Enhanced photocatalytic CO2 conversion over 0D/2D CsPbBr3/BiOCl S-scheme heterojunction via boosting charge separation.

The stable contact of heterogeneous interfaces and the substantial exposure of active sites are crucial for enhancing the photocatalytic performance of semiconductor catalysts. However, most reported two-dimensional (2D)/2D CsPbBr3 and BiOCl heterostructures are fabricated using electrostatic self-assembly methods, which exhibit significant deficiencies in precise interface quality control and effective active site exposure. In this study, we fabricate a zero-dimensional (0D)/2D CsPbBr3/BiOCl heterojunction via a two-step calcination method, achieving an efficient direct S-scheme configuration. Optimizing interfacial contact and band alignment between CsPbBr3 quantum dots and BiOCl nanosheets enhances cross-plane charge transfer, promoting superior charge separation. This 0D/2D CsPbBr3/BiOCl heterojunction exhibits enhanced carrier mobility and high conversion rates without cocatalysts or sacrificial agents. The mechanism underlying the accelerated S-scheme charge transfer is comprehensively elucidated through a combination of analytical techniques and density functional theory (DFT) calculations. This study offers a novel approach for managing charge carrier segregation and mobility in CO2 reduction photocatalysts.

Inhibition of Norovirus GII.4 binding to HBGAs by Sargassum fusiforme polysaccharide.

Norovirus (NoV) is the main pathogen that causes acute gastroenteritis and brings a heavy socio-economic burden worldwide. In this study, five polysaccharide fractions, labeled pSFP-1-5, were isolated and purified from Sargassum fusiforme (S. fusiforme). In vitro experiments demonstrated that pSFP-5 significantly prevented the binding of type A, B and H histo-blood group antigens (HBGAs) to NoV GII.4 virus-like particles (NoV GII.4 VLPs). In addition, in vivo experiments revealed that pSFP-5 was effective in reducing the accumulation of NoV in oysters, indicating that pSFP-5 could reduce the risk of NoV infection from oyster consumption. The results of transmission electron microscopy showed that the appearance of NoV GII.4 VLPs changed after pSFP-5 treatment, indicating that pSFP-5 may achieve antiviral ability by altering the morphological structure of the viral particles so that they could not bind to HBGAs. The results of the present study indicate that pSFP-5 may be an effective anti-NoV substance and can be used as a potential anti-NoV drug component.

Au NPs modified Ni-B nanosheets/graphene oxide three-dimensional network as label-free electrochemical immunosensor for the detection of diethylstilbestrol.

Three-dimensional (3D) network provide a promising platform for construction of high sensitive electrochemical immunosensor due to the benefits of high specific surface area and electron mobility. Herein, a sensitive label-free electrochemical immunosensor based on Au nanoparticles modified Ni-B nanosheets/graphene matrix was constructed to detect diethylstilbestrol (DES). The 3D network not only could increase the electron transport rate and surface area, but also could provide confinement area, which is conducive to increases the collision frequency with the active site. Moreover, Au NPs also have good biocompatibility, which is beneficial for ligating antibodies. Benefiting from the 3D network structure and Au collective effect, the electrochemical immunosensor possess sterling detection ability with wide linear response range (0.00038-150 ng/mL) and low detection limit (31.62 fg/mL). Moreover, the constructed immunosensor can also be extend to detect DES in Tap-water and river water. This work may provide a novel material model for the construction of high sensitive immunosensor.

Dual-responsive electrochemical immunosensor for CYFRA21-1 detection based on Au/Co Co-loaded 3D ordered macroporous carbon interconnected framework.

Cytokeratin 19 fragment antigen 21-1 (CYFRA21-1) is a protein fragment released into the bloodstream during the death of lung epithelial cells, serving as a predictive biomarker in diagnosing non-small cell lung cancer (NSCLC) and need to be accurately detected. Herein, a dual-responsive label-free electrochemical immunosensor was developed based on a three-dimensional ordered interconnecting macroporous carbon skeleton material modified with gold-cobalt nanoparticles (Au/Co NPs-3D MCF) to detect cytokeratin-19 fragment (CYFRA21-1). The three-dimensional ordered interconnect macroporous structure, by providing a high specific surface area and an electrochemically active area, not only enhances the electron transport channel and reduces mass transfer resistance, but also offers a confined region that elevates the collision frequency with the active site. In addition to exhibiting excellent biocompatibility for antibody binding, gold-cobalt nanoparticles contribute significantly to the overall robustness of the immunosensor. By capitalizing on the 3D network structure and collective effect of Au and Co NPs, the Au/Co NPs-3D MCF immunosensors exhibit exceptional response signals in both chronocurrent testing and square-wave voltammetry, allowing for a wide linear response range of 0.0001-100 ng/mL and a low detection limit. Moreover, the constructed immunosensor is capable of detecting CYFRA21-1 in human serum and has the potential for further extension to detect multiple biomarkers. This work opens up new avenues for the construction of other highly selective 3D network immunosensors.

A dual-mode label-free electrochemical immunosensor for ultrasensitive detection of procalcitonin by on-site vulcanization of dual-MOF heterostructure.

Detection of procalcitonin (PCT) is crucial for the early identification of sepsis. PCT is primarily utilized in the multiple diagnosis of bacterial and viral illnesses along with to guide the application of antibiotics. Considering their advantages of high specificity and straightforward usage, electrochemical immunosensors offer significant application prospects in the detection of disease indicators. A dual-mode electrochemical immunosensor was constructed in this study to reliably identify PCT. In light of the synergistic effect of the dual-MOF derived heterostructure, the immunosensor demonstrating excellent square wave voltammetry (SWV) signals as well as significant catalytic activity for the H2O2 redox process. In addition to maintaining a low detection limit (SWV: 0.31 fg/mL and i-t: 0.098 fg/mL), the immunosensor offers an extensive linear response range (0.000001-100 ng/mL). The excellent performance is on account of the introduction of the local on-site sulfurized dual-MOF heterostructure with abundant metal chalcogenides/MOF interfaces, which boosts the specific surface area, offers an abundance of active sites, enhances conductivity, and raises catalytic activity. Furthermore, the immunosensor exhibits outstanding specificity, stability and reproducibility for the determination of PCT in serum, which is of great crucial for the clinical screening and diagnosis of sepsis.

Bionic nanotheranostic for multimodal imaging-guided NIR-II-photothermal cancer therapy.

In photothermal therapy (PTT), the photothermal conversion of the second near-infrared (NIR-II) window allows deeper penetration and higher laser irradiance and is considered a promising therapeutic strategy for deep tissues. Since cancer remains a leading cause of deaths worldwide, despite the numerous treatment options, we aimed to develop an improved bionic nanotheranostic for combined imaging and photothermal cancer therapy. We combined a gold nanobipyramid (Au NBP) as a photothermal agent and MnO2 as a magnetic resonance enhancer to produce core/shell structures (Au@MnO2; AM) and modified their surfaces with homologous cancer cell plasma membranes (PM) to enable tumour targeting. The performance of the resulting Au@MnO2@PM (AMP) nanotheranostic was evaluated in vitro and in vivo. AMP exhibits photothermal properties under NIR-II laser irradiation and has multimodal in vitro imaging functions. AMP enables the computed tomography (CT), photothermal imaging (PTI), and magnetic resonance imaging (MRI) of tumours. In particular, AMP exhibited a remarkable PTT effect on cancer cells in vitro and inhibited tumour cell growth under 1064 nm laser irradiation in vivo, with no significant systemic toxicity. This study achieved tumour therapy guided by multimodal imaging, thereby demonstrating a novel strategy for the use of bionic gold nanoparticles for tumour PTT under NIR-II laser irradiation.

Research Progress on Biological Accumulation, Detection and Inactivation Technologies of Norovirus in Oysters.

Noroviruses (NoVs) are major foodborne pathogens that cause acute gastroenteritis. Oysters are significant carriers of this pathogen, and disease transmission from the consumption of NoVs-infected oysters occurs worldwide. The review discusses the mechanism of NoVs bioaccumulation in oysters, particularly the binding of histo-blood group antigen-like (HBGA-like) molecules to NoVs in oysters. The review explores the factors that influence NoVs bioaccumulation in oysters, including temperature, precipitation and water contamination. The review also discusses the detection methods of NoVs in live oysters and analyzes the inactivation effects of high hydrostatic pressure, irradiation treatment and plasma treatment on NoVs. These non-thermal processing treatments can remove NoVs efficiently while retaining the original flavor of oysters. However, further research is needed to reduce the cost of these technologies to achieve large-scale commercial applications. The review aims to provide novel insights to reduce the bioaccumulation of NoVs in oysters and serve as a reference for the development of new, rapid and effective methods for detecting and inactivating NoVs in live oysters.

Ultrathin Rh Nanosheets with Rich Grain Boundaries for Efficient Hydrogen Oxidation Electrocatalysis.

Two-dimensional (2D) Pt-group ultrathin nanosheets (NSs) are promising advanced electrocatalysts for energy-related catalytic reactions. However, improving the electrocatalytic activity of 2D Pt-group NSs through the addition of abundant grain boundaries (GBs) and understanding the underlying formation mechanism remain significant challenges. Herein, we report the controllable synthesis of a series of Rh-based nanocrystals (e.g., Rh nanoparticles, Rh NSs, and Rh NSs with GBs) through a CO-mediated kinetic control synthesis route. In light of the 2D NSs' structural advantages and GB modification, the Rh NSs with rich GBs exhibit an enhanced electrocatalytic activity compared to pure Rh NSs and commercial Pt/C toward the hydrogen oxidation reaction (HOR) in alkaline media. Both experimental results and theoretical computations corroborate that the GBs in the Rh NSs have the capacity to ameliorate the adsorption free energy of reaction intermediates during the HOR, thus resulting in outstanding HOR catalytic performance. Our work offers novel perspectives in the realm of developing sophisticated 2D Pt-group metal electrocatalysts with rich GBs for the energy conversion field.

Dual-targeting nanotheranostics for MRI-guided enhanced chemodynamic therapy of hepatoma via regulating the tumor microenvironment.

Chemodynamic therapy (CDT), as a reactive oxygen species (ROS)-based therapeutic modality, has attracted much attention in recent years. However, the insufficient therapeutic effect of CDT is due to the antioxidant system in the tumor microenvironment, such as high levels of glutathione (GSH). In this study, we developed a biological/physical dual-targeting nanotheranostic agent (relaxation rate, r1: 6.3 mM-1 s-1 and r2: 13.11 mM-1 s-1) for enhanced CDT of SMCC-7721 tumors. This nanotheranostic agent is composed of a homologous tumor cell membrane (TCM), magnetic ferric oxide, and manganese oxide and is denoted as FM@TCM nanoparticles (NPs). A favorable effect of in vitro CDT on SMCC-7721 cells (IC50: 20 µg mL-1) is demonstrated, attributed to the Fenton reaction and oxidative stress resulting from the reduction of the GSH level. In vivo T1/T2 magnetic resonance imaging (MRI) confirms that the tumor accumulation of FM@TCM NPs is promoted by concurrent bioactive targeting of the homologous TCM and physico-magnetic targeting of tumor tissues with an external magnetic field. Impressive chemodynamic therapeutic effects on SMCC-7721 tumors are demonstrated through the catalysis of endogenous hydrogen peroxide and depletion of GSH to generate high levels of ROS. Dual-targeting FM@TCM NPs inhibit SMCC-7721 tumor growth (∼90.9%) in vivo without any biotoxicity. This nanotheranostic agent has great potential for use in MRI-guided CDT.

Principal component analysis-artificial neural network-based model for predicting the static strength of seasonally frozen soils.

Seasonally frozen soils are exposed to freeze‒thaw cycles every year, leading to mechanical property deterioration. To reasonably describe the deterioration of soil under different conditions, machine learning (ML) technology is used to establish a prediction model for soil static strength. Six key influencing factors (moisture content, compaction degree, confining pressure, freezing temperature, number of freeze‒thaw cycles and thawing duration) are included in the modelling database. The accuracy of three typical ML algorithms (support vector machine (SVM), random forest (RF) and artificial neural network (ANN)) is compared. The results show that the ANN outperforms the SVM and RF. Principal component analysis (PCA) is combined with the ANN, and the PCA-ANN algorithm is proposed, which further improves the prediction accuracy. The deterioration of soil static strength is systematically researched using the PCA-ANN algorithm. The results show that the soil static strength decreased considerably after the first several freeze‒thaw cycles before the strength plateau occurred, and the strength reduction increased significantly with increasing moisture content and compaction degree. The PCA-ANN model can generate a reasonable prediction for the static strength or other soil properties of seasonally frozen soil, which will provide a scientific reference for practical engineering.

Green and Low-temperature Synthesis of Carbon Dots for Simple Detection of Kaempferol.

As a common flavonols, kaempferol (Kae) has a broad market as health food and medicine for its anti-inflammatory, anti-oxidation, and anti-cancer properties. In this study, a novel convenient and simple fluorescent sensor based on carbon dots (CDs) for the detection of Kae was developed. The fluorescent CDs, with excellent photo-luminescence (PL) and up-conversion luminescence (UCPL) properties, were successfully prepared by low-temperature oil bath reaction based on ascorbic acid as carbon source at 90 °C in one pot. Under the optimal conditions, the fluorescence (FL) intensity of CDs was gradually quenched by the increasing addition of Kae with a linear relationship between F0/F and Kae concentration in a wide range from 5 µM to 100 µM with a detection limit of 0.38 µM. And this designed sensor was favourably applied for the detection of Kae in actual sample (xin-da-kang tablets). Moreover, the proposed CDs has great application prospects as a drug-sensor for detecting Kae due to its simple operation, economical and green materials, low equipment requirement, and rapid detection.

Tuning Electron Transfer in Atomic-Scale Pt-Supported Catalysts for the Alkaline Hydrogen Oxidation Reaction.

Developing efficient atomic-scale metal-supported catalysts is of great significance for energy conversion technologies. However, the precise modulation of electron transfer between the metal and supporter in atomic-scale metal-supported catalysts to further improve the catalytic activity is still a major challenge. Herein, we show tunable electron transfer between atomic-scale Pt and tungsten nitride/oxide supports (namely, Pt/WN and Pt/W18O49). Pt/WN with modest electron exchange and Pt/W18O49 with aggressive electron exchange exhibit notably different catalytic activities for the alkaline hydrogen oxidation reaction (HOR), in which Pt/WN shows a 5.7-fold enhancement in HOR intrinsic catalytic performance in comparison to Pt/W18O49. Additionally, the tunable electronic transfer at the interface of Pt/WN and Pt/W18O49, as proven by the theoretical calculation, resulted in the discrepancy of the adsorption free energy of the reaction intermediates, as well as catalytic activity, for the HOR process. Our work provides new insights into the design of advanced atomic-scale metal-supported catalysts for electrocatalysis.

Ru Colloidosome Catalysts for the Hydrogen Oxidation Reaction in Alkaline Media.

Developing efficient hydrogen oxidation reaction (HOR) electrocatalysts in alkaline media is of great significance for anion exchange membrane fuel cells. Herein, we report the synthesis of hollow colloidosomes composed of Ru nanocrystals based on a novel gas/liquid interface self-assembly strategy. Structural characterizations reveal that much defects are present in the building block (Ru nanocrystals) of Ru colloidosomes. Theoretical calculations suggest that the defects in the Ru structure can optimize the adsorption binding energy of reaction intermediates for the HOR. Benefiting from the assembled colloidosome and optimized electronic structure, the Ru colloidosomes exhibit remarkable HOR catalytic performance in alkaline media with a mass activity higher than that of benchmark Pt/C. Our work may shed new light on the rational design of advanced electrocatalysts with an assembled structure for energy-related applications.

Retraction Notice to: MicroRNA-199a-5p accelerates nucleus pulposus cell apoptosis and IVDD by inhibiting SIRT1-mediated deacetylation of p21.

[This retracts the article DOI: 10.1016/j.omtn.2021.02.009.].

Ultrathin covalent and cuprophilic interaction-assembled copper-sulfur monolayer in organic metal chalcogenide for oriented photoconductivity.

We report the thinnest copper sulfur atomic monolayer in an organic copper chalcogenide [Cu(CMP)]n (CMP = 5-chloro-2-mercaptopyridine). The layer features a new type of copper sulfur structure woven by both covalent bond and cuprophilic interaction and shows an intriguing oriented photoconductivity.

Encapsulated ruthenium nanoparticles activated few-layer carbon frameworks as high robust oxygen evolution electrocatalysts in acidic media.

Noble metals have been extensively employed as high active catalysts for oxygen evolution reaction (OER), are usually subjected to serious surface transformation and poor structural stability, especially in acid media, which need imperatively remedied. Herein, the interfacial engineering of Ru via few-layer carbon (Ru@FLC) was carried out, in which FLC can significantly suppress the corrosion of Ru in acid media, ensuring the efficient interfacial charge transport between Ru and FLC. As a result, a low overpotentials@10 mA cm-2 of 258 mV and small Tafel slopes of 53.1 mV dec-1 for oxygen evolution OER were achieved in acid media. DFT calculations disclose that outer FLC could induce charge redistribution and effectively optimize intermediates free energy adsorption, resulting in greatly reduce the energy barrier for OER. Our work may offer a new avenue to produce progressive OER electrocatalysts for energy-related applications in acid solution.

A universal route with fine kinetic control to a family of penta-twinned gold nanocrystals.

Some of the major difficulties hindering the synthesis of different types of colloidal nanocrystals are their complex synthetic methods and the lack of a universal growth mechanism in one system. Herein, we propose a general strategy of kinetically controlled seed-mediated growth to synthesize a family of penta-twinned gold nanocrystals. Specifically, different kinds of penta-twinned nanocrystals (truncated penta-twinned decahedra, truncated bipyramids, bipyramids, truncated bipyramids with tips, star-like penta-twinned nanocrystals, decahedra with concave edges, and decahedra) with tunable sizes and high purity were readily achieved in one system solely by tailoring the deposition kinetics of adatoms on different sites of decahedral seeds. The controllable deposition kinetics can be realized by changing the ratio of reductant/gold precursors (R), which dictates whether horizontal or vertical features along the 5-fold axis direction of Au decahedral seeds are produced. Additionally, the selective growth of a second metal (silver) on penta-twinned gold seeds can be reached through minor modification of R, which opens a new avenue for mechanistic investigation by visualizing the seed localization within the final particles. The present work demonstrates a general paradigm for the kinetic growth of penta-twinned crystals and would be extended to the synthesis of other families of nanocrystals.

Nitrogen-Doped Cobalt Diselenide with Cubic Phase Maintained for Enhanced Alkaline Hydrogen Evolution.

The introduction of heteroatoms is one of the most important ways to modulate the intrinsic electronic structure of electrocatalysts to improve their catalytic activity. However, for transition metal chalcogenides with highly symmetric crystal structure (HS-TMC), the introduction of heteroatoms, especially those with large atomic radius, often induces large lattice distortion and vacancy defects, which may lead to structural phase transition of doped materials or structural phase reconstruction during the catalytic reaction. Such unpredictable situations will make it difficult to explore the connection between the intrinsic electronic structure of doped catalysts and catalytic activity. Herein, taking thermodynamically stable cubic CoSe2 phase as an example, we demonstrate that nitrogen incorporation can effectively regulate the intrinsic electronic structure of HS-TMC with structural phase stability and thus promote its electrocatalytic activity for the hydrogen evolution activity (HER). In contrast, the introduction of phosphorus can lead to structural phase transition from cubic CoSe2 to orthorhombic phase, and the structural phase of phosphorus-doped CoSe2 is unstable for HER.

MicroRNA-199a-5p accelerates nucleus pulposus cell apoptosis and IVDD by inhibiting SIRT1-mediated deacetylation of p21.

Intervertebral disc degeneration (IVDD) is a multifactorial pathological process associated with low back pain in which nucleus pulposus cell senescence is disrupted. Increasing evidence reveals that IVDD can be modulated by microRNAs (miRNAs or miRs). In the current study, we set out to elucidate the role of miR-199a-5p in nucleus pulposus cell apoptosis and IVDD progression. After sample collection, we found highly expressed miR-199a-5p in nucleus pulposus tissues of both patients diagnosed with IVDD and in IVDD rat models. Next, normal and degenerated nucleus pulposus cells were isolated and transfected with miR-199a-5p mimic, miR-199a-5p inhibitor, overexpressed sirtuin 1 (oe-SIRT1), and oe-p21, followed by detection of nucleus pulposus cell apoptosis and proliferation. In addition, the binding of miR-199a-5p and SIRT1, the interaction between p21 and SIRT1, and the regulation of p21 acetylation by SIRT1 were analyzed. We found that miR-199a-5p overexpression promoted nucleus pulposus cell apoptosis and IVDD. Overexpression of SIRT1 countered the effect of miR-199a-5p overexpression, while overexpression of p21 reversed the effect of miR-199a-5p silencing. Also, miR-199a-5p inhibited SIRT1, promoted p21 acetylation, and upregulated p21 expression, thus accelerating nucleus pulposus cell apoptosis and IVDD. Overall, miR-199a-5p promotes nucleus pulposus cell apoptosis and IVDD by suppressing SIRT1-dependent deacetylation of p21.

Porous CoSe2@N-doped carbon nanowires: an ultra-high stable and large-current-density oxygen evolution electrocatalyst.

Nitrogen doped carbon functionalized CoSe2 nanowires (CoSe2@N-C NWs), which act as potential oxygen evolution reaction (OER) catalysts with a large current density and high stability have been reported. Owing to the collaborative optimization of electrical conductivity, free adsorption energy and binding strength of OER intermediates, the prepared CoSe2@N-C NWs exhibit an enhanced 6.61-fold catalytic activity compared to the pristine CoSe2 NW electrode in 1.0 M KOH solution at the overpotential of 340 mV.