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Sinomenine (SIN) is commonly used as part of rheumatoid arthritis (RA) therapy in China, but there is still no published evidence of the efficacy of SIN monotherapy. This work investigates the efficacy and safety of SIN in treating RA patients and analyzes the correlation between ornithine level and the alleviation of disease activity in RA patients. In this 24 week, randomized, placebo-controlled, double-blind clinical trial, people with mild to moderate RA were randomly assigned (1:1:1, stratified by hospital) to receive SIN (120 mg, twice daily), methotrexate (MTX) (10 mg per week), or SIN + MTX therapy. The primary outcome was the proportion of patients who achieved a 50% improvement in the American College of Rheumatology (ACR) criteria at week 24 and who showed improvement according to the clinical disease activity index (CDAI). In this prospective subgroup analysis, we also assessed whether the 24 week alterations of disease activity in the treatment group were significantly correlated to the levels of blood ornithine. Of the 135 enrolled participants, 38, 39, and 36 patients were treated with SIN, MTX, and SIN + MTX, respectively. In the SIN-treated group, 52.63% of patients achieved ACR50 after 24 weeks of treatment, which was comparable to the results in the MTX-treated and SIN + MTX-treated groups. Hepatic and gastrointestinal disorders were the main adverse events; however, the ratio of patients suffering from hepatic disorder in the SIN group (1/38) was much lower than that in the MTX (10/39) and SIN + MTX (8/36) groups. A total of 221 serum samples were collected at the four follow-up time points in the three treatments, and the levels of ornithine, citrulline, and arginine were obtained through ultra-high performance liquid chromatography-quadrupole time-of-flight mass spectrometry (UHPLC-Q-TOF/MS). The serum ornithine level decreased after the 24 week treatment along with a decrease in disease activity, and may reflect therapeutic responses with a sensitivity value of 80%. In conclusion, SIN revealed a comparable efficacy to MTX for treating RA patients, but with fewer side effects. In addition, the serum ornithine level was found for the first time to have a close correlation with the alleviation of RA, which shows the value of this measure as an assessment indicator of drugs in treating RA.

Riboflavin (RF) is one of the necessary vitamins. If human body lacks RF, it will lead to inflammation and dysfunction of mouth, lips and skin. Thus sensitive and accurate determination of RF is necessary. Here, an electroactive covalent-organic framework nanobelt (COFTFPB-Thi) with thickness of 1.4 nm was prepared by amine-aldehyde condensation reaction between thionine and 1, 3, 5-tris (p-formylphenyl) benzene, which was then grown vertically on three-dimensional porous carbon derived from kenaf stem (3D-KSC) for double signal ratiometric electrochemical detection of RF. The resulted 3D-KSC/COFTFPB-Thi showed two reduction peaks at −0.08 V and −0.23 V, which came from the reduction of COFTFPB-Thi and the conjugated structure of COFTFPB-Thi, respectively. In the presence of RF, those RF molecules near the electrode surface were oxidized at 0.6 V. Then some oxidized RF (RFox) adsorbed on COFTFPB-Thi would oxidize COFTFPB-Thi into COFTFPB-Thi(ox) while other RFox adsorbed on 3D-KSC kept unchanged. When the potential was scanned from 0.6 V to −0.6 V, both COFTFPB-Thi(ox) and RFox adsorbed on 3D-KSC were reduced at −0.08 V and −0.45 V accordingly, while the reduction peak of −0.23 V of the conjugated structure of COFTFPB-Thi kept constant. When j-0.45/j-0.23 was used as the response signal, the detection limit was 44 nM and the linear range was 0.13 μM −0.23 mM. By using j-0.08/j-0.23 as the response signal, a detection limit of 90 nM and a linear range of 0.30 μM-0.23 mM (S/N = 3) were obtained. By using double signals, the measurement results can be corrected to make the results more accurate and reliable. The sensor also showed good selectivity, reproducibility and stability, which provided a good application prospects.

Developing a low-cost, highly active and durable catalyst for acidic oxygen reduction reaction (ORR) is of significant importance for proton-exchange electrolyte membrane fuel cell. In this work, we report an efficient catalyst based on Mn, Co and N co-doped carbon (MnCo–N–C) for acidic ORR. Electron microscopy and X-ray absorption spectroscopy indicate that atomic CoNx and MnNx sites are dispersed in the carbon matrices of MnCo–N–C. Raman spectroscopy verifies that the doping of Mn into carbon matrices can enable a higher graphitization degree, which can improve the corrosion resistance and catalytic durability of the MnCo–N–C catalyst towards ORR in challenging acidic media. As a result, the MnCo–N–C catalyst exhibits significantly improved ORR durability with a higher current retention of 81% after 50 h of test compared with that (52%) of the Co–N–C catalyst. Moreover, the half-wave potential of the MnCo–N–C catalyst increases by 100 mV compared with that of the Co–N–C catalyst.

Natural bio-enzyme catalysts usually exhibit unexpected performances for many significant reactions, which are worthy of reference. Here we report artificial metal-sulfur-carbon (M-S-C) mimic-enzyme catalysts based on bionic design. The catalysts combine metal centers and functional ligands, which realize the universal fabrication of phase and adjustable dimension. The synthesized catalysts inherit the highly active and selective feature of bio-enzyme catalysts. When directly used for carbon dioxide electroreduction reaction, the Sn-S-C catalyst exhibits high selectivity for formate (Faradaic efficiency >95%), as well as a continuous stability over 120 h at a high current density of 740 mA cm−2, greatly outperforming the reported catalysts for formate formation. The catalytic sites and pathways are probed with in-situ Fourier transform infrared (FTIR) spectra, in-situ Raman spectra and synchrotron-radiation X-ray photoelectron spectra. These results break the inherent conundrum which is impossible to simultaneously realize activity and durability under high selectivity. Our findings offer a versatile strategy to inherit from nature and integrate different components, thus designing efficient catalysts for various challenging reactions and energy conversions via a natural sustainable way.

Nitrate acts as a fundamental raw material in modern industrial and agricultural fields. Recently, photocatalytic nitrogen oxidation into nitrate has been expected to be an alternative method to replace the industrial nitrate synthesis process, which encounters many challenges, i.e., huge energy consumption and greenhouse gas emission. We synthesized Ce-doped W18O49 nanowires (Ce-W18O49) to realize photocatalytic nitrogen oxidation into nitrate under mild conditions. The defect state generated by coupling of Ce3+ introduction and surface plasma state acts as an "electron trap" to restrain photogenerated electrons, so as to facilitate the separation of photogenerated electron-hole pairs and prolong their lifetime. W18O49 doped with 5 mol % Ce exhibited the highest yield of nitrate (319.97 μg g-1 h-1) without any sacrificial agent, which is about 5 times higher than that of pristine W18O49. This work provides new insight into achieving high-efficiency photocatalytic nitrate evolution activity from direct N2 oxidation by controlling the energy band structure of photocatalysts.

To meet the current energy needs of society, the highly efficient and continuous production of clean energy is required. One of the key issues facing the green hydrogen evolution is the construction of efficient, low-cost electrocatalysts. Prussian blue (PB), Prussian blue analogs (PBAs), and their derivatives have tunable metal centers and have attracted significant interest as novel photo- and electrochemical catalysts. In this review, recent research progress into PB/PBA-based hollow structures, substrate-supported nanostructures, and their derivatives for green water splitting is discussed and summarized. First, several remarkable examples of nanostructured PB/PBAs supported on substrates (copper foil, carbon cloth, and nickel foam) and hollow structures (such as single-shelled hollow boxes, open hollow cages, and intricate hollow structures (multi–shell and yolk–shell)) are discussed in detail, including their synthesis and formation mechanisms. Subsequently, the applications of PB/PBA derivatives ((hydr)oxides, phosphides, chalcogenides, and carbides) for water splitting are discussed. Finally, the limitations in this research area and the most urgent challenges are summarized. We hope that this review will stimulate more researchers to develop technologies based on these intricate PB/PBA structures and their derivatives for highly efficient, green water splitting.

Light-induced heat is largely neglected in traditional photocatalytic systems, especially for the thermodynamically and kinetically challenging CO2 reduction to C2 fuels. Herein, we first design asymmetric Metal1-O-Metal2 triple-atom sites confined in phenakite to facilitate C-C coupling and employ photoinduced heat to increase molecular thermal vibration and accelerate CO2 reduction to C2 fuels. Using O-vacancy-rich Zn2GeO4 nanobelts as prototypes, quasi in situ Raman spectra disclose the Zn-O-Ge triatomic sites are likely the reactive sites. Density functional theory calculations reveal that the asymmetric Zn-O-Ge sites could promote C-C coupling through inducing distinct charge distributions of neighboring C1 intermediates, whereas the created O vacancies could lower the energy barrier of the rate-determining hydrogenation step from 1.46 to 0.67 eV. Catalytic performances under different testing conditions demonstrate that light initiates the CO2 reduction reaction. In situ Fourier-transform infrared spectra and D2O kinetic isotopic effect experiments disclose that light-induced heat kinetically triggers C-C coupling and accelerates OCCO* hydrogenation via providing abundant hydrogen species. Consequently, in a simulated air atmosphere under 0.1 W/cm2 illumination at 348 K, the O-vacancy-rich Zn2GeO4 nanobelts demonstrate an acetate output of 12.7 μmol g-1 h-1, a high acetate selectivity of 66.9%, a considerable CO2-to-CH3COOH conversion ratio of 29.95%, and a stability of up to 220 h.

Layered materials have attracted tremendous interest for accessing two-dimensional structures. Materials such as graphite or transition metal dichalcogenides, in which the layers are held together by van der Waals interactions, can be exfoliated through a variety of processes in a manner that retains the structure and composition of the monolayers, but this has proven difficult for solids with stronger interlayer interactions. Here, we demonstrate the exfoliation of AgCrS2, a member of the AMX2 family (where A is a monovalent metal, M is a trivalent metal and X is a chalcogen), through intercalation with tetraalkylammonium cations, chosen for their suitable redox potential. The as-exfoliated nanosheets consist of Ag layers sandwiched between two CrS2 layers, similar to their structure in the bulk. They show superionic behaviour at room temperature, with an ionic conductivity of 33.2 mS cm−1 at 298 K that originates from Ag+ ions rapidly hopping between neighbouring tetrahedral interstices; in the bulk, this behaviour is only observed above 673 K. Layered materials held together by weak interactions can be exfoliated into monolayers that retain the structure and composition of their bulk counterpart, but this has remained challenging to achieve for non-van der Waals materials. Now, AgCrS2 has been exfoliated into such [CrS2]Ag[CrS2] nanosheets through intercalation with tetraalkylammonium cations chosen for their suitable redox potential. The nanosheets show superionic behaviour at room temperature.

Extracting photogenerated species from bulk to surface is an essential process for gaining efficient semiconductor-based photocatalysis. However, compared with charged photogenerated carriers, neutral exciton exhibits negligible response to electric field. Accordingly, traditional strategies involving band-alignment construction for boosting directional transfer of charge carriers are impracticable for extracting bulk excitons. To this issue, we here propose that the extraction of bulk exciton could be effectively implemented by surface modification. By taking confined layered bismuth oxycarbonate (Bi2O2CO3) as an example, we highlight that the incorporation of iodine atoms on the surface could modify the micro-region electronic structure and hence lead to reduced energy of surface excitonic states. Benefiting from the energy gradient between bulk and surface excitonic states, iodine-modified Bi2O2CO3 possesses high-efficiency bulk exciton extraction, and hence exhibits promoted performance in triggering 1O2-mediated selective oxidation reaction. This work presents the positive role of surface modification in regulating excitonic processes of semiconductor-based photocatalysts.

Self-organized and vertically oriented TiO2 nanotubes (TNTs) were synthesized via anodization of Ti sheet in a glycerol-based used electrolyte. Graphite (Gt) is doped in TNTs by physical vapor deposition (PVD) under Ar-atmosphere at 700 °C using polyvinyl alcohol (PVA) as a precursor. The samples were characterized using FESEM, HRTEM, XRD, Raman, XPS, and UV–vis diffuse reflectance spectroscopy. HRTEM, XRD, and Raman analysis confirm the suppression of phase transformation from anatase to rutile due to Gt doping. The UV–vis absorption properties and photocatalytic activity of the pristine and Gt-doped TNTs have been investigated. The bandgap absorption edge of Gt-doped TNTs shifts towards a higher wavelength (~ 550 nm) compared to the pristine TNTs (~ 390 nm). Moreover, the Gt-doped TNTs show strong absorption in the visible region. This makes it a good candidate for energy-storing applications. It has been found that Gt-doped TNTs display two-fold enhanced photocatalytic activity for methyl orange (MO) degradation compared to pristine. The enhanced photo-degradation of Gt-doped TNTs is ascribed to the higher absorptivity, better crystallinity, and lower bandgap of TNTs due to Gt doping. The enhanced photo-degradation ability of Gt-doped TNTs can be used to clean industrial wastewater.

Spintronics is a promising alternative to the conventional silicon transistor-based electronics that are gradually approaching their physical limitations. Ultrathin two-dimensional van der Waals (vdW) materials (2D materials) with controllable spin degrees of freedom are recognized as extremely promising spintronic materials in architectures for the post-Moore era. In this Perspective, we review recent progress on spin-dependent transport behaviors (SDTBs) confined at the 2D scale, which are the mainstream paradigms for spintronic devices. We first present the mechanism and the key factors of SDTBs in 2D nonmagnetic materials-based hybrid devices. Then, some chemical modulation strategies for inducing short-range magnetic order and magneto-electric performance into 2D nonmagnetic materials are discussed. Furthermore, we concentrate on introducing intriguing SDTBs in 2D long-range ferromagnetic materials-based vdW devices. Finally, we highlight the current challenges in the study of spin-dependent transport of 2D modified materials and 2D material-based spintronic devices, in the hope of accelerating their applications.

Electrochemical water splitting for hydrogen generation is a promising pathway for renewable energy conversion and storage. One of the most important issues for efficient water splitting is to develop cost-effective and highly efficient electrocatalysts to drive sluggish oxygen-evolution reaction (OER) at the anode side. Notably, structural transformation such as surface oxidation of metals or metal nonoxide compounds and surface amorphization of some metal oxides during OER have attracted growing attention in recent years. The investigation of structural transformation in OER will contribute to the in-depth understanding of accurate catalytic mechanisms and will finally benefit the rational design of catalytic materials with high activity. In this Review, we provide an overview of heterogeneous materials with obvious structural transformation during OER electrocatalysis. To gain insight into the essence of structural transformation, we summarize the driving forces and critical factors that affect the transformation process. In addition, advanced techniques that are used to probe chemical states and atomic structures of transformed surfaces are also introduced. We then discuss the structure of active species and the relationship between catalytic performance and structural properties of transformed materials. Finally, the challenges and prospects of heterogeneous OER electrocatalysis are presented.

The major obstacle for selective CO2 photoreduction to C2 hydrocarbons lies in the difficulty of C-C coupling, which is usually restrained by the repulsive dipole-dipole interaction between adjacent carbonaceous intermediates. Herein, we first construct semiconducting atomic layers featuring abundant Metaln+-Metalδ+ pair sites (0 < δ < n), aiming to tailor asymmetric charge distribution on the carbonaceous intermediates and hence trigger their C-C coupling for selectively yielding C2 hydrocarbons. As an example, we first fabricate Co-doped NiS2 atomic layers possessing abundant Ni2+-Niδ+ (0 < δ < 2) pairs, where Co doping strategy can ensure higher amount of Ni2+-Niδ+ pair sites. In-situ Fourier-transform infrared spectroscopy, quasi in-situ Raman spectroscopy and density-functional-theory calculations disclose the Ni2+-Niδ+ pair sites endow the adjacent CO intermediates with distinct charge densities, thus decreasing their dipole-dipole repulsion and hence lowering the rate-limiting C-C coupling reaction barrier. As a result, in simulated flue gas (10% CO2 balance 90% N2), the ethylene selectivity for Co-doped NiS2 atomic layers reaches up to 74.3% with an activity of 70 µg·g−1·h−1, outperforming previously reported photocatalysts under similar operating conditions.

Physical separation of C2H2 from CO2 on metal-organic frameworks (MOFs) has received substantial research interest due to the advantages of simplicity, security, and energy efficiency. However, that C2H2 and CO2 exhibit very close physical properties makes their separation exceptionally challenging. Previous work appeared to mostly focused on introducing open metal sites that aims to enhance the C2H2 affinity at desired sites, whereas the reticular manipulation of organic components has rarely been investigated. In this work, by reticulating preselected amino and hydroxy functionalities into isostructural ultramicroporous chiral MOFs-Ni2(l-asp)2(bpy) (MOF-NH2) and Ni2(l-mal)2(bpy) (MOF-OH)-we targeted efficient C2H2 uptake and C2H2/CO2 separation, which outperforms most benchmark materials. Explicitly, MOF-OH adsorbs substantial amount of C2H2 with record storage density of 0.81 g mL-1 at ambient conditions, which even exceeds the solid density of C2H2 at 189 K. In addition, MOF-OH gave IAST selectivity of 25 toward equimolar mixture of C2H2/CO2, which is nearly twice higher than that of MOF-NH2. Notably, the adsorption enthalpies for C2H2 at zero converge in both MOFs are remarkably low (17.5 kJ mol-1 for MOF-OH and 16.7 kJ mol-1 for MOF-NH2), which to our knowledge are the lowest among efficient rigid C2H2 sorbents. The efficiencies of both MOFs for the separation of C2H2/CO2 are validated by multicycle breakthrough experiments. DFT calculations provide molecular-level insight over the adsorption/separation mechanism. Moreover, MOF-OH can survive in boiling water for at least 1 week and can be easily scaled up to kilograms eco-friendly and economically, which is very crucial for potential industrial implementation.

The development of advanced electrocatalysts for electro-oxidation reactions has attracted much attention because of the critical role of such electrocatalysts in improving the overall efficiency of coupled hydrogen production. We have developed an efficient lanthanum-doped α-Ni(OH)2 bifunctional catalyst with a 1D-2D-3D hierarchical nanostructure. It shows superior activity and stability in the anodic oxygen evolution reaction (OER) and urea oxidation reaction (UOR). Enrichment of the edge sites and conducting La doping in α-Ni(OH)2 phase enable formation and stabilization of abundant local Ni3+ ions. This guarantees ultralow onset potentials in electro-oxidation reactions. The 1D-2D-3D hierarchical nanostructure significantly boosts the in situ generation of high-valence active species, which results in efficient and stable OER and UOR performances, and the synergistic merit of doping-induced facile reaction kinetics. Because of the structural benefits of a large surface area, charge-transfer promotion, good structural stability, and bifunctionality, a 1% La-doped α-Ni(OH)2 hierarchical nanostructure gives superior OER and UOR performances with low overpotentials, large catalytic current densities, and excellent operational stability. It is therefore a promising catalyst for use in simultaneous alkaline wastewater treatment and hydrogen production.

Chemical investigation on the cultures of the fungus Marasmius berteroi, resulted in the isolation of 10 compounds including 2 new ones named (S)-3,7-dihydroxy-1-indanone (1) and (S)-3-hydroxy-4-methoxy-3-methyl isobenzofuran-1(3H)-one (2). Their structures were determined based on NMR, HRESIMS and ECD spectra analysis. Compounds 5-6, 10 revealed moderate inhibitory activity against the nematode Panagrellus redivivus with mortality ratio of 95 %, 85 %, and 75 % at 2.5 mg/mL, respectively.

CircRNAs have emerged as potential therapeutic targets for diseases such as gastric cancer (GC). We identified highly dysregulated circRNAs in GC tissue and further explored their potential mechanisms in the progression of GC. Hsa_circ_0091994 (cicrRNA_105040) was identified as a highly upregulated circRNA in GC tissues, whose host gene is negatively associated with the overall survival of patients. Using cell counting kit-8 and Annexin V assays, we observed that hsa_circ_0091994 knockdown inhibited the viability of AGS and HGC-27 cells by inducing apoptosis. Scratch wound healing assays showed that hsa_circ_0091994 knockdown also inhibited GC cell healing. Bioinformatics analysis and a luciferase assays revealed that hsa_circ_0091994 knockdown inhibits GC progression by suppressing miR-324-5p and HMGA1 expression. The antitumor effect of hsa_circ_0091994 knockdown was confirmed in vivo using a mouse xenograft model. Hsa_circ_0091994 knockdown inhibited the progression of GC by inhibiting the miR-324-5p/HMGA1 axis.

Cobalt-based oxides and hydroxides have always been one of the optimal catalysts for Oxygen Evolution Reaction (OER) in alkaline environment in recent years. However, it remains a challenge for simple cobalt oxides such as CoO, Co3O4 and CoOOH to provide high catalytic activity both with ideal conductivity and stability. Herein, we prepared a new type of sulfur-incorporated cobalt oxide nanocages as high efficiency OER catalyst using Co-MOF as precursor. With the help of sodium sulfide, one step water-warm immersion-alcohol refluxing method can achieve the cavitation of precursors and uniform incorporation of sulfur atoms meanwhile. The hollow cubic structure constructed by fluffy nanosheets is beneficial to the exposure of active sites, the regulation of electronic structure and improve the electron transfer speed. After electrochemical testing, the prepared CoS@CoO showed outstanding OER activity compared with other cobalt-based catalysts. More importantly, this material has also withstood the electrochemical test of long range due to the stable structural foundation provided by Co-MOF. This work comes up with a new idea for OER activity promotion of hollow doped cobalt-based catalysts through morphology control and electronic structure optimization.

Litter-leached dissolved organic carbon (DOC) plays an essential role in regulating biogeochemical cycles in forests. However, it is unclear how tree litter-leached DOC amounts and biodegradation vary with mycorrhizal types and leaf habits. We collected leaf litter from 14 common tree species belonging to different mycorrhizal types (arbuscular mycorrhizal, AM; and ectomycorrhizal, ECM) and leaf habits (deciduous broadleaf, evergreen broadleaf, and evergreen coniferous) in subtropical forests of southern China. We used a soaking experiment to determine litter-leached DOC, dissolved total nitrogen (DTN), and dissolved total phosphorus (DTP) amounts, and DOC aromaticity and molecular weight, and then assessed leaf litter-leached DOC biodegradation using a 42-day incubation experiment. AM broadleaf tree litter produced greater amounts of DOC with lower aromatic content and molecular weight than ECM broadleaf tree litter. In contrast, AM evergreen coniferous litter leached lower amounts of DOC with greater aromaticity than ECM evergreen coniferous litter. In the litter leachates, AM broadleaf trees often had higher DOC:DTN ratio than ECM broadleaf trees, while AM evergreen coniferous species had a lower DOC:DTP ratio than ECM evergreen coniferous species. For both deciduous and evergreen broadleaf trees, AM species had greater DOC biodegradation than ECM species due to the lower aromatic content and molecular weight. However, litter-leached DOC biodegradation did not differ between AM and ECM evergreen coniferous trees. Tree mycorrhizal associations can indicate the interspecific variations of litter-leached DOC amounts and biodegradation, but such tree mycorrhizal effect is highly dependent on leaf habit in subtropical forests.

A novel pretreatment method was used to ameliorate the treatment effect of iodine contained radioactive waste. The pretreatment sample (15 w%) held the highest amorphous index (0.50) at 600 °C, and iodine element was in a state of uniform distribution. The density of the sample could increase to 2.95 gcm3 by using the novel method, which was higher than other similar studies. The leaching result of iodine was as low as 1.53 × 106 gm2d1 after 7 days treatment, which indicated that the solidified body has good stability in a long run.

A new alkaloid named methyl 2-(3,4-dihydro-2H-pyrrol-5-yl)acetate (1), together with 24 known compounds, was isolated from the acetone extract of the fruiting bodies of Ramaria stricta. Their structures were elucidated on HR-ESI-MS and extensive 1D and 2D NMR spectroscopy. The nematocidal assay showed that three compounds, benzoic acid, 3-hydroxy-2-methylbenzaldehyde, and 4-(hydroxy)benzylbenzoic acid, exhibited a certain activity against Panagrellus redivivus.

Here we report a simple all-nucleic-acid enzyme-free catalyzed hairpin assembly assisted amplification strategy with quantum dots (QDs) as the nanoscale signal reporter for homogeneous visual and fluorescent detection of A549 lung cancer cells from clinical blood samples. This work was based on the phenomenon that CdTe QDs can selectively recognize Agsup+/supand C-Agsup+/sup-C and by using mucin 1 as the circulating tumor cells (CTCs) marker and aptamer as the recognition probe. Under optimized conditions, the limits of detections as low as 0.15 fg/mL of mucin 1 and 3 cells/mL of A549 cells were achieved with fluorescence signals. A 1 fg/mL concentration of mucin 1 and 100 cells/mL of A549 can be distinguished by the naked eye. This method was used to quantitatively analyze CTCs in 51 clinical whole blood samples of patients with lung cancer. The levels of CTCs detected in clinical samples by this method were consistent with those obtained using the folate receptor-polymerase chain reaction clinical test kit and correlated with radiologic and pathological findings.

To long-term immobilization of secondary iodine-waste, iodine loaded silver-coated silica-gel (AgIs), glass-powder was used to directly solidify AgIs at low temperature. B2O3-Bi2O3-ZnO-SiO2 was used as raw materials to manufacture the glass-matrix under different temperature. The samples with the richest glass phase were obtained at 1000 °C, and were used to solidify AgIs with different content of I−. The sample with 30 wt% I− possessed the highest amorphous index (0.62) at 600 °C. Element I was uniformly distributed, and the density reached to 3.06 g/cm3. This work highlights a simple way to solidify secondary iodine-waste at low temperature.

Myzus persicae is one of the most important economic pests of cultivated crops. In the present study, we used an integrated approach involving high-performance liquid chromatography fractionation, affinity enrichment, and mass spectrometry-based proteomics to carry out a comprehensive proteomic analysis of lysine crotonylation in M. persicae. Altogether, 7530 lysine crotonylation sites were identified in 2452 protein groups. Intensive bioinformatic analyses were then carried out to annotate those lysine crotonylated targets identified in terms of Gene Ontology annotation, domain annotation, subcellular localization, Kyoto Encyclopedia of Genes and Genomes pathway annotation, functional cluster analysis, etc. Analysis results showed that lysine-crotonylated proteins were involved in many biological processes, such as the amino acid metabolism, aminoacyl-tRNA biosynthesis, spliceosomes, ribosomes, and so forth. Notably, the interaction network showed that there were 199 crotonylated proteins involved in the amino acid metabolism and numerous crotonylation targets associated with fatty acid biosynthesis and degradation. The results provide a system-wide view of the entire M. persicae crotonylome and a rich data set for functional analysis of crotonylated proteins in this economically important pest, which marks an important beginning for the further research.

Rationally designing high-activity catalyst for oxygen evolution reaction (OER) is of primary importance due to its sluggish kinetic process in water splitting. Herein, we report a metallic (V) and nonmetallic (F) double doping in Co3O4 with nanoneedles structure, which is synthesized through facile oil bath and annealing. Electrochemical measurements show that the Co3O4 dopped with fluorine and vanadium (F0.2-V-Co3O4-350) only needs a low overpotential of 320 mV to afford a current density of 10 mA cm−2, which is superior to commercial RuO2. The excellent electrocatalytic performance can be attributed to double doping of vanadium and fluorine which have strong electron absorption effect to optimize the density of electrons in Co3O4. Besides, nanoneedles structure can enlarge exposure of active sites. And its great durability is evaluated through 2000 cycles CV test. Furthermore, the optimal ratio of fluorine to vanadium and different annealing temperatures of the target catalyst are explored reasonably.

The renewable-electricity-powered CO2 electroreduction reaction provides a promising means to store intermittent renewable energy in the form of valuable chemicals and dispatchable fuels. Renewable methane produced using CO2 electroreduction attracts interest due to the established global distribution network; however, present-day efficiencies and activities remain below those required for practical application. Here we exploit the fact that the suppression of *CO dimerization and hydrogen evolution promotes methane selectivity: we reason that the introduction of Au in Cu favors *CO protonation vs. C−C coupling under low *CO coverage and weakens the *H adsorption energy of the surface, leading to a reduction in hydrogen evolution. We construct experimentally a suite of Au-Cu catalysts and control *CO availability by regulating CO2 concentration and reaction rate. This strategy leads to a 1.6× improvement in the methane:H2 selectivity ratio compared to the best prior reports operating above 100 mA cm−2. We as a result achieve a CO2-to-methane Faradaic efficiency (FE) of (56 ± 2)% at a production rate of (112 ± 4) mA cm−2., The electroreduction of CO2 offers a promising approach to produce carbon-neutral methane using renewable electricity. This study shows that the introduction of Au in Cu enables selective methane production from CO2 by regulating *CO availability.

Understanding the detailed process of spontaneous formation of intrinsic defects and their ability to tune the electronic structures in functional materials has become a key prerequisite for their technological applications. Here, by using in situ scanning tunneling microscopy, we report the observation of one-dimensional Frenkel chain defects on the cleaved CsBi4Te6 surface due to the migration of Te atoms for the first time. Further scanning tunneling spectroscopy measurements clearly revealed a self-electron doping effect of the Frenkel chain defects, which could directly affect their thermoelectric and superconducting properties. The unique one-dimensional Frenkel tellurium atomic chain defect and its doping effect on the electronic structure observed here not only shed light on tuning the electric properties of a series of tellurides but also possess profound implications for enriching the microscopic details of defect chemistry and materials science.

Herein, we first design a fast low-pressure ultraviolet light irradiation strategy for easily regenerating the nearly equivalent surface vacancies. Taking the defective Bi2 O2 CO3 nanosheets as an example, nearly equal amount of oxygen vacancies can be regenerated under UV light irradiation. Synchrotron-radiation quasi in situ X-ray photoelectron spectra disclose the Bi sites in the O-defective Bi2 O2 CO3 nanosheets can act as the highly active sites, which not only help to activate CO2 molecules, but also contribute to stabilizing the rate-limiting COOH* intermediate. Also, in situ Fourier transform infrared spectroscopy and in situ mass spectrometry unravel the UV light irradiation contributes to accelerating CO desorption process. As a result, the O-defective Bi2 O2 CO3 nanosheets achieve a stability up to 2640 h over 110 cycling tests and a high evolution rate of 275 μmol g-1 h-1 for visible-light-driven CO2 reduction to CO.

Caveolin-1 (Cav-1) is a constitutive structural protein of caveolae in the plasma membrane. It plays an important role in maintaining blood brain barrier (BBB) integrity. In this study, we identified that miR-103-3p, a hypoxia-responsive miRNA, could interact with Cav-1. In endothelial cells, miR-103-3p mimic diminished the expression of Cav-1 and tight junction proteins, which were rescued by the inhibition of miR-103-3p. We found a substantial increase of miR-103-3p and decease of Cav-1 in the rat subarachnoid hemorrhage (SAH) model. Pre-SAH intracerebroventricularly injection of miR-103-3p antagomir relieved Cav-1 loss, sequentially reduced BBB permeability and improved neurological function. Finally, we demonstrated that the salutary effects of miR-103-3p antagomir were abolished in Cav-1 knock-out mice, suggesting that Cav-1 was required for the miR-103-3p inhibition-induced neurovascular protection. Taken together, our findings suggest that the inhibition of miR-103-3p could exert neuroprotective effects through preservation of Cav-1 and BBB integrity, making miR-103-3p a novel therapeutic target for SAH.

Four carbonyl hydrido RuII complexes with different functionalized α,α'-diimine ligands have been synthesized and well characterized by IR, UV/vis, CV, ESI/MS, and 1H NMR spectra. One of the complexes was also characterized by X-ray crystallography. The luminescence of these complexes has been investigated at room temperature in CH2Cl2 solution and low temperature glassy media at 77 K. The emissions are originated from either ligand-centered π–π* transitions or metal center to ligand charge transfer (MLCT), which are highly dependent on the properties of the α-diimine ligands.

An accurate control-oriented electrothermal model is of great importance for onboard temperature monitoring and efficient performance management of lithium (Li)-ion batteries in automobile applications. This article presents a control-oriented electrothermal model for pouch-type electric vehicle batteries. This model uses the Chebyshev–Galerkin (CG) approximation method and captures the heat generation of positive and negative tabs, the heat flow between the tabs and the body, and the uneven heat generation inside the battery. This model consists of two lumped-mass submodels for positive and negative tabs and a 2-D CG submodel for the main battery body. The heat generation in the 2-D CG model is strongly dependent on the electrical parameters that are conversely functions of battery temperature. The lumped-mass models are decoupled from the 2-D CG model and parameterized separately by the particle swarm optimization algorithm and validated against the temperature measurements (covering three test scenarios) of a 20-Ah pouch-type Li-ion iron phosphate battery. The results demonstrate that the coupled model accurately predicts the temperatures of the tabs and the temperature distribution inside the battery. Besides, the computational complexity of the coupled model is also evaluated, and the result shows that the model has great potential for real-time temperature monitoring and efficient thermal management.

Direct CH4 photoconversion into liquid oxygenates under mild conditions still represents a huge challenge. Herein, two-dimensional oxide semiconductors are designed to generate abundant active O- species for activating C-H bond of methane. Taking the synthetic ZnO nanosheets as an example, in situ electron paramagnetic resonance spectra verified their lattice oxygen atoms could capture photoexcited holes and generate active O- species, which could efficiently abstract H from CH4 to generate ·CH3 radicals. Gibbs free energy calculations and in situ Fourier-transform infrared spectroscopy corroborated the rate-limiting step was the first C-H bond activation process, whereas the exoergic oxidation of *CHO to HCOOH was easier than the endoergic overoxidation to CO, accounting for the selective production of liquid oxygenates. As a result, the formation rate of liquid oxygenates over ZnO nanosheets reached 2.21 mmol g-1 h-1 with a selectivity of 90.7% at atmospheric pressure and approximately 50 °C, outperforming previously reported photocatalysts under similar conditions.

The demand for DC gas-insulated switchgear/gas-insulated transmission line (GIS/GIL) becomes more and more urgent in recent years owing to the rapid development of high voltage direct current (HVDC) transmission systems. Insulators in DC GIS/GIL could easily accumulate a large number of charges on its surface during long-term operation, which might lead to overstressing of polymeric insulation or surface flashover. Therefore, it is of great significance to propose an effective method for dissipating extra surface charges. However, achieving charge dissipation without opening the tank is still a great challenge to SF 6 -insulated equipment for a long time. In this paper, a novel method, which is named X-ray based non-contact charge dissipation method (XNCDM) for insulators in SF 6 -insulated equipment, is proposed. The effects of X-ray irradiation on the charges dissipation and the influences of irradiation dose were experimentally investigated in SF 6 . The mechanisms underlying are discussed in detail. Results show that surface charges on the insulator can be almost completely dissipated after short-time X-ray irradiation with enough dose, owing to the significant enhancement of electric conduction along the insulator surface and charge neutralization by gas ions near the gas-solid interface. This paper provides a novel technique for realizing rapid surface charge dissipation on the insulator, which is of great significance for a variety of engineering applications of DC GIS/GIL.