN/MoSiP heterobilayers: potential optoelectronic/photocatalytic materials
Herein, we propose a new GaN/MoSiP van der Waals (vdWs) heterostructure constructed by vertically stacking GaN and MoSiP monolayers. Its electronic, optical, and photocatalytic properties are explored DFT++BSE calculations. The calculated binding energy and phonon spectrum demonstrated the material's high stabilities. The projected band structure of GaN/MoSiP suggests that it has a desirable direct bandgap and displays type-I band alignment. It also exhibits a particularly large absorption coefficient for visible and near-infrared light while considering electron-hole interactions. Intriguingly, a small biaxial tensile strain of +1% can transform the band alignment to type-II using a direct Z-scheme mechanism for water splitting. The Z-scheme optimizes redox ability, thus perfectly engulfing the redox potentials of water and showing excellent photocatalytic activity in different layers. Our findings indicate that the GaN/MoSiP vdWs heterostructure is a promising optoelectronic and photocatalytic material.
Biomolecular ligands as tools to modulate the optical and chiroptical properties of gold nanoclusters
Biomolecule-stabilized gold nanoclusters (AuNCs) have become functional nanomaterials of interest because of their unique optical properties, together with excellent biocompatibility and stability under biological conditions. In this review, we explore the recent advancements in the application of biomolecular ligands for synthesizing AuNCs. Various synthesis approaches that are employing amino acids, peptides, proteins, and DNA as biomolecular scaffolds are reviewed. Furthermore, the influence of the synthesis conditions and nature of the biomolecule on the emerging optical (absorption and photoluminescence) and chiroptical properties of AuNCs is discussed. Finally, the latest research on the applications of biomolecule-stabilized AuNCs for biosensing, bioimaging, and theranostics is presented.
Leveraging the dual role of ROS in liver diseases with nanomaterials: clearing and amplifying for therapy
The dual role of reactive oxygen species (ROS) in various liver diseases leads to the potential of nanomaterials in addressing challenges related to liver conditions. Considering the pivotal role of ROS in liver disease progression, the design and application of nanomaterials need to align with distinct disease characteristics and the unique liver microenvironment. By reviewing the interaction between nanomaterials and ROS in liver diseases and their potential applications in liver disease treatment, this work discusses the multifaceted properties of nanomaterials and their high specificity and prospects in liver disease treatments.
Energetic MOF-derived FeC nanoparticles encased in N,S-codoped mesoporous pod-like carbon nanotubes for efficient oxygen reduction reaction
The rational design of advanced oxygen reduction reaction (ORR) catalysts is essential to improve the performance of energy conversion devices. However, it remains a huge challenge to construct hierarchical micro-/meso-/macroporous nanostructures, especially mesoporous transport channels in catalysts, to enhance catalytic capability. Herein, motivated by the characteristics of energetic metal-organic frameworks (EMOFs) that produce an abundance of gases during high-temperature pyrolysis, we prepared a unique tetrazine-based EMOF-derived electrocatalyst (denoted as FeC@NSC-900) consisting of highly dispersed FeC nanoparticles and N,S-codoped mesoporous carbon nanotubes. The mesopore-dominated core-shell structure endows FeC@NSC-900 with excellent catalytic activity and efficient mass transfer. Thus, optimal FeC@NSC-900 demonstrates a high half-wave potential of 0.922 V and great stability in 0.1 M KOH, outperforming commercial Pt/C and most of the reported ORR catalysts. As far as we know, this work is the first application of a tetrazine-based EMOF derivative for the electrocatalytic ORR and is expected to offer some constructive insights into potential of EMOFs for new-generation catalyst design.
Recent advances in poly(amino acids), polypeptides, and their derivatives in drug delivery
Poly(amino acids), polypeptides, and their derivatives have demonstrated significant potential as biodegradable biomaterials in the field of drug delivery. As degradable drug carriers, they can effectively load or conjugate drug molecules including small molecule drugs, nucleic acids, peptides, and protein-based drugs, enhancing the stability and targeting of the drugs . This strategy ultimately facilitates precise drug delivery and controlled release, thereby improving therapeutic efficacy and reducing side effects within the body. This review systematically describes the structural characteristics and preparation methods of poly(amino acids) and polypeptides, summarizes the advantages of poly(amino acids), polypeptides, and their derivatives in drug delivery, and detailedly introduces the latest advancements in this area. The review also discusses current challenges and opportunities associated with poly(amino acids), peptides, and their derivatives, and offers insights into the future directions for these biodegradable materials. This review aims to provide valuable references for scientific research and clinical translation of biodegradable biomaterials based on poly(amino acids) and peptides.
The intriguing role of L-cysteine in the modulation of chiroplasmonic properties of chiral gold nano-arrows
Developing chiral plasmonic nanostructures represents a significant scientific challenge due to their multidisciplinary potential. Observations have revealed that the dichroic behavior of metal plasmons changes when chiral molecules are present in the system, offering promising applications in various fields such as nano-optics, asymmetric catalysis, polarization-sensitive photochemistry and molecular detection. In this study, we explored the synthesis of plasmonic gold nanoparticles and the role of cysteine in their chiroplasmonic properties. Specifically, we synthesized chiral gold nano-arrows using a seed-mediated-growth synthesis method, in which gold nanorods are used as seeds while incorporating L-cysteine into growth solution as a chiral ligand. Our results show clearly that the chiral molecule transfers chirality to gold nanocrystals and the morphology is controlled through kinetic growth. In addition, we demonstrate that the chiroplasmonic properties, such as the sign of circular dichroism, can be modulated using only one enantiomeric form in the growth solution. To understand the origin of such an effect, we conducted theoretical modelling using density functional theory. Our results point to the intermolecular cysteine interactions as a key factor in the dichroic properties of surface-molecule chiral systems.