DNA-Templated Click Ligation Chain Reaction Catalyzed by Heterogeneous Cu2O for Enzyme-Free Amplification and Ultrasensitive Detection of Nucleic Acids.

Nucleic acids play a pivotal role in the diagnosis of diseases. However, rapid, cost-efficient, and ultrasensitive identification of nucleic acid targets still represents a significant challenge. Herein, we describe an enzyme-free DNA amplification method capable of achieving accurate and ultrasensitive nucleic acid detection via DNA-templated click ligation chain reaction (DT-CLCR) catalyzed by a heterogeneous nanocatalyst made of Cu2O (hnCu2O). This hnCu2O-DT-CLCR method is built on two cross-amplifying hnCu2O-catalyzed DNA-templated azide-alkyne cycloaddition-driven DNA ligation reactions that boast a fast reaction rate and a high DNA ligation yield in minutes, enabling rapid exponential amplification of specific DNA targets. This newly developed hnCu2O-DT-CLCR-enabled DNA amplification strategy is further integrated with two signal reporting mechanisms to achieve low-cost and easy-to-use biosensors: an electrochemical sensor through the conjugation of a methylene blue redox reporter to a DNA probe used in hnCu2O-DT-CLCR and a colorimetric sensor through the incorporation of the split-to-intact G-quadruplex DNAzyme encoded into hnCu2O-DT-CLCR. Both sensors are able to achieve specific detection of the intended DNA target with a limit of detection at aM ranges, even when challenged in complex biological matrices. The combined hnCu2O-DT-CLCR and sensing strategies offer attractive universal platforms for enzyme-free and yet efficient detection of specific nucleic acid targets.

Preparation and measurement of a sandwiched Sn atomic beam source for laser resonance ionization mass spectrometry.

Isotope analysis of Sn plays a crucial role in geochemical studies and in monitoring nuclear contamination. Nevertheless, prevalent analytical techniques for examining Sn isotopes encounter the issue of isobaric interference, markedly impacting the accuracy of the test results. Laser resonance ionization mass spectrometry (LRIMS) can effectively overcome the difficulties associated with the isobaric interference inherent in commercial mass spectrometry. In this paper, different amounts of Sn were prepared on Re filaments by electrodeposition and tested via LRIMS. The results showed that the average detection efficiency of LRIMS decreased with increasing total Sn content from 1 µg to 4 µg, and the fluctuations in the test results among the samples increased significantly. Therefore, the electrodeposition process, as well as the composition and morphology of the deposits were characterized by SEM, EDS and XPS; results showed that the degradation of the samples with increasing Sn content was attributed to the complexity of the composition, micro-structure, valence of the deposits, and the interference of various elements. To cope with the anomalies encountered above, the deposits were heat-treated at 600 °C in a hydrogen atmosphere to eliminate detrimental impurities, like Cl, and Sn was effectively reduced to an almost singular atomic state. Furthermore, a titanium layer was covered on the surface of the heat-treated deposit by magnetron sputtering. Ultimately, a highly efficient and stable Sn atomic beam source with a sandwiched structure has been successfully developed and exhibits broad application prospect.

Half-life determination of the ground state decay of 167Tm and 168Tm.

Precise determination of half-lives of 167Tm and 168Tm are important for their application in nuclear medicine diagnostics, nuclear forensics, and other nuclear data measurements. We produced 167Tm and 168Tm sources using an α-particle beam bombarded 165Ho target and a series purification steps. A series of 173 measurements was performed over a period of 44 days using a high-purity germanium (HPGe) detector to track the count rate change as a function of time by following the 207.8 keV and 531.5 keV γ-lines to determine the radioactive decay half-life of 167Tm. The measurement of half-life of 168Tm ground state has been performed using the same HPGe γ-ray spectrometer to observe γ-lines at 198.3 keV, 816.0 keV, 184.3 keV, 741.4 keV and 914.9 keV. Weighted least-squares fits of exponential decay curves were performed for the dataset of each γ-ray emission, with final determined half-lives of 9.250(15) d and 93.41(12) d for 167Tm and 168Tm, respectively. The uncertainty budgets are presented and discussed in detail. Our result of 167Tm half-life is consistent with the Evaluated Nuclear Structure Data File (ENSDF) recommended half-life of 9.25(2) d. The outcome of 168Tm half-life determination is longer than the ENSDF recommended half-life of 93.1(2) d. Further independent measurements would be ideal to resolve the discrepancy.

Cellulose-based biomass composite films for plastic replacement: Synergistic UV shielding, antibacterial and antioxidant properties.

With the gradual increase in environmental awareness and the growing demand for food safety, sustainable and environmentally friendly cellulose-based materials have become a promising alternative to petroleum-based plastics. However, in practice, packaging materials prepared from cellulose-based materials still have some unsatisfactory properties, such as monofunctionality, low transparency, and lack of UV shielding, antibacterial or antioxidant properties. Herein, a novel synthetic strategy is proposed in this paper, specifically, tannic acid (TA), a green natural extract with antibacterial and antioxidant properties, is used as a plasticizer and cross-linker, and oxidized cellulose nanocellulose (TOCN) modified with folic acid (FA) grafting is blended with TA, and cellulose-based biomass thin films with ultraviolet (UV) shielding, antibacterial, and antioxidant properties have been successfully prepared by using a simple vacuum-assisted filtration. The experimental results showed that the films could completely block ultraviolet light at wavelengths of 200-400 nm while providing 81.47 % transparency in the visible spectrum, while the introduction of TA conferred excellent antibacterial and antioxidant capabilities with antioxidant activity of up to 95 %, and also resulted in films with excellent mechanical properties. Therefore, this work provides ideas for the design and manufacture of competitive biomass green packaging materials, laying the foundation for future applications in food packaging.

Multiplexed electrochemical nucleic acid sensor based on visible light-mediated metal-free thiol-yne click reaction for simultaneous detection of different nucleic acid targets.

Simultaneous detection of multiple tumor biomarkers with a simple and low-cost assay is crucial for early cancer detection and diagnosis. Herein, we presented a low-cost and simple assay for multiplexed detection of tumor biomarkers using a spatially separated electrodes strategy. The sensor is fabricated based on a metal-free thiol-yne click reaction, which is mediated by visible light, on commercially available indium tin oxide (ITO) electrodes. Four biomarkers, including p53 DNA, Brca2 DNA, K-ras DNA, and MicroRNA-204 RNA, were used as model analytes, and the corresponding oligonucleotide probes were modified on the desired electrode units sequentially with 530 nm irradiation light in the presence of photosensitizer Eosin Y. By this visible light-mediated coupling reaction, oligonucleotide probe densities of up to 9.2 ± 0.7 × 1010 molecules/cm2 were readily obtained on the ITO electrode surface. The proposed multiplexed E-NA sensor could detect four different nucleic acid targets concurrently without crosstalk among adjacent electrodes and was also successfully applied for detecting targets in a 20% fetal calf serum sample. The detection limits for p53 DNA, Brca2 DNA, K-ras DNA, and MicroRNA-204 RNA were 0.72 nM, 0.97 nM, 2.15 nM, and 1.73 nM, respectively. The developed approach not only has a great potential for developing cost-effective biosensors on affordable substrates for nucleic acid target detection, but also be easily extended to detect other targets by modifying the specific oligonucleotide probes anchored on the electrode.

Preparation of sustainable oxidized nanocellulose films with high UV shielding effect, high transparency and high strength.

UV protection has become crucial as increasing environmental pollution has led to the destruction of the ozone layer, which has a weakened ability to block UV rays. In this paper, we successfully prepared cellulose-based biomass films with high UV shielding effect, high transparency and high tensile strength by graft-modifying oxidized cellulose nanocellulose (TOCN) with folic acid (FA) and borrowing vacuum-assisted filtration. The films had tunable UV shielding properties depending on the amount of FA added. When the FA addition was 20 % (V/V), the film showed 0 % transmittance in the UV region (200-400 nm) and 90.61 % transmittance in the visible region (600 nm), while the tensile strength was up to 150.04 MPa. This study provides a new integrated process for the value-added utilization of nanocellulose and a new route for the production of functional biomass packaging materials. The film is expected to be applied in the field of food packaging with UV shielding.

Selective Adsorption and Recovery of Silver from Acidic Solution Using Biomass-Derived Sulfur-Doped Porous Carbon.

It is vital to recycle precious metals effectively such as silver from waste sources because of limited natural reserves. Herein, passion fruit (Passiflora edulis Sims) shell-derived S-doped porous carbons (SPCs) were newly synthesized by hydrothermal carbonization and following with activation by KOH/(NH4)2SO4, and the adsorption of Ag+ on SPC under acidic solutions was investigated. It was found that the activator of (NH4)2SO4 can not only introduce the doping of S elements but also increase the proportion of mesopores in the as-prepared SPC. As the active site, the increasing S doping can improve the adsorption of Ag+ on SPC. The kinetic data of Ag+ adsorption by SPC was consistent with the pseudo-second-order kinetic model. The Langmuir isothermal model was used to well fit the Ag+ adsorption isotherms of SPC, and the maximum adsorption capacity of the optimized SPC-3 for Ag+ is up to 115 mg/g in 0.5 mol/L HNO3 solution. SPC-3 showed good selectivity toward Ag+ over diverse competing cations, which is mainly attributed to the strong bonding between Ag+ ions and the sulfur-containing functional groups on the surface of SPC-3 resulting in the formation of Ag2S nanoparticles. The adsorbed Ag could be recovered as an elemental form by a simple calcination. This study provides a new insight into the design of an environmentally friendly and efficient adsorbent for the selective recovery of silver from acidic aqueous media.

Copper-Based Electrocatalysts for Nitrate Reduction to Ammonia.

Ammonia (NH3) is a highly important industrial chemical used as fuel and fertilizer. The industrial synthesis of NH3 relies heavily on the Haber-Bosch route, which accounts for roughly 1.2% of global annual CO2 emissions. As an alternative route, the electrosynthesis of NH3 from nitrate anion (NO3-) reduction (NO3-RR) has drawn increasing attention, since NO3-RR from wastewater to produce NH3 can not only recycle waste into treasure but also alleviate the adverse effects of excessive NO3- contamination in the environment. This review presents contemporary views on the state of the art in electrocatalytic NO3- reduction over Cu-based nanostructured materials, discusses the merits of electrocatalytic performance, and summarizes current advances in the exploration of this technology using different strategies for nanostructured-material modification. The electrocatalytic mechanism of nitrate reduction is also reviewed here, especially with regard to copper-based catalysts.

Electrodeposition and characterization of Sn on Re filaments for laser resonance ionization mass spectrometry.

The isotopic analysis of Sn is crucial for geochemical research and surveillance of nuclear contamination. However, commonly used methods face the challenge of isobaric interference. Laser resonance ionization mass spectrometry (LRIMS) is a promising technology for effectively eliminating the isobaric interference effect as it combines the advantages of both resonance ionization and mass spectrometry technologies. In this study, an atomic source of 1 µg Sn was prepared by electrodeposition on a Re filament in a 1-5 × 0.7 mm spot for LRIMS measurement. The effects of voltage, duration, length of the active area, and Pb content on the deposition yield were studied, and the morphology, composition, and valence of the Sn deposits were examined. A maximum yield of over 90% in a 3 × 0.7 mm spot was achieved through the surface modification of Re filaments and optimisation of the electrodeposition parameters. As the Sn0 atomic state was predominant in the deposit, the average detection efficiency of the LRIMS device using the as-deposited Sn samples was approximately 3.63 × 10-4, which was almost an order of magnitude higher than that of the sample dropped with graphene oxide solution (4.39 × 10-5).

SIR: Self-supervised Image Rectification via Seeing the Same Scene from Multiple Different Lenses.

Deep learning has demonstrated its power in image rectification by leveraging the representation capacity of deep neural networks via supervised training based on a large-scale synthetic dataset. However, the model may overfit the synthetic images and generalize not well on real-world fisheye images due to the limited universality of a specific distortion model and the lack of explicitly modeling the distortion and rectification process. In this paper, we propose a novel self-supervised image rectification (SIR) method based on an important insight that the rectified results of distorted images of a same scene from different lenses should be the same. Specifically, we devise a new network architecture with a shared encoder and several prediction heads, each of which predicts the distortion parameter of a specific distortion model. We further leverage a differentiable warping module to generate the rectified images and re-distorted images from the distortion parameters and exploit the intra- and inter-model consistency between them during training, thereby leading to a self-supervised learning scheme without the need for ground-truth distortion parameters or normal images. Experiments on synthetic dataset and real-world fisheye images demonstrate that our method achieves comparable or even better performance than the supervised baseline method and representative state-of-the-art (SOTA) methods. The proposed self-supervised method also provides a possible way to improve the universality of distortion models while keeping their self-consistency. Code and datasets will be available at https://github.com/loong8888/SIR.

Half-life determination of 111Ag.

111Ag is a radionuclide that can be generated by neutron capture on 110Pd and whose decay properties and production feasibility make it a potential therapeutic agent against arthritis. Due to the discrepancies of recent published values of the half-life of 111Ag with previous published works which are not thoroughly documented for detailed experiment procedures and uncertainty budgets evaluation, an independent redetermination of the 111Ag half-life value is required. In this work, a solid 111Ag source was prepared and repeatedly measured in a high purity Germanium (HPGe) detector to determine its half-life. In total, more than fifty measurements were performed over a period of 26.3 days, corresponding to ∼3.5 half-lives of 111Ag. The experimental method and corresponding uncertainty budget are presented. The result of 7.419(15) days is consistent with the recently published value, 7.423(13) days, by Collins et al. and deviates by 0.418% from the currently recommended value 7.45(1) days. A new recommend half-life value of 7.437(7) days was determined utilizing all available experimental values by a power-moderated mean (PMM) method.

HyFormer: Hybrid Transformer and CNN for Pixel-Level Multispectral Image Land Cover Classification.

To effectively solve the problems that most convolutional neural networks cannot be applied to the pixelwise input in remote sensing (RS) classification and cannot adequately represent the spectral sequence information, we propose a new multispectral RS image classification framework called HyFormer based on Transformer. First, a network framework combining a fully connected layer (FC) and convolutional neural network (CNN) is designed, and the 1D pixelwise spectral sequences obtained from the fully connected layers are reshaped into a 3D spectral feature matrix for the input of CNN, which enhances the dimensionality of the features through FC as well as increasing the feature expressiveness, and can solve the problem that 2D CNN cannot achieve pixel-level classification. Secondly, the features of the three levels of CNN are extracted and combined with the linearly transformed spectral information to enhance the information expression capability, and also used as the input of the transformer encoder to improve the features of CNN using the powerful global modelling capability of the Transformer, and finally the skip connection of the adjacent encoders to enhance the fusion between different levels of information. The pixel classification results are obtained by MLP Head. In this paper, we mainly focus on the feature distribution in the eastern part of Changxing County and the central part of Nanxun District, Zhejiang Province, and conduct experiments based on Sentinel-2 multispectral RS images. The experimental results show that the overall accuracy of HyFormer for the study area classification in Changxing County is 95.37% and that of Transformer (ViT) is 94.15%. The experimental results show that the overall accuracy of HyFormer for the study area classification in Nanxun District is 95.4% and that of Transformer (ViT) is 94.69%, and the performance of HyFormer on the Sentinel-2 dataset is better than that of the Transformer.

Determination of the half-life of 161Tb.

161Tb has potential applications in targeted radionuclide therapy and nuclear forensic science. However, the half-lives of 161Tb in previous studies show a discrepancy. In this study, 161Tb samples were produced by irradiating 160Gd2O3 with thermal neutron flux. A series of procedures were applied to extract a pure 161Tb solution and three solid samples were prepared. The half-life of 161Tb has been measured with a high-purity germanium (HPGe) detector. The time-dependency of the 161Tb activity was followed by assessing the count rate of their characteristic gamma-ray emissions at 48.9 keV and 74.6 keV over a period of 33-43 days. The experiment and uncertainty budget are discussed in detail. Different uncertainty propagation equations were applied for random uncertainties, medium-frequency deviations and potential systematic errors. The result for the 161Tb half-life of 6.967 (11) d was determined by the weighted mean of half-lives from three samples, which confirms that the half-life is longer than the of the current evaluated half-life of 6.89 (2) d. From all available quoted experimental values, a recommended half-life of 6.934 (14) d was determined by the power-moderated method (PMM). Based on recent four published half-life values, a half-life of 161Tb of 6.9582 (33) d was determined by the PMM analysis.

Evaluation of Several Satellite-Based Soil Moisture Products in the Continental US.

Satellite-based soil moisture products are suitable for large-scale regional monitoring due to the accessibility. Five soil moisture products including SMAP, ESA CCI, and AMSR2 (ascending, descending, and average) were selected in the continental United States (US) from 2016 to 2021. To evaluate the performance of the products and assess their applicability, ISMN (International Soil Moisture Network) data were used as the in situ measurement. PBIAS (Percentage of BIAS), R (Pearson correlation coefficient), RMSE (Root Mean Square Error), ubRMSE (unbiased RMSE), MAE (Mean Absolute Error), and MBE (Mean Bias Error) were selected for evaluation. The performance of five products over six observation networks and various land cover types was compared, and the differences were analyzed at monthly, seasonal, and annual scales. The results show that SMAP had the smallest deviation with the ISMN data because PBIAS was around -0.13, and MBE was around -0.02 m3/m3. ESA CCI performed the best in almost all aspects; its R reached around 0.7, and RMSE was only around 0.07 m3/m3 at the three time scales. The performance of the AMSR2 products varied greatly across the time scales, and increasing errors and deviations showed from 2016 to 2020. The PBO_H2O and USCRN networks could reflect soil moisture characteristics in the continental US, while iRON performed poorly. The evaluation of the networks was closely related to spatial distributions. All products performed better over grasslands and shrublands with R, which was greater than 0.52, and ubRMSE was around 0.1 m3/m3, while products performed worse over forests, where PBIAS was less than -0.62, and RMSE was greater than 0.2 m3/m3, except for ESA CCI. From the boxplot, SMAP was close to the ISMN data with differences less than 0.004 m3/m3 between the median and lower quartiles.

Disposable multiplexed electrochemical sensors based on electro-triggered selective immobilization of probes for simultaneous detection of DNA and proteins.

Electrically addressable covalent immobilization of probes on a multiplexed electrode for the simultaneous detection of multiple targets within the same sample is often regarded as a difficult milestone to be achieved. Herein, we demonstrated a reagentless disposable multiplexed electrochemical DNA and aptamer-based sensing platform for the simultaneous determination of various targets. The electrochemically triggered "click" chemistry was developed, and three biomarkers, including p53, thrombin, and VEGF165 were used as model analytes. The proposed sensor consisted of three independent screen-printed carbon electrodes (SPCE), with an alkyne-azide cycloaddition reaction that was activated selectively by means of electrical triggering, so that different DNA probes can be modified on the desired electrode units in sequence. In terms of simultaneous detection, the sensor was able to quantify the DNA target of p53 with a detection limit of 0.35 nM, whereas the limits of detection for protein quantification of thrombin and VEGF165 were 0.22 nM and 0.014 nM, respectively. The proposed sensor not only showed encouraging reproducibility and stability, but also performed well even in 50% serum samples. Therefore, the work described here offers a general strategy for developing a multiplexed sensor with promising potential to achieve rapid, simple and cost-effective analysis of biological samples.

Co3O4@CdS Hollow Spheres Derived from ZIF-67 with a High Phenol and Dye Photodegradation Activity.

The Co3O4@CdS double-layered hollow spheres were first prepared by the template-removal method with the assistance of the ZIF-67 material; the structure has been proved by transmission electron microscopy (TEM). The Co3O4@CdS hollow spheres calcinated at 400 °C exhibited the highest photodegradation activity. Nearly 90% phenol was degraded after 2 h of visible-light irradiation. More than 80% rhodamine-B (RhB) was degraded within the first 30 min and nearly eliminated after 1 h of irradiation. The mechanism of the photodegradation reaction was investigated. Based on the analysis of electron spin resonance (ESR) spectra and radical trapping test, it was found that superoxide radicals are the major oxidative species for dye degradation and holes and hydroxyl radicals are the major oxidative species for phenol degradation. These results may be used in industrial wastewater treatment. The reaction obeys first-order reaction kinetics, and the rate constant of the Co3O4@CdS hollow sphere in dye degradation is 0.05 min-1 and that in phenol degradation is 0.02 min-1, which is three times higher than that of CdS nanoparticles. These results indicated the high oxidizing ability of the samples.

A facile solution-phase synthesis of cobalt phosphide nanorods/hollow nanoparticles.

A simple one-step solution-phase synthesis of cobalt phosphide nanorods (NRs) and hollow nanoparticles (NPs) has been reported in this paper. The phase and morphology evolutions of cobalt phosphide were researched by varying the reaction conditions. The detailed research confirms that oleylamine (OAm) in the reaction firstly reduces Co(acac)2 to the Co phase and the reaction between P atoms from TOP and Co atoms results in the Co2P phase. The as-synthesized NRs and NPs show superparamagnetic behavior at room temperature and ferromagnetic properties at 2 K. The current route provides a new and general chemical method for tunable preparation of cobalt phosphide nanostructures, which are important for further magnetic and catalytic studies.

Naked-eye quantitative aptamer-based assay on paper device.

This work initially describes the design of low-cost, naked-eye quantitative aptamer-based assays by using microfluidic paper-based analytical device (µPAD). Two new detection motifs are proposed for quantitative µPAD measurement without using external electronic readers, which depend on the length of colored region in a strip-like µPAD and the number of colorless detection microzones in a multi-zone µPAD. The length measuring method is based on selective color change of paper from colorless to blue-black via formation of iodine-starch complex. The counting method is conducted on the basis of oxidation-reduction reaction between hydrogen peroxide and potassium permanganate. Their utility is well demonstrated with sensitive, specific detection of adenosine as a model analyte with the naked eye in buffer samples and undiluted human serum. These equipment-free quantitative methods proposed thus hold great potential for the development of more aptamer-based assays that are simple, cost-efficient, portable, and user-friendly for various point-of-care applications particularly in resource-constrained environments.

Synthesis, resolution and biological evaluation of cyclopropyl analogs of abscisic acid.

cis-2,3-Cyclopropanated abscisic acid (cis-CpABA) has high photostability and good ABA-like activity. To further investigate its activity and action mechanism, 2S,3S-2,3-cyclopropanated ABA (3a) and 2R,3R-2,3-cyclopropanated ABA (3b) were synthesized. Bioassay showed that 3a displayed higher inhibitory activity in germination than that of 3b and ABA at the concentration of 3.0 µM, but 3a and 3b had much weaker inhibitory activity in inhibition seedling growth compared to ABA. The study of photostability revealed that 3a and 3b showed high stability under UV light exposure, which were 4 times and 3 times greater than (±)-ABA, respectively. Action mechanism study showed that 3a presented higher inhibition on phosphatase activity of HAB1 than 3b, although they all inferior to ABA. Molecular docking studies of 3a, 3b and ABA receptor PYL10 were agreement with the bioassay data and confirmed the importance of the configuration of the 2,3-cyclopropyl ABA analogs for their bioactivity in somewhat. This study provides a new approach for the design of ABA analogs, and the results validated structure-based design for this target class.

Timing readout in paper device for quantitative point-of-use hemin/G-quadruplex DNAzyme-based bioassays.

This work describes a quantitative point-of-use hemin/G-quadruplex DNAzyme-based assay that integrates a simple timing detection motif with low-cost, portable microfluidic paper-based analytical devices (µPADs). The timing readout is based on the selective DNAzyme-mediated wettability change of paper from hydrophilicity to hydrophobicity. Its utility is well demonstrated with sensitive, specific detection of K(+) ion as a model analyte in artificial samples as well as real human serum samples. This new method only requires a ubiquitous cheap timer (or a cell phone with a timing function) to provide quantitative results. It could offer new opportunities for the development of more peroxidase-mimicking DNAzyme-based bioassays that are simple, affordable, portable, and operable by minimally-trained users for broad point-of-use applications especially in resource-poor settings.