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Sustainable metal-air batteries demand high-efficiency, environmentally-friendly, and non-precious metal-based electrocatalysts with bifunctionality for both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). In this research, novel functional carbon nanotubes with multi-active sites including well-dispersed single-atom iron throughout the walls and encapsulated ultrafine iron nanoparticles were synthesized as an electrocatalyst (FeNP@Fe-N-C) through one-step pyrolysis of metal-organic frameworks. High-resolution synchrotron powder X-ray diffraction and X-ray absorption spectroscopy were applied to characterize the unique structure of the electrocatalyst. In comparison to the commercial Pt/C and RuO2 electrodes, the newly prepared FeNP@Fe-N-C presented a superb bifunctional performance with its narrow potential difference (Egap) of 0.73 V, which is ascribed to the metallic Fe nanoparticles that boosts the adsorption and activation of oxygen on the active sites with an enhanced O2 adsorption capacity of 7.88 cm3 g−1 and synergistically functionalizes the iron atoms dispersed on the nanotubes. A rechargeable zinc-air battery based on FeNP@Fe-N-C exhibited a superior open-circuit voltage (1.45 V), power density (106.5 mW cm−2), and stable cycling performance. The green technique developed in this work for the fabrication of functional nanotubes raises the prospect of making more efficient electrocatalysts for sustainable energy cells.

Based on the structural modification of regorafenib, 28 pyrazinyl–aryl urea derivatives were synthesized and their in vitro antiproliferative activities were evaluated. Six compounds (5-16, 5-17, 5-18, 5-19, 5-22, and 5-23) exhibited favorable inhibitory activity against the human bladder cancer T24 cell line, and 5-23 demonstrated the strongest inhibitory activity (IC(50) = 4.58 ± 0.24 μM) with high selectivity. Compound 5-23 induced apoptosis in the low concentration range (≤7.5 μM) combined with shorter incubation time (≤10 h) via the activation of caspases, while high concentrations and prolonged incubation times led to necroptotic cell death by activating the RIPK1/RIPK3/MLKL signaling pathway. Induced apoptosis and necroptosis were closely associated with intracellular reactive oxygen species generation and decreased mitochondrial membrane potential. Compared with regorafenib, 5-23 displayed improved pharmacokinetic profiles in an in vivo rat model. Molecular docking and structure–activity relationship analyses were in agreement with the biological data. Compound 5-23 may be a potent anti-bladder cancer agent and this small molecule can be considered as a promising structure for further optimization.

Flaxseed has displayed the potential beneficial as functional foods. However, most studies focused on effects of flaxseed extracts or ingredients in flaxseed. Besides, few studies showed that flaxseed extracts contributed to anti-type 1 diabetes (T1D), yet the underlying mechanism is still unknown. In the present study, 16.7% of milled flaxseed (MF)-added diet was given to diabetic mice induced by streptozocin for 6 weeks. The results showed that MF feeding 1) slightly decreased blood glucose levels and improved the ability of glucose tolerance by oral glucose tolerance test, 2) decreased liver tumor necrosis factor-α levels and increased liver glycogen levels with significance via down-regulating TLR4/NF-κB pathways, 3) and significantly altered some beneficial bacteria in gut microbiota. In conclusion, the present study showed that milled flaxseed showed the potential on anti-T1D through anti-inflammation via TLR4/NF-κB and altering the gut microbiota in STZ-induced diabetic mice.

Developing electrocatalysts with excellent catalytic performance and superior durability for hydrogen evolution reaction (HER) remains a challenge. Herein, metal-nitrogen sites (M–Nx, M = Ni and Cu) are successfully implanted into zeolitic imidazolate zinc framework (ZIF-8)-derived nitrogen-doped porous carbon (ZIF/NC) to prepare Ni-ZIF/NC and Cu-ZIF/NC electrocatalysts for the HER. These M–Nx active sites significantly enhanced the electrocatalytic activities of Ni-ZIF/NC and Cu-ZIF/NC. Metal Ni acted as a catalyst for catalysis of Ni-ZIF/NC to form carbon nanotubes-like structures, which provided convenient ion transmission pathways. Owing to its special morphology and an increased number of defects, Ni-ZIF/NC displayed superior electrocatalytic activity in the HER compared to those of Cu-ZIF/NC and ZIF/NC. In an alkaline environment, Ni-ZIF/NC exhibited an overpotential at the current density of 10 mA cm−2 (η10) of 163.0 mV and Tafel slope of 85.0 mV dec−1, demonstrating an electrocatalytic property equivalent to that of Pt/C. In an acidic environment, Ni-ZIF/NC yielded a η10 of 177.4 mV and Tafel slope of 83.9 mV dec−1, which were comparable to those of 20 wt.% Pt/C. Moreover, Ni-ZIF/NC and Cu-ZIF/NC also exhibited superior stabilities in alkaline environments. This work offers a valuable strategy for controlling the morphology and implanting M–Nx active sites into carbon for designing novel catalysts for use in alternative new energy applications.

In this project, firstly, polyaniline-based polyester–cotton fabric was prepared by in situ polymerization using polyester–cotton fabric as the base fabric, aniline as the monomer, ammonium persulfate as the oxidizer, and camphor sulfonic acid as the dopant. Secondly, cobalt ferrite/carbon fiber powder-coated polyaniline-based polyester–cotton fabric was prepared by the textile coating process using polyaniline-based polyester–cotton fabric as the base fabric, PU2540-type polyurethane as the adhesive, and cobalt ferrite and carbon fiber powder as functional particles. Finally, the effect of the cobalt ferrite and carbon fiber powder doping ratio on the shielding effectiveness, reflection loss, dielectric constant real part, imaginary part, and loss angle tangent of cobalt ferrite/carbon fiber powder-coated polyaniline-based polyester–cotton fabric was studied by using the controlled variable method with emphasis on the cobalt ferrite/carbon fiber powder doping ratio. The results show that in the frequency range of 0.01–3.0 GHz, when the doping ratio of cobalt ferrite to carbon fiber powder is 0:3, the reflection loss of cobalt ferrite/carbon fiber powder-coated polyaniline-based polyester–cotton fabric reaches the minimum value at 1.49 GHz, the minimum reflection loss is –21.4 dB, and the effective absorption band is 1.25–1.94 GHz. In the test band, the shielding efficiency, reflection loss, the real part and imaginary part of the dielectric constant, and the loss angle tangent of the carbon fiber powder-coated polyaniline-based polyester–cotton fabric are larger than those of cobalt ferrite-coated polyaniline-based polyester–cotton fabric. The smaller the doping ratio of cobalt ferrite to carbon fiber powder, the larger value of the shielding efficiency, reflection loss, the real part and imaginary part of the dielectric constant, and loss angle tangent of the cobalt ferrite/carbon fiber powder-coated polyaniline-based polyester–cotton fabric.

Irritable bowel syndrome (IBS) is one of the functional gastrointestinal disorders characterized by chronic and/or recurrent symptoms of abdominal pain and irregular defecation. Changed gut microbiota has been proposed to mediate IBS; however, contradictory results exist, and IBS-specific microbiota, metabolites, and their interactions remain poorly understood. To address this issue, we performed metabolomic and metagenomic profiling of stool and serum samples based on discovery (n = 330) and validation (n = 101) cohorts. Fecal metagenomic data showed moderate dysbiosis compared with other diseases, in contrast, serum metabolites showed significant differences with greater power to distinguish IBS patients from healthy controls. Specifically, 726 differentially abundant serum metabolites were identified, including a cluster of fatty acyl-CoAs enriched in IBS. We further identified 522 robust associations between differentially abundant gut bacteria and fecal metabolites, of which three species including Odoribacter splanchnicus, Escherichia coli, and Ruminococcus gnavus were strongly associated with the low abundance of dihydropteroic acid. Moreover, dysregulated tryptophan/serotonin metabolism was found to be correlated with the severity of IBS depression in both fecal and serum metabolomes, characterized by a shift in tryptophan metabolism towards kynurenine production. Collectively, our study revealed serum/fecal metabolome alterations and their relationship with gut microbiome, highlighted the massive alterations of serum metabolites, which empower to recognize IBS patients, suggested potential roles of metabolic dysregulation in IBS pathogenesis, and offered new clues to understand IBS depression comorbidity. Our study provided a valuable resource for future studies, and would facilitate potential clinical applications of IBS featured microbiota and/or metabolites.

The electrochemical CO2 conversion to formate is a promising approach for reducing CO2 level and obtaining value-added chemicals, but its partial current density is still insufficient to meet the industrial demands. Herein, we developed a surface-lithium-doped tin (s-SnLi) catalyst by controlled electrochemical lithiation. Density functional theory calculations indicated that the Li dopants introduced electron localization and lattice strains on the Sn surface, thus leading to both the activity and selectivity enhancement of the CO2 electroreduction to formate. The s-SnLi electrocatalyst exhibited one of the best CO2-to-formate performances, including a partial current density of -1.0 A·cm-2 for producing formate and a corresponding Faradaic efficiency of 92%. Furthermore, Zn-CO2 batteries equipped with the s-SnLi catalyst displayed one of the highest power densities of 1.24 mW·cm-2 and an outstanding stability of > 800 cycles. Our work suggests an efficient approach to incorporate the electron localization and lattice strain as the active catalytic sites to synergistically achieve highly efficient CO2-to-formate electrosynthesis toward potential commercialization.

Methyl jasmonate (MeJA) has been widely used to improve the biosynthesis of secondary metabolites such as triterpenoid saponins in medicinal plants. However, the underlying molecular mechanisms remain poorly understood. Differing from roots that accumulate protopanaxatriol-type saponins, Panax notoginseng leaves with a lower biomass mainly contain protopanaxadiol (PPD)-type saponins. Therefore, it is interesting to explore whether MeJA can activate the biosynthesis of PPD-type saponins in P. notoginseng leaves. In this study, we found MeJA could effectively induce the accumulation of PPD-type saponins, including ginsenoside Rb1, Rc, Rb2, Rb3 and notoginsenoside Fa, Fe in P. notoginseng leaves based on a newly established high-performance liquid chromatography method. Transcriptome analysis showed that differentially expressed genes (DEGs) induced by MeJA were mainly enriched in “terpenoid backbone biosynthesis”, “biosynthesis of unsaturated fatty acids”, “sesquiterpenoid and triterpenoid biosynthesis”, “fatty acid metabolism”, and “phenylpropanoid biosynthesis”. Furthermore, the expression profile and quantitative real-time PCR analysis of DEGs showed that MeJA could positively induce the molecular response of endogenous jasmonic acid (JA) signaling pathway, and increased PPD-type saponins mediated by MeJA in P. notoginseng leaves may be related to the high expression of FPS, SS, SE, DS and UGTs, and the low expression of CYP716A53v2 and β-AS. The results provide a molecular understanding for MeJA-elicited biosynthesis of triterpenoid saponins and facilitate the further characterization of the genes responsible for biosynthesis of PPD-type saponins in P. notoginseng leaves.

Summary Treatments that target single mediators of sepsis have failed to reduce its high mortality rate. Here we developed multifunctional tannic acid-Zn2+-gentamicin nanoparticles (TA-Zn-Gen NPs) that target multiple mediators of sepsis to improve sepsis treatment. TA-Zn-Gen NPs with lower gentamicin content possessed net negative surface charge but still bound cell-free DNA (cfDNA) with high affinity. The TA-Zn-Gen NPs exhibited five modes of anti-sepsis activity: (1) scavenged cfDNA and inhibited cfDNA-initiated activation of toll-like receptors and NF-κB signaling; (2) inhibited activated macrophage-induced macrophage recruitment; (3) scavenged reactive oxygen species (ROS) and reduced ROS-induced DNA damage and cell death; (4) inhibited nitric oxide production induced by lipopolysaccharides; and (5) potent antibacterial activity. The NPs reduced multiple organ damage and increased the survival rate of mice with severe sepsis. Together, the results demonstrate the potency of targeting multiple mediators for sepsis treatment, and support the development of multifunctional NPs for treating other intractable inflammation-related diseases.

Biodiesel has great potential as an alternative fuel for diesel engines. However, poor low-temperature flow property and high viscosity of biodiesel limit its use in engines. Therefore, alcohol comes into researchers’ eyes as a promising additive for diesel–biodiesel (DB) blends. In this study, the effects of lower and higher alcohol contents with different speeds on combustion and emissions characteristics were investigated in a modified single cylinder diesel engine. The results indicated that the maximum pressure rise rate (MPRR) maintained a consistent drop ratio as speed increased from 1500 rpm to 1800 rpm for the tested fuels. However, B10E10 (10% biodiesel and %10 ethanol by volume) had a big drop, which meant that engine’s power ability had a big loss at high speed. The declining rate with speed decreased for indicated thermal efficiency (ITE) when adding alcohol to diesel–biodiesel blends, especially n-pentanol. Moreover, compared with other tested fuels, B10P10 (10% biodiesel and 10% n-pentanol) had smaller cycle variation and more stable combustion state as speed changed, despite it had the highest coefficient of variation (COV) at 1000 rpm. It can be found that has advantages in combustion stability, and can well reduce the total hydrocarbon (THC) and carbon monoxide (CO) emissions under the condition of medium speed commonly used by vehicle. Overall consideration, using diesel/biodiesel/alcohol ternary fuels may be a better choice for diesel engines.

Background This study aimed to evaluate the effect of the three-port approach and conventional five-port laparoscopic radical cystectomy (LRC) with an ileal conduit. Methods Eighty-four patients, who were diagnosed with high-risk non-muscle-invasive and muscle-invasive bladder carcinoma and underwent LRC with an ileal conduit between January 2018 and April 2020, were retrospectively evaluated. Thirty and fifty-four patients respectively underwent the three-port approach and five-port LRC. Clinical characteristics, pathological data, perioperative outcomes, and follow-up data were analysed. Results There were no differences in perioperatively surgical outcome, including pathology type, prostate adenocarcinoma incidence, tumour staging, and postoperative creatinine levels between the two groups. The operative time (271.3 ± 24.03 vs. 279.57 ± 48.47 min, P = 0.299), estimated blood loss (65 vs. 90 mL, P = 0.352), time to passage of flatus (8 vs. 10 days, P = 0.084), and duration of hospitalisation post-surgery (11 vs. 12 days, P = 0.922) were no clear difference between both groups. Compared with the five-port group, the three-port LRC group was related to lower inpatient costs (12 453 vs. 14 134 $, P = 0.021). Our follow-up results indicated that the rate of postoperative complications, 90-day mortality, and the oncological outcome did not show meaningful differences between these two groups. Conclusions Three-port LRC with an ileal conduit is technically safe and feasible for the treatment of bladder cancer. On comparing the three-port LRC with the five-port LRC, our technique does not increase the rate of short-term and long-term complications and tumour recurrence, but the treatment costs of the former were reduced.

Background: Cerebral ischemia-reperfusion injury is caused by a blood reperfusion injury in the ischemic brain and usually occurs in the treatment stage of ischemic disease, which can aggravate brain tissue injury. Objective: Curcumin was reported to exert a good therapeutic effect on neural cells against ischemia- reperfusion injury, However, the mechanism is not clear. Methods: In this study, Oxygen-Glucose Deprivation (OGD) model of fetal rat cerebral cortical neurons and the Middle Cerebral Artery Occlusion (MCAO) model of rats were employed to mimic cerebral ischemia-reperfusion injury in vitro and in vivo, respectively. Results: We confirmed that curcumin has a promotive effect on neuronal proliferation and an inhibitory effect on neuronal pyroptosis. Furthermore, we found that curcumin could improve cerebral infarction. The results of western blotting showed that curcumin down-regulated the expression of nucleotide-binding oligomerization domain-containing protein-, leucine-rich repeats-, and pyrin domain-containing protein 1 (NLRP1), cysteinyl aspartate-specific protease 1 (caspase-1), gasdermin D (GSDMD), IL-1β, IL-6, TNF-α, and iNOS proteins in OGD and MCAO models. NLRP1- dependent neuronal pyroptosis played an important role in cerebral ischemia-reperfusion injury. Conclusion: Curcumin could effectively inhibit NLRP1-dependent neuronal pyroptosis by suppressing the p38 MAPK pathway and therefore exerted neuroprotective effects against cerebral ischemia- reperfusion injury.

Feeding low-protein (LP) diets with essential amino acids could be an effective strategy for ruminants from economic, health and environmental perspectives. This study was conducted to investigate the effects of rumen-protected methionine and lysine (RML) in the LP diet on growth performance, innate immunity, and gut health of growing lambs. After 15 days of adaption, sixty-three male Hulunbuir lambs aged approximately 4 months were allotted to three dietary groups and each group had three pens with seven lambs for 60 days. The dietary treatments were as follows: a normal protein diet (14.5% CP, positive control; NP), LP diet (12.5% CP, negative control; LP), and LP diet with RML (12.5% CP, LP + RML). Lambs fed with LP + RML diet showed improved villus architecture and gut barrier function than those fed with the other two diets. The mRNA expressions of interleukin-1β, tumor necrosis factor-α, interferon-γ, toll-like receptor-4, and myeloid differentiation primary response 88 were downregulated in most regions of the intestinal segments by feeding the LP + RML diet. Compared with the NP diet, feeding lambs with the LP diet increased the abundance of Candidatus_Saccharimonas in all regions of the intestinal tract and reversed by feeding the LP + RML diet. Lambs in the LP + RML diet group had lower abundance of Erysipelotrichaceae_UCG-009 and Clostridium_sensu_stricto_1 than those in the LP diet group. The results showed that supplementing RML in the LP diet exhibited beneficial effects on host immune function, intestinal mucosal integrity, and microbiota composition. • Adding methionine and lysine in a low-protein diet improve the intestinal mucosal growth and integrity. • Feeding a low-protein diet with methionine and lysine enhance the innate immune status. • Adding methionine and lysine in a low-protein diet alter the intestinal microbiota composition.

Titanium nitride (TiN) is widely used in electrode materials in fast charging/discharging supercapacitors (SCs) due to its outstanding conductivity. However, the low capacitance of the TiN electrode limits its further application in the SCs. Therefore, the reasonable design of the TiN electrode with high electrochemical and mechanical properties is still a challenge. In this paper, the silicon nanowires/titanium nitride electrode (Si NWs/TiN) is prepared by depositing TiN onto the etched Si nanowires by direct current magnetron sputtering. The Si NWs are prepared by etching silicon in 4.8 M HF/0.02 M AgNO3 aqueous solution for different times (5 min, 15 min, 30 min, 60 min). The mechanism of the effect of etched silicon substrate morphology on the electrochemical performance of Si NWs/TiN electrode was studied. As the etching time increases, the differences of the TiN surface structure, lattice defects and surface chemical composition will change the capacitance performance and charge storage mechanism of the Si NWs/TiN electrode. The prepared Si30 NWs/TiN electrode exhibits an outstanding specific capacitance as high as 113.55 F g−1 at a scan rate of 5 mV s−1 with 0.5 M H2SO4 solution as electrolyte. The specific capacitance of the Si30 NWs/TiN electrode is as high as 7.5 times that of the electrode without etching at 100 mV s−1. The Si30 NWs/TiN electrode has an excellent cyclic stability performance, which the electrode has a decay rate of 12.4% after 2000 cycles. This indicates that the electrode has reliable stability. The electrode of the supercapacitor prepared by this method can open up a new way to expand the specific surface area of other transition metal nitride.

Microarc oxidation (MAO) is a popular surface treatment process to generate oxide coatings with excellent mechanical properties on valve metals. As a plasma discharge technique, the discharge mechanism in MAO is different from that in the bipolar plate. Due to the alternating arcs and multiple electrolytes in MAO, it is difficult to control and optimize the coating properties. Based on the arcing mechanism and ion motion, the boundary conditions of no-arc discharge, alternating arc discharge, and continuous arc discharge are derived, and the relationship between the discharge current and breakdown current and sustained arc current is investigated. For the same electrolyte, the boundary conditions are determined by equivalent concentration and conductivity. The results show that in the stable alternating arc discharge regime, the higher the concentration and smaller the conductivity, the more intense is the discharge. According to the boundary conditions, MAO experiments are designed using phosphate electrolytes to improve the hardness of oxide coatings. By selecting electrolyte characteristics close to the continuous arc discharge boundary in the stable alternating arc discharge regime, the arc discharge is most intense and brightest and the largest energy is transferred to the Al2O3 coating. Consequently, the crystallinity and mechanical properties are improved significantly.

The renewable energy-powered electroreduction of carbon dioxide or monoxide (CO) has been emerging as an attractive means to decarbonize the emission-intensive chemical manufacturing, which heavily relies on fossil fuels nowadays. One potential approach to promote the activity of electrocatalysts is to construct hybrid interface that can increase the stability of intermediates on electrode surfaces. Herein we developed a copper nanoparticle/polypyrrole (Cu-Ppy) nanowire composite as an efficient electrocatalyst for electrochemical CO reduction reaction. Compared to pure Cu nanoparticles, the Cu-Ppy composite exhibited a dramatically enhanced Faradaic efficiency of converting CO to ethylene (C2H4) from 34% to 69% at −0.78 V vs. reversible hydrogen electrode (RHE) in KOH electrolyte, and an excellent C2H4 partial current density of 276 mA·cm−2 at −1.18 V vs. RHE. Density functional theory calculations showed that the Cu-Ppy composite could bind CO more strongly as compared to pure Cu. As the Ppy coating allowed to stabilize OCCO*, a key intermediate in the C2H4 formation, both the activity and selectivity of Cu-Ppy for CO-to-C2H4 were increased. Our work suggests that constructing rationally designed hybrid interface can tune the local environment of catalyst surface toward enhanced activity and product selectivity.

A single-crystal islands (SCI) technique using low thermal budget pulse laser process is proposed and demonstrated to fabricate single-crystal silicon islands over amorphous dielectric for monolithic 3-D and back-end-of-line (BEOL) FinFET circuits. By laser recrystallizing mask-defined a-Si islands encapsulated with conformal silicon nitride film, designed single-crystal Si islands can be obtained. The single crystallinity of the island are verified with SECCO Etch, high-resolution electron microscopy (HREM), transmission electron microscopy (TEM), and electron backside scattering (EBSD). About 40 nm FinFETs were successfully fabricated in the SCI Si islands and shown to exhibit excellent electrical performance and low variability that are compatible with the FinFETs fabricated on commercial silicon-on-insulator (SOI) wafer.

The exploration of future energy storage devices with lightweight, flexible, and highly efficient energy management strategy has attracted increased interest in recent years. The design and implementation of unique supercapacitor electrodes are expected to overcome these challenges. Herein, we report a facile electrochemical polymerization method to prepare sandpaper-based conductive polymer flexible supercapacitors. The prepared electrodes present hollow barnacle-like structure, and the maximum specific capacitance of the assembled supercapacitor is 303.3 mF cm−2. After 10,000 charge–discharge cycles, the capacitance retention maintains 92.7%. Moreover, the device has good flexibility, and the capacitance retention is as high as 92.5% after 2000 bending cycles, which is of great significance to applications.

Coencapsulation of chemotherapeutic agents and photosensitizers into nanocarriers can help to achieve a combination of chemotherapy and photodynamic therapy for superior antitumor effects. However, precise on-demand drug release remains a major challenge. In addition, the loaded photosensitizers usually tend to aggregate, which can significantly weaken their fluorescent signals and photodynamic activities. To address these issues, herein, a smart nanocarrier termed as singlet oxygen-responsive nanoparticle (SOR-NP) was constructed by introducing singlet oxygen (1O2)-sensitive aminoacrylate linkers into amphiphilic mPEG-b-PCL copolymers. Boron dipyrromethene (BDP) and paclitaxel (PTX) as model therapeutic agents were coloaded into an 1O2-responsive nanocarrier for realizing light-controlled drug release and combination cancer treatment. This polymeric nanocarrier could substantially relieve the aggregation of encapsulated BDP due to the presence of a long hydrophobic chain. Therefore, the formed SOR-NPBDP/PTX nanodrug could generate bright fluorescent signals and high levels of 1O2, which could mediate cell death via PDT and rupture aminoacrylate linker simultaneously, leading to collapse of SOR-NPBDP/PTX and subsequent PTX release. The light-triggered drug release and combined anticancer effects of SOR-NPBDP/PTX were validated in HepG2 and MCF-7 cancer cells and H22 tumor-bearing mice. This study provides a promising strategy for tumor-specific drug release and selective photodynamic-chemo combination treatment.

A fast and simple ultra-high performance supercritical fluid chromatography method has been developed for the determination of six analytes, namely (paeonol, coumarin, cinnamic alcohol, cinnamic acid, paeoniflorin and amygdalin) in Guizhi Fuling capsule and tablet samples. The influence of the key chromatographic parameters for the separation purposes was evaluated. The optimal column was Trefoil CEL1 column. The optimal mobile phase was a gradient mixture of carbon dioxide and methanol at flow rate of 1.0 mL min-1 . The back pressure of the system was set to 1.38×107 Pa and the temperature to 45 ℃. The six compounds were separated within 11 min by the proposed ultra-high performance supercritical fluid chromatography method with satisfactory resolution. Method validation confirmed that the procedure is accurate with the recovery rates from 87.04% to 104.30%, intra-day precision values less than less than 4.81% and inter-day precision less than 5.22%, and linear with R2 higher than 0.9967. Therefore, this work provides a simple and novel method for the simultaneous analysis of six compounds in Guizhi Fuling capsule and tablet samples. This article is protected by copyright. All rights reserved.

Insufficient active sites and fast charge carrier recombination are detrimental to photocatalytic activity of graphitic carbon nitride (g-C3N4). In this work, a combination of pore creating with thermal exfoliation was employed to prepare porous g-C3N4 nanosheets for photocatalytic water splitting into hydrogen. Hexadecyl trimethyl ammonium chloride (CTAC) as the soft template promoted the formation of porous g-C3N4 during the thermal condensation of melamine. On further post-synthesis calcination, the porous g-C3N4 aggregates were exfoliated into discrete nanosheets, accompanied by an increase in specific surface area and defects. Optimal porous g-C3N4 nanosheets achieved 3.6 times the photocatalytic hydrogen evolution rate for bulk counterpart. The enhanced photocatalytic activity may be ascribed to TCN-1%CTAC has larger specific surface area, stronger optical absorption intensity and higher photogenerated electron–hole separation efficiency. The external quantum efficiency of TCN-1%CTAC was measured to be 3.4% at 420 nm. This work provides a simple combinatorial strategy for the preparation of porous g-C3N4 nanosheets with low cost, environmental friendliness and enhanced photocatalytic activity.

Halloysite nanotubes (HNTs) were employed to design and synthesize palladium-based heterogeneous catalysts with the purpose of exploring an efficient non-mercuric catalyst for acetylene hydrochlorination. Various Pd/UHNTs catalysts with urea modification were prepared using ultrasonic-assisted impregnation method and the Pd/9UHNTs catalyst exhibited the best catalytic performance, with 90% acetylene conversion and above 94% vinyl chloride selectivity under the reaction conditions of T = 160 °C, a C2H2 gas hourly space velocity (GHSV) = 150 h−1 and V(HCl): V(C2H2) = 1.25. The results demonstrated that the urea additive (mainly nitrogen species) significantly immobilized Pd species and inhibited the carbon deposition on the catalyst surface, thus contributing to enhance the catalytic performance of Pd/HNTs catalysts during the reaction.

Renewable energy-powered methane (CH4 ) conversion at ambient conditions is an attractive but highly challenging field. Due to the highly inert character of CH4 , the selective cleavage of its first C-H bond without over-oxidation is essential for transforming CH4 into value-added products. In this work, we developed an efficient and selective CH4 conversion approach at room temperature using intermediate chlorine species (*Cl), which were electrochemically generated and stabilized on mixed cobalt-nickel spinels with different Co/Ni ratios. The lower overpotentials for *Cl formation enabled an effective activation and conversion of CH4 to CH3 Cl without over-oxidation to CO2 , and Ni3+ at the octahedral sites in the mixed cobalt-nickel spinels allowed to stabilize surface-bound *Cl species. The CoNi2 Ox electrocatalyst exhibited an outstanding yield of CH3 Cl (364 mmol g-1 h-1 ) and a high CH3 Cl/CO2 selectivity of over 400 at room temperature, with demonstrated capability of direct CH4 conversion under seawater working conditions.

Glycosylation is important for biological functions of proteins and greatly affected by diseases. Exploring the glycosylation profile of the protein-specific glycosylation and/or the site-specific glycosylation may help understand disease etiology, differentiate diseases and ultimately develop therapeutics. Patients with multiple sclerosis (MS) and patients with neuromyelitis optica spectrum disorder (NMOSD) are sometimes difficult to differentiate due to the similarity in their clinical symptoms. The disease-related glycosylation profiles of MS and NMOSD have not yet been well studied. Here, we analyzed site-specific glycan profiles of serum proteins of these patients by using a recently developed mass spectrometry technique. A total of 286 glycopeptides from 49 serum glycoproteins were quantified and compared between healthy controls (n = 6), remitting MS (n = 45) and remitting NMOSD (n = 23) patients. Significant differences in the levels of site-specific N-glycans on inflammation-associated components [IgM, IgG1, IgG2, complement components 8b (CO8B) and attractin], central nerve system-damage-related serum proteins [apolipoprotein D (APOD), alpha-1-antitrypsin, plasma kallikrein and ADAMTS-like protein 3] were observed among three study groups. We furthered demonstrated that site-specific N-glycans on APOD on site 98, CO8B on sites 243 and 553 are potential markers to differentiate MS from NMOSD with an area under receiver operating curve value > 0.75. All these observations indicate that remitting MS or NMOSD patients possess a unique disease-associated glyco-signature in their serum proteins. We conclude that monitoring one’s serum protein glycan profile using this high-throughput analysis may provide an additional diagnostic criterion for differentiating diseases, monitoring disease status and estimating response-to-treatment effect.

Cancer metastasis is still a major obstacle in clinical cancer therapy and a paramount cause of cancer deaths. Designing multifunctional nanoplatforms with an enhanced diagnostic sensitivity and anti-metastasis efficiency against tumors represents a major trend in current cancer management. Herein, we report the preparation of low-molecular-weight poly(ethylenimine) (PEI)-poly(ethylene glycol) (PEG) nanogels (NGs) loaded with transforming growth factor-β1 (TGF-β1) siRNA and ultrasmall iron oxide nanoparticles (Fe3O4 NPs) for gene therapy and T1-weighted magnetic resonance (MR) imaging of tumors and tumor metastasis in a mouse sarcoma model. In this work, ultrasmall Fe3O4 NPs stabilized by sodium citrate were first prepared and then mixed with PEI (800 Da) and PEG (400 Da)-diacrylate as a cross-linker to form Fe3O4/PEI-PEG NGs with an average size of 76.3 nm via an inverse microemulsion method. The developed hybrid NGs display good cytocompatibility and enhanced MR imaging performance (r1 relaxivity = 1.0346 mM-1 s-1). The Fe3O4/PEI-PEG NGs can be further used to compact TGF-β1 siRNA through electrostatic interaction and efficiently deliver siRNA to cancer cells and a tumor model to silence the TGF-β1 gene, which inhibits the growth and invasion of cancer cell in vitro significantly, as well as the growth of a subcutaneous sarcoma tumor model and lung metastasis in vivo. The designed hybrid NG-ultrasmall iron oxide NPs may be extended for the delivery of other drugs or genes for theranostics of different biological systems.

Background The beneficial effects of ω−3 polyunsaturated fatty acids (PUFA) vary between different sources. However, there is a paucity of comparative studies regarding the effects and mechanisms of marine and plant ω−3 PUFA on obesity. Objective The aim of this study was to evaluate the effects of fish oil (FO) and perilla oil (PO) on glucolipid metabolism, inflammation, and adipokine in mice fed a high-fat (HF) diet in association with the contribution of toll-like receptor 4 (TLR4)/myeloid differentiation primary response 88 (MyD88) pathway. Methods C57BL/6J mice and MyD88−/− mice were randomly divided into 4 groups: normal chow diet, HF diet, HF diet accompanied by daily gavage with either FO or PO. After 4 weeks, blood biochemistries, adipocyte histology, mRNA, and protein expression of MyD88-dependent and -independent pathways of TLR4 signaling in epididymal adipose tissue were measured. Results In C57BL/6J mice, there were no statistical differences between FO and PO in decreasing body weight, glucose, insulin, triglyceride, total cholesterol, interleukin-6, and increasing adipocyte counts. FO and PO decreased mRNA and protein expression of TLR4, MyD88, tumor necrosis factor receptor-associated factor 6, inhibitor of nuclear factor kappa B kinase beta and nuclear factor-kappa B p65. In MyD88−/− mice, the beneficial effects of FO and PO on HF diet-induced metabolism abnormalities and inflammation were abolished. FO and PO had no impacts on mRNA and protein expression of receptor-interacting protein-1, interferon regulate factor 3, and nuclear factor-kappa B p65. Conclusion FO and PO exhibit similar protective effects on metabolic disorders and inflammation through inhibiting TLR4 signaling in a manner dependent on MyD88. These findings highlight plant ω−3 PUFA as an attractive alternative source of marine ω−3 PUFA and reveal a mechanistic insight for preventive benefits of ω−3 PUFA in obesity and related metabolic diseases.

This study tested the hypothesis that therapy with double overexpression of miR‐19a‐3p and miR‐20a‐5p (miRDOE) to human inducible pluripotent stem cell–derived mesenchymal stem cells (iPS‐MSCs) was superior to iPS‐MSCs alone for preserving renal function in rat with pre‐existing chronic kidney disease (CKD), followed by ischaemia‐reperfusion (IR) injury. In vitro study demonstrated that the protein expressions of oxidative stress (NOX‐1/NOX‐2/NOX4/oxidized protein/p22phox), inflammatory downstream signalling (TLR2&4/MyD88/TRAF6/IKK‐ß/p‐NFκB/IL‐1ß/IL‐6/MMP‐9) and cell apoptosis/death signalling (cleaved caspase‐3/mitochondrial Bax/p‐ERKs/p‐JNK/p‐p38) at time‐points of 24‐hour/48‐hour cell cultures were significantly increased in p‐Cresol‐treated NRK‐52E cells than in the control that was significantly reversed by miR‐19a‐3p‐transfected iPS‐MSC (all P

4-Hydroxyphenylpyruvate dioxygenase (HPPD) is an important target for both drug and pesticide discovery. As a typical Fe(II)-dependent dioxygenase, HPPD catalyzes the complicated transformation of 4-hydroxyphenylpyruvic acid (HPPA) to homogentisic acid (HGA). The binding mode of HPPA in the catalytic pocket of HPPD is a focus of research interests. Recently, we reported the crystal structure of Arabidopsis thaliana HPPD (AtHPPD) complexed with HPPA and a cobalt ion, which was supposed to mimic the pre-reactive structure of AtHPPD-HPPA-Fe(II). Unexpectedly, the present study shows that the restored AtHPPD-HPPA-Fe(II) complex is still nonreactive toward the bound dioxygen. QM/MM and QM calculations reveal that the HPPA resists the electrophilic attacking of the bound dioxygen by the trim of its phenyl ring, and the residue Phe381 plays a key role in orienting the phenyl ring. Kinetic study on the F381A mutant reveals that the HPPD-HPPA complex observed in the crystal structure should be an intermediate of the substrate transportation instead of the pre-reactive complex. More importantly, the binding mode of the HPPA in this complex is shared with several well-known HPPD inhibitors, suggesting that these inhibitors resist the association of dioxygen (and exert their inhibitory roles) in the same way as the HPPA. The present study provides insights into the inhibition mechanism of HPPD inhibitors.

A Cd(ΙI)-based luminescent coordination polymer, namely [Cd(L)2(H2O)2]n (1), has been synthesized by 1-(tetrazo-5-yl)-4-(triazo-1-yl)benzene ligand (HL) and structurally characterized. The selectiv...

Exploring novel p-hydroxyphenylpyruvate dioxygenase (EC 1.13.11.27, HPPD) inhibitors has become one of the most promising research directions in herbicide innovation. On the basis of our tremendous interest in exploiting more powerful HPPD inhibitors, we designed a family of benzyl-containing triketone-aminopyridines via a structure-based drug design (SBDD) strategy and then synthesized them. Among these prepared derivatives, the best active 3-hydroxy-2-(3,5,6-trichloro-4-((4-isopropylbenzyl)amino)picolinoyl)cyclohex-2-en-1-one (23, IC50 = 0.047 μM) exhibited a 5.8-fold enhancement in inhibiting Arabidopsis thaliana (At) HPPD activity over that of commercial mesotrione (IC50 = 0.273 μM). The predicted docking models and calculated energy contributions of the key residues for small molecules suggested that an additional π-π stacking interaction with Phe-392 and hydrophobic contacts with Met-335 and Pro-384 were detected in AtHPPD upon the binding of the best active compound 23 compared with that of the reference mesotrione. Such a molecular mechanism and the resulting binding affinities coincide with the proposed design scheme and experimental values. It is noteworthy that inhibitors 16 (3-hydroxy-2-(3,5,6-trichloro-4-((4-chlorobenzyl)amino)picolinoyl)cyclohex-2-en-1-one), 22 (3-hydroxy-2-(3,5,6-trichloro-4-((4-methylbenzyl)amino)picolinoyl)cyclohex-2-en-1-one), and 23 displayed excellent greenhouse herbicidal effects at 150 g of active ingredient (ai)/ha after postemergence treatment. Furthermore, compound 16 showed superior weed-controlling efficacy against Setaria viridis (S. viridis) versus that of the positive control mesotrione at multiple test dosages (120, 60, and 30 g ai/ha). These findings imply that compound 16, as a novel lead of HPPD inhibitors, possesses great potential for application in specifically combating the malignant weed S. viridis.

In this study, pure tetragonal zirconia (t-ZrO2), with an average size of approximately 7 nm, was prepared by a modified hydrothermal method using zirconium nitrate (Zr(NO3)4) as the zirconium source and glycerol as the additive. The effects of pH and glycerol content on the phase and morphology of the ZrO2 were investigated, and the mechanism is discussed herein. The tetragonal phase gradually increased with an increase in pH, while the grain size of the powder gradually decreased. The effect of glycerol addition on the crystal phase of the powder was also investigated, and the results showed that the monoclinic phase gradually decreased with an increase in the amount of glycerol added. With a glycerol to zirconium molar ratio of 3:1, a single tetragonal phase was produced. In addition, a high-performance ZrO2 ultrafiltration membrane was prepared by coating the inner surface of the tubular ZrO2 membrane. The characterization results show that the thickness of the membrane was approximately 1.5 μm, the pure water flux was approximately 84 L m−2 h−1·bar−1, and the molecular weight cut-off was approximately 7000 Da. The reproducibility of the high-performance ZrO2 ultrafiltration membranes was also evaluated. It was found that the synthesised ZrO2 membrane has high reproducibility and stability.

The application of flexible, robust, and low-cost solid polymer electrolytes in next-generation all-solid-state lithium metal batteries has been hindered by the low room-temperature ionic conductivity of these electrolytes and the small critical current density of the batteries. Both issues stem from the low mobility of Li+ ions in the polymer and the fast lithium dendrite growth at the Li metal/electrolyte interface. Herein, Mg(ClO4)2 is demonstrated to be an effective additive in the poly(ethylene oxide) (PEO)-based composite electrolyte to regulate Li+ ion transport and manipulate the Li metal/electrolyte interfacial performance. By combining experimental and computational studies, we show that Mg2+ ions are immobile in a PEO host due to coordination with ether oxygen and anions of lithium salts, which enhances the mobility of Li+ ions; more importantly, an in-situ formed Li+-conducting Li2MgCl4/LiF interfacial layer homogenizes the Li+ flux during plating and increases the critical current density up to a record 2 mA cm-2. Each of these factors contributes to the assembly of competitive all-solid-state Li/Li, LiFePO4/Li, and LiNi0.8Mn0.1Co0.1O2/Li cells, demonstrating the importance of surface chemistry and interfacial engineering in the design of all-solid-state Li metal batteries for high-current-density applications.

Lipophilic shellfish toxins pose significant threats to the health of seafood consumers and public health. The symptoms of these kinds of toxins include severe diarrhea, abdominal cramps, nausea and gastrointestinal disorders. These symptoms could be hardly distinguished with many other symptoms of food poisoning and diseases. Therefore, a fast and accurate determination method in human biological samples is urgently needed for the accurate judgement of food poisoning incident, which is important for the investigation of public health emergencies and clinical treatment of poisoned patients. However, there were several flaws of the previous studies reported on the analysis of lipophilic shellfish toxins: (1) limited target compounds were covered; (2) the pre-treatment process was complex; (3) the sensitivity of the compound was low. In this study, a simple extraction method coupled with ultra-high performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS) was developed for the simultaneous determination of 12 lipophilic shellfish toxins, including azaspir acid 1 (AZA1), azaspir acid 2 (AZA2), azaspir acid 3 (AZA3), dinophysistoxin 1 (DTX1), dinophysistoxin 2 (DTX2), gymnodimine (GYM), hyessotoxin (HYTX), okadaic acid (OA), pinnatoxin (Pntx), pectenotoxins 2 (PTX2), spirolides 1 (SPX1), yessotoxin (YTX), in plasma and urine. Firstly, the instrument conditions were optimized. Different additions in mobile phase were compared and 0.05% (v/v) ammonia solution was selected since it can improve the peak shape of YTX and HYTX, and increase the respondence by four times. Secondly, the volume of acetonitrile (0.2, 0.4, 0.6, 0.8, 1.0 mL) use for the extraction of the target compounds in plasma was optimized. Satisfactory recoveries were obtained when 0.6 mL of acetonitrile was used. At the same time, satisfactory recoveries were obtained when 0.9 mL of acetonitrile was used in urine samples. Finally, under the optimized conditions, the 12 compounds in plasma and urine samples were ultrasonically extracted with acetonitrile. Chromatographic separation was performed on a Phenomenex Kinetex C18 column (50 mm×3 mm, 2.6 μm) with 90% (v/v) acetonitrile aqueous solution and water containing 0.05% (v/v) ammonia as mobile phases. Gradient elution with a flow rate of 0.40 mL/min was employed. The 12 compounds were monitored in the multiple reactions monitoring (MRM) mode with electrospray ionization (ESI) under both positive and negative conditions. The matrix effects of the 12 compounds ranged from 0.8 to 1.1. Therefore, external standard calibration curves were used for the quantification. The 12 shellfish toxins showed good linear relationship in the range of 0.03-36.25 μg/L with the correlation coefficients greater than 0.995. The limits of detection (LODs, S/N=3) were 0.08-0.21 ng/mL for the urine samples and 0.10-0.28 μg/L for the plasma samples, respectively. The limit of quantitations (LOQs, S/N=10) were 0.23-0.63 μg/L for the urine samples and 0.31-0.84 μg/L for the plasma samples, respectively. The recoveries of the 12 compounds were in the range of 72.7%-124.1% at three spiked levels (i. e., LOQ, three times LOQ, and ten times LOQ). The intra-day and inter-day precisions were 2.1%-20.0% and 2.1%-15.3%, respectively. The method was applied in the detection of the 12 lipophilic shellfish toxins in the urine and plasma samples of healthy humans and mice previously injected with the 12 shellfish toxins intraperitoneally. None of the 12 toxins were found in the samples from healthy human, while all of the 12 lipophilic shellfish toxins were found in the urine and plasma samples collected from the poisoned mice in the range of 1.14-2.35 μg/L and 1.01-1.17 μg/L, respectively. The established method has the advantages of sensitive, quick, easy to operate, and of low sample volume. It can be used for the simultaneous determination of 12 lipophilic shellfish toxins in urine and plasma samples.

Co(II) and Cu(II) complexes, [Co2(H2L)2(phen)2(H2O)4](H2O)2 (1) and [Cu2(L)0.5(phen)2Cl2]n (2) [H4L = 5,5'-(diazene-1,2-diyl)diisophthalic acid, phen = 1,10-phenanthroline], have been solvothermall...

It is well accepted that grain-boundary phases in metallic alloys greatly deteriorate the mechanical properties. In our work, we report on a novel strategy to prepare high strength-ductility β-type (Ti69.71Nb23.72Zr4.83Ta1.74)97Si3 (at.%) (TNZTS) alloys by tailoring grain-boundary metastable Si-containing phase. Specifically, the thin shell-shaped metastable S1 phase surrounding the columnar β-Ti grain was intercepted successfully via nonequilibrium rapid solidification achieved by selective laser melting (SLM). Subsequently, the thin shell-shaped metastable (Ti, Nb, Zr)5Si3 (called S1) phase was transformed into globular (Ti, Nb, Zr)2Si (called S2) phase by the solution heat treatment. Interestingly, the globular S2 phases reinforced TNZTS alloy exhibits ultrahigh yield strength of 978 MPa, ultimate strength of 1010 MPa and large elongation of 10.4 %, overcoming the strength–ductility trade-off of TNZTS alloys by various methods. Especially, the reported yield strength herein is ∼55 % higher than that of conventionally forged TNZT alloys. Dynamic analysis indicates the globularization process of the metastable S1 phase is controlled by the model of termination migration. The quantitative analysis on strengthening mechanism demonstrates that the increase in yield strength of the heat-treated alloys is mainly ascribed to the strengthening of the precipitated silicide and the dislocations induced by high cooling rate. The obtained results provide some basis guidelines for designing and fabricating β-titanium alloys with excellent mechanical properties, and pave the way for biomedical application of TNZTS alloy by SLM.

Organozirconium chemistry has found extensive applications in organic synthesis since its discovery in the last century. Alkyl­zirconocenes, which are easily generated by the hydrozirconation of alkenes with the Schwartz reagent, are widely utilized for carbon–carbon­ and carbon–heteroatom bond formation. This short review summarizes the progress to date on the applications alkylzirconocenes in organic synthesis.1 Introduction2 General Methods for Generating Alkylzirconocenes3 Transformations of Alkylzirconocenes by Heteroatoms4 Insertion of Unsaturated Groups into Alkylzirconocenes5 Transmetalations6 Cross-Coupling Reactions of Alkylzirconocenes7 Photochemistry of Alkylzirconocenes8 Bimetallic Reagents of Zirconium9 Asymmetric Transformations10 Applications of Alkylzirconocenes Generated from the Negishi Reagent11 Conclusions and Outlook

Sulfidated zerovalent iron (S-ZVI) has been extensively used for reducing pollutants. In this study, the oxidation process in the reductive removal of p-nitrophenol (PNP) by S-ZVI was confirmed under anaerobic conditions. We revealed that a PNP oxidation process involving •OH resulted from the H2O2 activation by surface-bound Fe(II) in S-ZVI, in which H2O2 was generated via a surface-mediated reaction between water and FeS2. Only the PNP reduction process occurred for ZVI. Herein, efficient PNP degradation by S-ZVI resulted from two functions: reduction into p-aminophenol due to enhanced electron transfer and PNP oxidation into p-benzoquinone by •OH radicals from the interaction of surface-bound Fe(II) and in situ generated H2O2, the contributions of the oxidation and reduction processes to PNP degradation over S-ZVI were 10 and 90%, respectively. Sulfur in S-ZVI suppressed the pH increase in the reaction media and produced more surface-bound Fe(II) than ZVI for •OH generation via the heterogeneous Fenton reaction process. Since different degradation pathways could lead to different effects on the water environment, such as toxicity, our findings suggest that the oxidizing process induced by S-ZVI during groundwater decontamination should be considered.

Herbicide resistance has become one of the foremost problems in crop production worldwide. New herbicides are required to manage weeds that have evolved resistance to the existing herbicides. However, relatively few herbicides with new modes of action (MOAs) have been discovered in the past two decades. Therefore, the discovery of new herbicides (i.e., new chemical classes or MOAs) remains a primary but ongoing strategy to overcome herbicide resistance and ensure crop production. In this mini-review, starting with the inherent characteristics of the target proteins and the inhibitor structures, we propose two strategies for the rational design of new herbicides and one computational method for the risk evaluation of target mutation-conferred herbicide resistance. The information presented here may improve the utilization of known targets and inspire the discovery of herbicides with new targets. We believe that these strategies may trigger the sustainable development of herbicides in the future. © 2021 Society of Chemical Industry.

Summary Electrochemical CO2 reduction is a promising approach for upgrading excessive CO2 into value-added chemicals, while the exquisite control of the catalyst atomic structures to obtain high C2+ alcohol selectivity has remained challenging due to the intrinsically favored ethylene pathways at Cu surface. Herein, we demonstrate a rational strategy to achieve ∼70% faradaic efficiency toward C2+ alcohols. We utilized a CO-rich environment to construct Cu catalysts with stepped sites that enabled high surface coverages of ∗CO intermediates and the bridge-bound ∗CO adsorption, which allowed to trigger CO2 reduction pathways toward the formation alcohols. Using this defect-site-rich Cu catalyst, we achieved C2+ alcohols with partial current densities of > 100 mA·cm−2 in both a flow-cell electrolyzer and a membrane electrode assembly (MEA) electrolyzer. A stable alcohol faradaic efficiency of ∼60% was also obtained, with ∼500 mg C2+ alcohol production per cm2 catalyst during a continuous 30-h operation.

The pursuit of energy density has driven electric vehicle (EV) batteries from using lithium iron phosphate (LFP) cathodes in early days to ternary layered oxides increasingly rich in nickel; however, it is impossible to forgo the LFP battery due to its unsurpassed safety, as well as its low cost and cobalt-free nature. Here we demonstrate a thermally modulated LFP battery to offer an adequate cruise range per charge that is extendable by 10 min recharge in all climates, essentially guaranteeing EVs that are free of range anxiety. Such a thermally modulated LFP battery designed to operate at a working temperature around 60 °C in any ambient condition promises to be a well-rounded powertrain for mass-market EVs. Furthermore, we reveal that the limited working time at the high temperature presents an opportunity to use graphite of low surface areas, thereby prospectively prolonging the EV lifespan to greater than two million miles. Ternary layered oxides dominate the current automobile batteries but suffer from material scarcity and operational safety. Here the authors report that, when operating at around 60 °C, a low-cost lithium iron phosphate-based battery exhibits ultra-safe, fast rechargeable and long-lasting properties.

A new Cu(II) coordination polymer (CP) of [Cu5(µ3-OH)2(bcpt)4(bib)2] (1, bib = 1,4-bis(1-imidazoly)benzene and H2bcpt = 3,5-bis(3′-carboxyphenyl)-1,2,4-triazole) was synthesized by reaction of Cu(N...

Unprecedented palladium-catalysed regio- and stereo-selective coupling reactions of homoallenylboronates with (hetero)aryl iodides, allyl bromides and alkynyl bromides in aqueous solution were successfully developed. The corresponding 1,3-dienes, skipped dienes and conjugate enynes were obtained as products, respectively, in high yields and with specific stereoselectivity. Therefore, the homoallenylboronates were potentially powerful and flexible “platform” molecules to form the complex 1,3-dienyl compounds.

Mn-based Prussian blue analogue is regarded as one of the promising cathodes for sodium ions battery owing to its high theoretical capacity and low cost. However, the unstable structure during charging/discharging process and the poor cycle life hinder its commercial application. In this work, potassium ions stabilized hollow Mn-based Prussian blue analogue is synthesized through a simple sodium citrate assisted method using for cathode of sodium-ions batteries. Although unique hollow structure could suffer volume variation during charging/discharging process, the K+ is introduced to further stabilize its structure. The PBAs cathode exhibits a high reversible specific capacity of 128 mA h g−1 at 50 mA and superior rate performance of 72 mA h g−1 at a high current density of 3200 mA g−1, which is attributed to its stable structure and enhanced sodium ions transport kinetics. Ex-situ XRD/Raman tests and electrochemical measurements further prove the synergistic effect of various alkali ions (K+/Na+) and unique hollow structure. They work together to improve the structural stability and promote sodium ions diffusion rate of Mn-based PBAs.

The electrocatalytic reduction of carbon monoxide (CO) is an emerging direction with new catalyst structures, among which the bimetallic component catalysts feature both functional diversity and high-density of active sites. In this work, we demonstrate that the fine tuning of adjacent bimetallic sites can allow us to select different reaction pathways toward C1 or C2 products in the electroreduction of CO. Cu and Cu–Au alloy catalysts with different atomic ratios were fabricated and investigated for appropriate molecular distances. The pure Cu catalyst was found to be active for electroreducing CO to C2H4, as the adjacent Cu sites were beneficial for adsorbing multiple CO molecules and subsequent C–C coupling. On the other hand, alloying Cu with Au introduced steric hindrance and a larger intermolecular distance between adjacent adsorbed *CO intermediates, thus leading to a decrease of C2H4 selectivity but an enhanced CH4 pathway. Our work revealed the importance of spacing between active sites for CO electroreduction, which can benefit the catalyst design to further improve activities and selectivities in electrocatalytic CO reduction.

A novel "double-locked" probe, DCO-H2S-V, was prepared for detecting hydrogen sulfide in a highly viscous system. Experiments demonstrated that only when H2S and a high viscosity environment coexist in a cell, can the probe be activated effectively and emit fluorescence. This has been successfully used for detecting the changes in viscosity and H2S in a Parkinson's disease model, PC-12 cells treated with glutamate.

This article presents the first dedicated system-on-chip (SoC) that supports full data analysis workflow for genetic variant discovery for next-generation sequencing (NGS). The SoC implements four major steps: preprocessing, short-read mapping, haplotype calling, and variant calling. By adopting the sBWT-based short read mapping and Genome Analysis ToolKit haplotype caller-based variant calling algorithms, this work achieves a comparable precision as the software solutions. The dedicated hardware architecture achieves high parallelism with low hardware complexity. In this SoC, the multitask sorting engine and the dynamic programming processing engine are proposed for essential computing tasks for NGS data analysis. An ARC processor is integrated to facilitate IO interfaces, including a DDR3 PHY. Fabricated in a 28-nm technology, the chip area is 12 mm2. It dissipates 975 mW at a clock frequency of 400 MHz from a 0.9-V supply. The SoC is able to complete variant discovery for the whole human genome within 37 min. Compared with an optimized graphic processing unit solution, this work is 66 $\times $ faster and also achieves an $1.59\times 10^{4}$ times higher energy efficiency and 3086 $\times $ higher area efficiency. Verified with the FDA standardized benchmark, the SoC achieves a precision of 99.6%. The prototype system demonstrates the analysis procedure in real time for on-site DNA sequencing.

In this study, we prepare dispersed MoS2 nanosheets by water bath ultrasonic stripping method uniformly. The MoS2 nanosheets are characterized by SEM, TEM and XRD, and then the gas formic acid is detected in detail. The experimental results show that the sensor patterned with MoS2 nanosheets has high response to formic acid gas with the response time of 11s, and the recovery time of 17s. The sensor exhibits excellent selectivity, repeatability and stability under a linear relationship between the resistance of the sensor and the gas concentration.