Search

An asymmetrical architecture is developed to discriminate monosaccharide enantiomers based on enzyme-like cascade reactions in homochiral CuMOF pockets. The increased enzyme-like activity under LSPR excitation enhanced the identification performance.

Hydrophobic AuNPs coated TiO2 nanotubes are developed as an interference-free SERSsubstrate. The hydrophobic interaction of volatile metabolites with the hydrocarbon moieties on the SERS substrate lead to a rapid and sensitive bacteria sensing.

Rapid and sensitive detection of bacteria from a complex real media remains a challenge. Herein, we report a visual bacterial sensing assay with excellent specificity, anti-interference ability, and sensitivity based on a surface plasmon resonance (SPR)-enhanced peroxidase (POD) mimetic. The POD mimetic based on Pt nanoparticles (NPs) asymmetrically decorated on Au/TiO

The development of anode materials with high-rate capability is critical to high-power lithium batteries. T-Nb2O5 has been widely reported to exhibit pseudocapacitive behavior and fast lithium storage capability. However, the other polymorphs of Nb2O5 prepared at higher temperatures have the potential to achieve even higher specific capacity and tap density than T-Nb2O5, offering higher volumetric power and energy density. Here, micrometer-sized H-Nb2O5 with rich Wadsley planar defects (denoted as d-H-Nb2O5) is designed for fast lithium storage. The performance of H-Nb2O5 with local rearrangements of [NbO6] octahedra blocks surpasses that of T-Nb2O5 in terms of specific capacity, rate capability, and stability. A wide range variation in valence of niobium ions upon lithiation was observed for defective H-Nb2O5 via operando X-ray absorption spectroscopy. Operando extended X-ray absorption fine structure and ex-situ Raman spectroscopy reveals a large and reversible distortion of the structure in the two-phase region. Computation and ex-situ X-ray diffraction analysis reveals that the shear structure expands along major lithium diffusion pathways and contracts in the direction perpendicular to the shear plane. Planar defects relieve strain through perpendicular arrangements of blocks, minimizing volume change and enhancing structural stability. In addition, strong Li adsorption on planar defects enlarges intercalation capacity. Different from nanostructure engineering, our strategy to modify the planar defects in the bulk phase can effectively improve the intrinsic property. The findings in this work offer new insights into designing fast Li-ion storage materials in micrometer sizes through defect engineering, and the strategy is applicable to the material discovery for other energy-related applications.

There is currently no ideal treatment for osteochondral lesions of the femoral head (OLFH) in young patients.We performed a 1-year single-arm study and 2 additional years of follow-up of patients with a large (defined as3 cm 2 ) OLFH treated with insertion of autologous costal cartilage graft (ACCG) to restore femoral head congruity after lesion debridement. Twenty patients ≤40 years old who had substantial hip pain and/or dysfunction after nonoperative treatment were enrolled at a single center. The primary outcome was the change in Harris hip score (HHS) from baseline to 12 months postoperatively. Secondary outcomes included the EuroQol visual analogue scale (EQ VAS), hip joint space width, subchondral integrity on computed tomography scanning, repair tissue status evaluated with the Magnetic Resonance Observation of Cartilage Repair Tissue (MOCART) score, and evaluation of cartilage biochemistry by delayed gadolinium-enhanced magnetic resonance imaging of cartilage (dGEMRIC) and T2 mapping.All 20 enrolled patients (31.02 ± 7.19 years old, 8 female and 12 male) completed the initial study and the 2 years of additional follow-up. The HHS improved from 61.89 ± 6.47 at baseline to 89.23 ± 2.62 at 12 months and 94.79 ± 2.72 at 36 months. The EQ VAS increased by 17.00 ± 8.77 at 12 months and by 21.70 ± 7.99 at 36 months (p0.001 for both). Complete integration of the ACCG with the bone was observed by 12 months in all 20 patients. The median MOCART score was 85 (interquartile range [IQR], 75 to 95) at 12 months and 75 (IQR, 65 to 85) at the last follow-up (range, 24 to 38 months). The ACCG demonstrated magnetic resonance properties very similar to hyaline cartilage; the median ratio between the relaxation times of the ACCG and recipient cartilage was 0.95 (IQR, 0.90 to 0.99) at 12 months and 0.97 (IQR, 0.92 to 1.00) at the last follow-up.ACCG is a feasible method for improving hip function and quality of life for at least 3 years in young patients who were unsatisfied with nonoperative treatment of an OLFH. Promising long-term outcomes may be possible because of the good integration between the recipient femoral head and the implanted ACCG.Therapeutic Level IV . See Instructions for Authors for a complete description of levels of evidence.

Background: In previous studies, a new Trichinella spiralis serine protease 1.1 (TsSP1.1) was identified in surface proteins of T. spiralis muscle larvae (ML) by proteomics analysis, but its functions in T. spiralis infection are unknown. The aim of this study was to investigate the roles of TsSP1.1 during larval intrusion of gut epithelium. Methods: From January 2019 to March 2021, complete TsSP1.1 cDNA sequence was cloned and expressed in Escherichia coli BL21 at the Department of Parasitology, Medical College of Zhengzhou University, Zhengzhou, China. Expression and location of TsSP1.1 in the parasite were investigated using indirect immunofluorescence assay (IIFA) and Western blotting. The in vitro intestinal epithelium cells (IECs) intrusion assay was used to ascertain the roles of TsSP1.1 during larval intrusion of IECs and gut epithelium. Results: TsSP1.1 was a surface and secretory protein, which was expressed at various T. spiralis stages, and principally localized at cuticle, stichosome and embryos of the nematode. rTsSP1.1 accelerated larval intrusion of IECs, whereas anti-rTsSP1.1 antibodies impeded larval intrusion. The acceleration and inhibtion was dose-dependently related to rTsSP1.1 and anti-TsSP1.1 antibodies. Block of the IIL with anti-rTsSP1.1 serum also impeded larval intrusion of gut mucosa. Conclusion: TsSP1.1 participates in T. spiralis intrusion of gut epithelium.

Enantioselective sensing of chiral molecules is an important issue for both biomedical research and the pharmaceutical industry. Here, an enantioselective photoelectrochemical (PEC) sensor was constructed by integrating TiO2 nanotubes (NTs) with metal-organic frameworks (MOFs) for the identification of enantiomers. TiO2 NTs prepared by electrochemical anodization can not only be used as the PEC platform but also as the metal-ion precursor to react with terephthalic acid (BDC) to form MIL-125(Ti) in situ. A postsynthetic exchange (PSE) method was used for exchanging the ligand of MIL-125 by 2-aminoterephthalic acid (BDC-NH2) for further functionalization. Homochirality was then successfully introduced into achiral MIL-125-NH2 by postsynthetic modification (PSM) with l-histidine (l-His). The resulting homochiral metal-organic frameworks (MOF)-in-NT architecture exhibits excellent discrimination ability for the chiral recognition of 3,4-dihydroxyphenylalanine (l/d-DOPA) enantiomers. Moreover, by adjusting the charge-carrier separation-induced photocurrent variation mechanism, the as-proposed homochiral PEC electrode exhibits a broad application potential for the discrimination of enantiomers. Because of the construction of binder-free monochiral MOF-in-NT structure directly on a Ti-metal substrate, the valuable feature is that the PEC sensing platform can be used directly, thereby providing a stable, simplified, and low-cost sensing device for the recognition of chiral enantiomers.

Enantioselective identification of chiral molecules is important for biomedical and pharmaceutical research. However, owing to identical molecular formulas and chemical properties of enantiomers, signal transduction and amplification are still the two major challenges in chiral sensing. In this study, we developed an enantioselective membrane by integrating homochiral metal-organic frameworks (MOFs) with nanochannels for the sensitive identification and quantification of chiral compounds. The membrane was designed using a TiO2 nanochannel membrane (TiNM) as the metal ion precursor of MOFs (using MIL-125(Ti)) and incorporating l-glutamine (l-Glu) into the framework of MIL-125(Ti). Using 3,4-dihydroxyphenylalanine (DOPA) as the model analyte, the as-prepared homochiral l-Glu/MIL-125(Ti)/TiNM exhibits a remarkable chiral recognition to d-DOPA than l-DOPA. More importantly, benefiting from the highly enlarged surface area and confinement effect provided by the MOFs-in-nanochannel architecture, the discrimination for chiral recognition is largely amplified through the chelation interaction of Fenton-like activity of Fe3+ onto DOPA. Using 2,2'-azino-bis(3-ethylbenzothiazoline-6-sulfonate) (ABTS) as the substrate, the positively charged ABTS•+ product via Fenton-like reaction induces significant ionic transport changes in nanochannels, which in turn provides information about chiral recognition. This innovative signal amplification strategy on homochiral nanochannels might pave a new way for sensitive monitoring and chiral recognition.

As one of the significant intracellular signaling molecules, hydrogen peroxide (H2O2) regulates some vital biological processes. However, it remains a challenge to develop noninvasive electrodes that can be used for sensing trace H2O2 at the cellular level. Here, we evaluated a high-performance solid-state electrochemiluminescence (ECL) H2O2 sensor based on MIL-88B(Fe) nanocrystal-anchored Ti microwires. Semiconducting TiO2 nanotubes (TiNTs) vertically grown around a Ti wire via an anodization technique act as an intrinsic ECL luminophore. By integrating with MIL-88B(Fe), the synergistic effect of the TiO2 luminophore and the remarkable peroxidase-like activity of MIL-88B(Fe) enable the resulting H2O2 sensor an ultrahigh sensitivity featuring a minimum detection limit of 0.1 nM (S/N = 3), long-term stability, high durativity, and wide-range linear response to a concentration of up to 10 mM. To demonstrate the concept of a MIL-88B(Fe)@TiO2 microelectrode for single-cell sensing, the electrode was used to detect intracellular H2O2 in a single cell. Moreover, benefiting from the heterojunction of MIL-88B(Fe)/TiO2, the microelectrode was found to exhibit excellent photocatalytic activity in the visible-light range, that is, the sensor surface can be self-cleaning after a short visible-light treatment. These advanced sensor characteristics involving easy reusability reveal that the MIL-88B(Fe)@TiO2 microelectrode is a new platform for cytosensing. This study provides a new strategy to design semiconductor materials with arbitrary shape and size, allowing for profound applications in biomedical and clinical analysis.

The high cost and easy denaturation of natural enzymes under environmental conditions hinder their practical usefulness in sensing devices. In this study, peroxidase (POD)-like metal-organic frameworks (MOFs) were in situ grown in the nanochannels of an anodized TiO2 membrane (TiO2NM) as an electrochemical platform for multitarget sensing. By directly using a nanochannel wall as the precursor of metal nodes, Ti-MOFs were in situ derived on the nanochannel wall. Benefitting from the presence of bipyridine groups on the ligands, the MOFs in the nanochannels provide plenty of sites for Fe3+ anchoring, thus endowing the resulting membrane (named as Fe3+:MOFs/TiO2NM) with remarkable POD-like activity. Such Fe3+-induced POD-like activity is very sensitive to thiol-containing molecules owing to the strong coordination effect of thiols on Fe3+. Most importantly, the POD-like activity of nanochannels can be in situ characterized by the current-potential (I-V) properties via catalyzing the oxidation of 2,2'-azinobis(3-ethylbenzothiazoline-6-sulfonate) (ABTS) substrate to the corresponding positively charged product ABTS•+. As a proof-of-concept application, the free-standing POD-like membranes were applied as a label-free assay in sensing cysteine, as well as monitoring acetylcholinesterase (AChE) activity through the generated thiol-containing product. Furthermore, based on the toxicity effect of organophosphorus (OP) compounds on AChE, the robust membranes were successfully utilized to evaluate the toxicity of diverse OP compounds. The POD-like nanochannels open up an innovative way to expand the application of nanochannel-based electrochemical sensing platforms in drug inspection, food safety, and environmental pollution.

Taking advantage of the intrinsic photocatalysis of TiO

It is important to detect cancer biomarkers at an early stage of tumor development for the effective diagnosis and treatment of cancer. As a well-known probe for detecting superoxide (·O

The dynamic changes and apical aneurysm formation in apical hypertrophic cardiomyopathy (HCM) have not been specifically described. This study aimed to describe these changes to better understand the progression of apical HCM.Seventy-two patients with apical HCM who underwent at least two cardiac magnetic resonance (CMR) examinations were retrospectively included in this study. The mean interval between the first and last CMR examinations was 50.1 ± 26.8 months (ranging from 4 to 118 months). Compared with the initial values, the left atrial diameter, maximum left ventricular wall thickness and late gadolinium enhancement extent significantly increased (all P 0.05), while the left ventricular ejection fraction significantly decreased (P 0.05), at the latest CMR examination. More importantly, the dynamic process of apical aneurysm formation in apical HCM was observed in a subset of patients, which may follow these four stages: starting with systolic apical cavity obliteration, then broadening of the apical slit in systole, further developing into an apical outpouching, and finally forming an apical aneurysm. Eleven patients experienced adverse cardiovascular events, including new-onset or progressive atrial fibrillation (n = 7), hospitalization with heart failure (n = 3) and implantable cardioverter defibrillator intervention (n = 1), at the time of the latest CMR examination.In the progression of apical HCM, cardiac structure and function will change accordingly. Apical aneurysm formation in apical HCM is a chronic and continuous dynamic process that may follow a 4-step pathway of disease progression.

As an intriguing and intrinsic feature of life, chirality is highly associated with many significant biological processes. Simultaneous recognition and quantification of enantiomers remains a major challenge. Here, a sensitive enantiomer identification device is developed on TiO

A cost-effective, facile, and sensitive fluorescence sensing strategy for Pb2+ ion detection has been developed based on the fluorescence resonance energy transfer (FRET) between carbon quantum dots (CQDs) and Au nanoparticles (NPs). Glutathione (GSH)-synthesized CQDs acted as both the fluorescence donor and the sorbent to extract Pb2+ ions from the solution via Pb-GSH complexes. Pb2+ ions on CQDs reacted with –SH groups on AuNPs to generate sandwich-type Au-PdS-CQDs, leading to a dramatic decrease in the fluorescence of the CQDs. To expand the potential applications of this strategy, we constructed a sensing strategy using self-organized TiO2 nanotube arrays (TiNTs). The high aspect ratio and transparency for light emitted from the CQDs enabled the TiNTs to serve as a sensitive solid visual platform for the highly selective detection of Pb2+ ions with a detection limit as low as 4.1 × 10−8 mg mL−1. More importantly, the long observation length combined with a small volume enabled a sample acquisition volume of only 2.1 × 10−3 μL, which is smaller than the traditional fluorescence analysis in solution and on commercially available test paper, thus endowing this visual platform with the potential for use in single-cell diagnostics.

Infectious diseases caused by bacteria are a global threat to the human health. Here, we propose a solvent “irrigation” technique to endow TiO2 nanotubes (NTs) to precisely modify with functional nanomaterials, and apply them in constructing a near-infrared (NIR) light controlled drug-delivery system for rapid necrosis of bacteria. In this design, the NIR stimuli-responsive functional shell is located on the external tube wall of TiO2 NT; the internal tube wall offers sufficient binding sites for drug loading. Using kanamycin as a model drug, we demonstrate that the reactive oxygen species generated in photocatalysis not only controllably release the loaded drug by scissoring the linked chains, but also effectively compromise bacteria membrane integrity by damaging the cell wall. Benefiting from the damages, antibiotics rapidly enter the bacteria and reach ≥99.9% reduction in Escherichia coli colony within only 2 h. Importantly, such a covalently conjugation-based delivery system can efficiently relieve radical-induced inflammation and cytotoxicity. This study provides an innovative design strategy for engineering delivery systems with tailorable components, enduring stimuli-response by multiple triggers.

The artificial solid-state nanopore/nanochannel based electrochemical sensing technique has demonstrated great advantages such as high sensitivity and minimalized equipment. However, its application is largely hindered by complex routes and high expense for fabrication. Here, we develop low-cost and easily accessible channels based on natural wood and present a pathway to utilize the wood membrane for local electrochemistry applications. Inspired by the natural mineralization of wood, Prussian blue (PB), an artificial peroxidase (POD)-like mimetic, is mineralized in wood channels via a contra-diffusion technique. Using glucose enantiomers (L/D-Glu) as model analysts, a target-activated strategy is used for chiral molecule recognition by combining glucose oxidase (GOx) with PB-modified wood channels. In the as-proposed hybrid channels, GOx catalyzes the oxidation of only D-Glu to gluconic acid and H2O2. These products dramatically activate the POD-like activity of PB and further trigger the oxidation of the uncharged substrate 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonate) (ABTS) to cationic species (ABTS˙+) in the channels. More importantly, benefitting from the confinement effect of the channel and the asymmetrical mineralization of PB, a significantly selective and sensitive identification of D-Glu is achieved. This study provides a promising way to use natural wood as a novel channel membrane to replace artificial channels for constructing electrochemical sensing platforms.

A photocatalysis-enzyme coupled system represents a most promising approach towards artificial photosynthesis and a direct use of solar energy for the synthesis of specific organic molecules or fuel. In contrast to extensively explored semiconductor photocatalysts, studies that successfully combine photocatalytic and enzymatic reactions are rare. In the present work we describe a photocatalyst–enzyme coupled approach that relies on the in situ synthesis of a hierarchically porous (hp) metal–organic framework (here using titania-based MIL-125) formed in the nanochannels of a TiO2 membrane. By engineering the nm-scale pore size in the MOF we achieve trapping of active cytochrome C (CytC). Benefiting from the intrinsic photocatalytic activity of the MOF [MIL-125 (Ti)] we develop a functional photocatalyst–enzyme system that is active under visible light. Moreover, the membrane-based architecture allows for in situ triggering and monitoring of the enzymatic reaction. Therefore, the platform represents not only a nanoscale photocatalytic reactor or device but also allows to monitor and understand photocatalytically coupled enzyme reactions.

The aim of this study was to investigate the characteristics of a novel type C lectin from Trichinella spiralis (TsCTL) and its role in larval invasion of intestinal epithelial cells (IECs). TsCTL has a carbohydrate recognition domain (CRD) of C-type lectin. The full-length TsCTL cDNA sequence was cloned and expressed in Escherichia coli BL21. The results of qPCR, Western blotting and immunofluorescence assays (IFAs) showed that TsCTL was a surface and secretory protein that was highly expressed at the T. spiralis intestinal infective larva (IIL) stages and primarily located at the cuticle, stichosome and embryos of the parasite. rTsCTL could specifically bind with IECs, and the binding site was localized in the IEC nucleus and cytoplasm. The IFA results showed that natural TsCTL was secreted and bound to the enteral epithelium at the intestinal stage of T. spiralis infection. The rTsCTL had a haemagglutinating effect on murine erythrocytes, while mannose was able to inhibit the rTsCTL agglutinating effect for mouse erythrocytes. rTsCTL accelerated larval intrusion into the IECs, whereas anti-rTsCTL antibodies and mannose significantly impeded larval intrusion in a dose-dependent manner. The results indicated that TsCTL specifically binds to IECs and promotes larval invasion of intestinal epithelium, and it might be a potential target of vaccines against T. spiralis enteral stages.

Chiral differentiation is an important topic in diverse fields ranging from pharmaceutics to chiral synthesis. The improvement of sensitivity and the elucidation of the mechanism of chiral recognition are still the two main challenges. Herein, a plasmon-free semiconductive surface-enhanced Raman spectroscopy (SERS) substrate with sensitive chiral recognition ability is proposed for the discrimination of enantiomers. A homochiral environment is constructed by typical π-π stacking between l-tryptophan (l-Trp) and phenyl rings on well-aligned TiO

The increasing organic and microbiological pollutions in fresh water caused by human activities and industrial development have become a global concern nowadays. In this study, three-dimensional (3D) hierarchical FeS

Steam generation via harvesting solar energy is one of the promising approaches for seawater desalination. Nowadays, organic contamination in seawater represents a great challenge that needs to be ...