Owing to the rapid increase in anthropogenic emission of carbon dioxide (CO2) in the atmosphere, which has resulted in a number of global climate challenges, a decrease in CO2 emissions is urgently needed in the current scenario. This study focuses on the development and characterization of composites for carbon dioxide (CO2) separation. The composites consist of two task-specific ionic liquids (TSILs), namely, tetramethylgunidinium imidazole [TMGHIM] and tetramethylgunidinium phenol [TMGHPhO], impregnated in ZIF-8. The performance of CO2 separation, including sorption capacity and selectivity, was evaluated for pristine ZIF-8 and composites of TMGHIM@ZIF-8 and TMGHPhO@ZIF-8. To demonstrate the thermal stability of the material, thermogravimetric analysis (TGA) was performed. Additionally, powder X-ray diffraction (XRD) and scanning electron microscopy (SEM) were utilized to showcase the crystal structures and morphology. Fourier transform infrared spectroscopy (FTIR) and BET were also utilized to confirm the successful incorporation of TSILs into ZIF-8. The composite synthesized with TMGHIM@ZIF-8 demonstrated superior CO2 sorption performance as compared with TMGHPhO@ZIF-8. This is attributed to its strong attraction toward CO2, resulting in a higher CO2/CH4 selectivity of 110 while pristine MOFs showed 12 that is 9 times higher than that of the pristine ZIF-8. These TSILs@ZIF-8 composites have significant potential in designing sorbent materials for efficient acid gas separation applications.
Mitochondrial therapy is a promising new strategy that offers the potential to achieve precise disease diagnosis or maximum therapeutic response. However, versatile mitochondrial theranostic platforms that integrate biomarker detection and therapy have rarely been exploited. Here, we report a charge-reversal nanomedicine activated by an acidic microenvironment for mitochondrial microRNA (mitomiR) detection and ion-interference therapy. The transporter liposome (DD-DC) was constructed from a pH-responsive polymer and a positively charged phospholipid, encapsulating NaCl nanoparticles with coloading of the aggregation-induced emission (AIE) fluorogens AIEgen-DNA/G-quadruplexes precursor and brequinar (NAB@DD-DC). The negatively charged nanomedicine ensured good blood stability and high tumor accumulation, while the charge-reversal to positive in response to the acidic pH in the tumor microenvironment (TME) and lysosomes enhanced the uptake by tumor cells and lysosome escape, achieving accumulation in mitochondria. The subsequently released Na+ in mitochondria not only contributed to the formation of mitomiR-494 induced G-quadruplexes for AIE imaging diagnosis but also led to an osmolarity surge that was enhanced by brequinar to achieve effective ion-interference therapy.
Biphenyl Compounds , G-Quadruplexes , MicroRNAs , Nanoparticles , Neoplasms , Quinaldines , Humans , Sodium Chloride , Neoplasms/diagnostic imaging , Neoplasms/therapy , Mitochondria , Hydrogen-Ion Concentration , Cell Line, Tumor , Tumor Microenvironment
Microdevices that offer hyperglycemia monitoring and controllable drug delivery are urgently needed for daily diabetes management. Herein, a theranostic separable double-layer microneedle (DLMN) patch consisting of a swellable GelMA supporting base layer for glycemia sensing and a phase-change material (PCM) arrowhead layer for hyperglycemia regulation has been fabricated. The Cu-TCPP(Fe)/glucose oxidase composite and 3,3',5,5'-tetramethylbenzidine coembedded in the supporting base layer permit a visible color shift at the base surface in the presence of glucose via a cascade reaction, allowing for the in situ detection of glucose in interstitial fluid. The PCM arrowhead layer is encapsulated with water monodispersity melanin nanoparticles from Sepia officinalis and metformin that is imparted with a near-infrared ray photothermal response feature, which is beneficial to the controllable release of metformin for suppression of hyperglycemia. By applying the DLMN patch to the streptozotocin-induced type 2 diabetic Sprague-Dawley rat model, the results demonstrated that it can effectively extract dermal interstitial fluid, read out glucose levels, and regulate hyperglycemia. This DLMN-integrated portable colorimetric sensor and self-regulated glucose level hold great promise for daily diabetes management.
In recent years, microneedles (MNs) have attracted a lot of attention due to their microscale sizes and high surface area (500-1000 µm in length), allowing pain-free and efficient drug delivery through the skin. In addition to the great success of MNs based transdermal drug delivery, especially for skin diseases, increasing studies have indicated the expansion of MNs to diverse nontransdermal applications, including the delivery of therapeutics for hair loss, ocular diseases, and oral mucosal. Here, the current treatment of hair loss, eye diseases, and oral disease is discussed and an overview of recent advances in the application of MNs is provided for these three noncutaneous localized organ diseases. Particular emphasis is laid on the future trend of MNs technology development and future challenges of expanding the generalizability of MNs.
Needles , Skin , Humans , Administration, Cutaneous , Alopecia , Drug Delivery Systems
Electrochemiluminescence (ECL) as an analytical technology with a perfect combination of electrochemistry and spectroscopy has received considerable attention in bioanalysis due to its high sensitivity and broad dynamic range. Given the selectivity of bio-recognition elements and the high sensitivity of the ECL analysis technique, ECL biosensors are powerful platforms for the sensitive detection of biomarkers, achieving the accurate prognosis and diagnosis of diseases. MicroRNAs (miRNAs) are crucial biomarkers involved in a variety of physiological and pathological processes, whose aberrant expression is often related to serious diseases, especially cancers. ECL biosensors can fulfill the highly sensitive and selective requirements for accurate miRNA detection, prompting this review. The ECL mechanisms are initially introduced and subsequently categorize the ECL biosensors for miRNA detection in terms of the quenching agents. Furthermore, the work highlights the signal amplification strategies for enhancing ECL signal to improve the sensitivity of miRNA detection and finally concludes by looking at the challenges and opportunities in ECL biosensors for miRNA detection.
An efficient separation technology involving ammonia (NH3) and carbon dioxide (CO2) is of great importance for achieving low-carbon economy, environmental protection, and resource utilization. However, directly separating NH3 and CO2 for ammonia-based CO2 capture processes is still a great challenge. Herein, we propose a new strategy for selective separation of NH3 and CO2 by functional hybrid membranes that integrate polyimide (PI) and ionic liquids (ILs). The incorporated protic IL [Bim][NTf2] is confined in the interchain segment of PI, which decreases the fractional free volume and narrows the gas transport channel, benefiting the high separation selectivity of hybrid membranes. At the same time, the confined IL also provides high NH3 affinity for transport channels, promoting NH3 selective and fast transport owing to strong hydrogen bonding interaction between [Bim][NTf2] and NH3 molecules. Thus, the optimal hybrid membrane exhibits an ultrahigh NH3/CO2 ideal selectivity of up to 159 at 30 °C without sacrificing permeability, which is 60 times higher than that of the neat PI membrane and superior to the state-of-the art reported values. Moreover, the introduction of [Bim][NTf2] also reduces the permeation active energy of NH3 and reverses the hybrid membrane toward "NH3 affinity", as understood by studying the effect of temperature. Also, NH3 molecules are much easier to transport at high temperature, showing great application potential in direct NH3/CO2 separation. Overall, this work provides a promising ultraselective membrane material for ammonia-based CO2 capture processes.
The second near-infrared (NIR-II) window laser-activated agents have attracted broad interest in an orthotopic cancer theranostic. However, developing NIR-II photothermal agents (PTAs) with advanced photothermal conversion efficiency (PTCE) and tumor-specific response elevation remains a crucial challenge. Herein, a hollow gold nanorod (AuHNR) with a strong localized surface plasmon resonance (LSPR) peak in the NIR-II window was coated with MnO2 and chitosan to obtain AuHNR@MnO2@CS (termed AuMC) by a one-step method. Upon exposure to the tumor microenvironment (TME), the overexpressed GSH triggered degradation of the MnO2 layer to release Mn2+ and resulted in the PTCE elevation owing to exposure of the AuHNR. Consequently, photoacoustic and magnetic resonance imaging for accurate diagnosis, Mn2+-mediated chemodynamic therapy, and AuHNR elevating PT therapy for precise treatment could be achieved. Both in vitro and in vivo experiments confirmed the good performance of the AuMC on an orthotopic bladder cancer precise theranostic. This study provided NIR-II activated, TME-response PT conversion efficiency enhanced PTAs and offered a tumor-selective theranostic agent for orthotopic bladder cancer in clinical application.
Paraffin and octadecyltrichlorosilane (OTS) coatings can alleviate collisions between alkali-metal atoms and cell walls and then prolong the atomic spin-polarization lifetime. The surface structure and collision effects of these antirelaxation coatings, as well as the methods to avoid antirelaxation invalidity, have been the focus of researchers. This study investigated the thermolability of coating surface structure and the collision interactions between alkali metal atoms and coatings, considering the influence of various coating preparation factors, where this collision interaction is indirectly analyzed by measuring the collision energy dissipation between an atomic force microscopy (AFM) probe and the atoms on the coating surface. We found that appropriate evaporation time, carbochain length, and postannealing process can enhance the thermostability of the paraffin coating and eliminate its morphological defects. Furthermore, the OTS/water concentration, the soaking time, and the type of solvent have different levels of influence on the cluster formation and the thermostability of the OTS coatings. Moreover, the antirelaxation performance of coatings has been shown to be characterized by counting the energy dissipated when the AFM probe collides with the antirelaxation coating, replacing the conventional light-atom interaction- based method for measuring the relaxation characteristics, but requiring specific coating preparation factors to be maintained.
Controllable self-assembly of the DNA-linked gold nanoparticle (AuNP) architecture for in vivo biomedical applications remains a key challenge. Here, we describe the use of the programmed DNA tetrahedral structure to control the assembly of three different types of AuNPs (â¼20, 10, and 5 nm) by organizing them into defined positioning and arrangement. A DNA-assembled "core-satellite" architecture is built by DNA sequencing where satellite AuNPs (10 and 5 nm) surround a central core AuNP (20 nm). The density and arrangement of the AuNP satellites around the core AuNP were controlled by tuning the size and amount of the DNA tetrahedron functionalized on the core AuNPs, resulting in strong electromagnetic field enhancement derived from hybridized plasmonic coupling effects. By conjugating with the Raman molecule, strong surface-enhanced Raman scattering photoacoustic imaging signals could be generated, which were able to image microRNA-21 and tumor tissues in vivo. These results provided an efficient strategy to build precision plasmonic superstructures in plasmonic-based bioanalysis and imaging.
Metal Nanoparticles , MicroRNAs , Nanostructures , Neoplasms , Photoacoustic Techniques , Humans , Gold/chemistry , Metal Nanoparticles/chemistry , Spectrum Analysis, Raman/methods , DNA/chemistry , Neoplasms/diagnostic imaging
The principal hallmark of Alzheimer's disease (AD) is neuron mitochondrial dysfunction, whereas mitochondrial miRNAs potentially play important roles. Nevertheless, efficacious mitochondria organelle therapeutic agents for treatment and management of AD are highly advisable. Herein, we report a multifunctional DNA tetrahedron-based mitochondria-targeted therapeutic platform, termed tetrahedral DNA framework-based nanoparticles (TDFNs), which was modified with triphenylphosphine (TPP) for mitochondria-targeting, cholesterol (Chol) for crossing the central nervous system, and functional antisense oligonucleotide (ASO) for both AD diagnosis and gene silencing therapy. After injecting intravenously through the tail vein of 3 × Tg-AD model mice, TDFNs can both easily cross the blood brain barrier and accurately arrive at the mitochondria. The functional ASO could not only be detected via the fluorescence signal for diagnosis but also mediate the apoptosis pathway through knocking miRNA-34a down, leading to recovery of the neuron cells. The superior performance of TDFNs suggests the great potential in mitochondria organelle therapeutics.
Alzheimer Disease , MicroRNAs , Mice , Animals , Alzheimer Disease/drug therapy , Alzheimer Disease/metabolism , MicroRNAs/genetics , MicroRNAs/metabolism , Mitochondria/metabolism , Neurons/metabolism , DNA, Mitochondrial/metabolism
Multiplexed microRNA (miRNA) profiling of more than four types in living cells is challenging due to fluorescent spectral overlap, representing a significant limitation in studying the complex interactions related to the occurrence and development of diseases. Herein, we report a multiplexed fluorescent imaging strategy based on an orthometric multicolor encoded hybridization chain reaction amplifier named multi-HCR. The targeting miRNA can trigger this multi-HCR strategy due to the specific sequence recognition, and then its self-assembly to amplify the programmability signals. We take the four-colored chain amplifiers, showing that the multi-HCR can form 15 combinations simultaneously. In a living process of hypoxia-induced apoptosis and autophagy under complicated mitochondria and endoplasmic reticulum stress, the multi-HCR demonstrates excellent performance in detecting eight different miRNA changes. The multi-HCR provides a robust strategy for simultaneously profiling multiplexed miRNA biomarkers in studying complicated cellular processes.
Since their first discovery in 1994, DNAzymes have been extensively applied in biosensing and therapy that act as recognition elements and signal generators with the outstanding properties of good stability, simple synthesis, and high sensitivity. One subset, RNA-cleaving DNAzymes, is widely employed for diverse applications, including as reporters capable of transmitting detectable signals. In this review, the recent advances of RNA-cleaving DNAzyme-based amplification strategies in scaled-up biosensing are focused, the application in diagnosis and disease treatment are also discussed. Two major types of RNA-cleaving DNAzyme-based amplification strategies are highlighted, namely direct response amplification strategies and combinational response amplification strategies. The direct response amplification strategies refer to those based on novel designed single-stranded DNAzyme, and the combinational response amplification strategies mainly include two-part assembled DNAzyme, cascade reactions, CHA/HCR/RCA, DNA walker, CRISPR-Cas12a and aptamer. Finally, the current status of DNAzymes, the challenges, and the prospects of DNAzyme-based biosensors are presented.
Biosensing Techniques , DNA, Catalytic , DNA , Oligonucleotides , RNA
The interstitial fluid (ISF) contains rich bioinformation for disease diagnosis and healthcare monitoring. However, the efficient sampling and detection of the biomolecules in ISF is still challenging. Herein, we develop a facile but versatile ISF analysis platform by combining controllable hollow microneedles (HMNs) and elaborate microfluidic paper-based analytical devices (µPADs). The HMNs and µPADs was fixed in a bottom PDMS layer. A top PDMS layer containing a cylindrical cavity to produce negative pressure for sampling was packaged on the bottom PDMS layer. The HMNs enable efficient and swift sampling of sufficient ISF to the µPADs through one-touch finger operation without extra manipulations. The µPADs realized to simultaneously detect glucose and lactic acid in the detection area to produce chromogenic agents and analyzed by the self-programed RGB application (APP) in smartphones. The HMN microfluidic paper-based chip provides a point-of-care platform for accurate detection of biomolecules in ISF, holding great promise in the development of wearable device.
Microfluidic Analytical Techniques , Microfluidics , Extracellular Fluid/chemistry , Colorimetry , Glucose/analysis , Needles , Paper
Mitochondria-targeted therapeutics are an attractive approach against energy-dependent cancer. However, effective mitochondria organelle therapeutics agents are still highly desirable. Herein, a mitochondria-targeted therapeutics platform, termed CDM@MUiO-DP@MCHM, consisting of macrophages-cancer hybrid membrane (MCHM) encapsulated MUiO-66 metal-organic frameworks (MOFs) is reported, which is loaded with microRNA (miRNA) biomarker detection probe (DP) for cancer diagnosis and copper-depleting moiety (CDM) for mitochondrial copper depletion to suppress cancer growth. Using nude mice bearing MCF-7 as model, after injecting intravenously via the caudal vein of mice, the encapsulation of MCHM can not only greatly enhance the cancer homing-targeting ability of the nanoparticles (NPs) but also endows the NPs the immune escape capacity to extend the circulation time. The miRNA-21 biomarker can be detected by the fluorescence signal for diagnosis, while the CDM induced energy deficiency and compromised mitochondria membrane potential, leading to apoptosis of the cancer cell. The good performance of CDM@MUiO-DP@MCHM suggest the great potential mitochondria organelle therapeutics.
Metal-Organic Frameworks , MicroRNAs , Nanoparticles , Neoplasms , Animals , Mice , Copper/pharmacology , Mice, Nude , Neoplasms/drug therapy , Mitochondria , MicroRNAs/pharmacology
Rapid, simple, sensitive and reliable approaches for biogenic amines quantification in various food samples are essential to food safety. Lateral flow immunoassay (LFIA) has been wildly utilized in point-of-care testing (POCT) owing to its advantage of flexibility and feasibility. Here, we reported a Fe3O4@Au nanoparticles (NPs) (Fe3O4@AuNPs) based multimodal readout LFIA for rapid putrescine (Put) and histamine (His) quantification with a LOD down to 10 and 10 ng/mL in naked eye mode, 2.31 and 4.39 ng/mL in photothermal mode, 0.17 and 0.31 ng/mL in magnetic mode, respectively. Such multi-mode assay has been successfully used to detect Biogenic amines (BAs) in raw aquatic foods, including fish, prawns, beef, and pork, with overall recoveries ranging from 93.68 to 109.34%. Meanwhile, it is easily expanded to detect other typical BAs with high sensitivity by simply replacing antibodies. In view of the multi-signal reading, two quantitative formats, and high sensitivity, it may greatly widen the application of lateral flow detection in food safety.
Metal Nanoparticles , Animals , Cattle , Gold , Colorimetry , Immunoassay , Putrescine , Magnetic Phenomena , Limit of Detection , Biogenic Amines
Antibiotic resistance of bacteria and persistent inflammation are critical challenges in treating bacteria infected wounds. Thus, it is urgent to develop versatile wound dressings that possess high-efficiency antibacterial performance and inflammation regulation. Herein, we have successfully constructed a hydrogel wound dressing consisting of the bimetallic metal-organic framework (MOF) loaded with glucose oxidase (GOx), termed as MOF(Fe-Cu)/GOx-polyacrylamide (PAM) gel. Hydrogel dressings can provide an efficient cascade-catalyzed system to accelerate wound healing via synergistic antibacterial and inflammatory modulation. Importantly, the catalytic property of the bimetallic MOF(Fe-Cu) is about five times that of the monometallic MOF(Fe). Based on such a cascade-catalyzed system, the abundant gluconic acid and H2O2 can be continuously produced by decomposing glucose via GOx. Such gluconic acid can notably improve the peroxidase performance of MOF(Fe-Cu), which can further efficiently decompose H2O2 to achieve the antibacterial. Meanwhile, MOF (Fe Cu)/GOx PAM gel can induce macrophages to change into an M2 phenotype, which can accelerate the transformation of the wound microenvironment to a remodeling state and then accelerate angiogenesis and neurogenesis. This work provides multifunctional bioactive materials for accelerating wound healing and will have great potential in clinical applications. STATEMENT OF SIGNIFICANCE: Antibiotic resistance and persistent inflammation are still the critical reasons for the slow healing of bacteria infected wounds. Herein, we prepared a hydrogel wound dressing composed of bimetallic metal organic framework (MOF) loaded with glucose oxidase (GOx). The catalytic activity of the bimetallic MOF(Fe-Cu) is significantly enhanced due to doping of copper, which makes it possess outstanding antibacterial ability based on cascade catalysis. Such dressing can promote the remodeling of inflammatory immunity by regulating macrophage polarization to suppress over-reactive inflammation, further accelerating the healing of bacteria-infected wounds. This study provides an innovative and effective way to accelerate the healing of bacteria infected wound by combining bacteria killing and inflammation modulation.
Glucose Oxidase , Hydrogels , Humans , Glucose Oxidase/pharmacology , Hydrogels/pharmacology , Hydrogen Peroxide/pharmacology , Anti-Bacterial Agents/pharmacology , Bandages , Inflammation/drug therapy
Optically pumped gradiometers have long been utilized in measurement in the International Geomagnetic Reference Field (IGRF). With advancements in technologies such as laser diodes and microfabrication, integrated gradiometers with compact sizes have become available, enabling improvements in magnetoencephalography and fetal magnetocardiography within shielded spaces. Moreover, there is a growing interest in the potential of achieving biomagnetic source detection without shielding. This review focuses on recent developments in optically pumped magnetic field gradiometers, including various fabrication methods and measurement schemes. The strengths and weaknesses of different types of optically pumped gradiometers are also analyzed.
Metal-organic frameworks (MOF) have attracted great potential in sonodynamic therapy (SDT) owing to large sonosensitizers' loading and fast reactive oxygen species' (ROS) diffusion; however, the low ligand-to-metal charge transfer efficiency sharply impairs the SDT effect. Herein, we report the design of MIL@Ag heterostructures with high electron-hole pairs separation efficiency and enhanced diverse ROS generation ability for deep-seated cancer treatment and bacterial infection. The MIL@Ag heterostructure is composed of Ti-based MOFs (named MIL), on which are in situ assembled silver nanoparticles (Ag NPs). The electrochemical experiments and density functional theory calculations verify that the introduction of Ag NPs can significantly improve the electron transfer efficiency and O2 adsorption capacity of MIL. Under ultrasound irradiation, the doped Ag NPs can trap the activated electrons from MIL to reduce surrounding O2 and produce superoxide radicals (â¢O2-), while the activated holes enable oxidizing H2O to produce hydroxyl radicals (â¢OH). Thus, they efficiently improve the therapeutic efficiency of SDT. MIL@Ag-PEG-mediated SDT implements A549 cancer cells' killing under a tissue barrier of 2 cm and eradicates the bacterial infection of Staphylococcus aureus, thus promoting wound healing. Therefore, MIL@Ag-PEG provides a promising strategy for augmenting SDT performance by rational heterostructure design of sonosensitizers.
