Reaction-Driven Dynamic and Reversible Transformations of Au Single Atoms and Au-Zr Alloys on Zirconia for Efficient Acetylene Hydrochlorination.

Catalysis involving gold supported on metal oxides has undergone extensive examination. However, the nature of the catalytic site under actual reaction conditions and the role of the support continue to be vigorously debated. This study addresses these issues through experimental investigations and theoretical simulations. We explore a novel catalytic mechanism that employs dynamic single-atom catalysis for the hydrochlorination of acetylene. This catalytic mechanism occurs in defective ZrO2-supported Au-Zr single-atom alloys. Specifically, the dynamic single-atom catalysis is a result of the mobility of the gold cation, which is accelerated by Cl radicals and strongly couples with the abundant unsaturated surface sites of ZrO2 in a synergistic manner. As a result, the Au electronic structure dynamically evolves, leading to a decrease in the addition reaction energy barrier. Notably, the Au cation can detach from the Au-Zr alloy structure to catalyze the hydrochlorination of acetylene near the Zr-Ov-Zr sites and then reintegrate back into the Au-Zr alloy structure upon completion of the reaction. This study underscores the significance of dynamic active sites under reaction conditions and their pivotal role in catalysis.

Sialic acid in human milk and infant formulas in China: concentration, distribution and type.

This study compared the concentrations, types and distributions of sialic acid (SA) in human milk at different stages of the postnatal period with those in a range of infant formulas. Breast milk from mothers of healthy, full-term and exclusively breastfed infants was collected on the 2nd (n 246), 7th (n 135), 30th (n 85) and 90th (n 48) day after birth. The SA profiles of human milk, including their distribution, were analysed and compared with twenty-four different infant formulas. Outcome of this observational study was the result of natural exposure. Only SA of type Neu5Ac was detected in human milk. Total SA concentrations were highest in colostrum and reduced significantly over the next 3 months. Approximately 68·7­76·1 % of all SA in human milk were bound to oligosaccharides. Two types of SA, Neu5Ac and Neu5Gc, have been detected in infant formulas. Most SA was present in infant formulas combined with protein. Breastfed infants could receive more SA than formula-fed infants with the same energy intake. Overall, human milk is a preferable source of SA than infant formulas in terms of total SA content, dynamics, distribution and type. These SA profiles in the natural state are worth to be considered by the production of formulas because they may have a great effect on infant nutrition and development.

Revealing the Effect of the [CoO]6 Microstructure in Pseudocapacitance by Controlled Delithium of LiCoO2.

Revealing the in-depth structure-property relationship and designing specific capacity electrodes are particularly important for supercapacitors. Despite many efforts made to tune the composition and electronic structure of cobalt oxide for pseudocapacitance, insight into the [CoO]6 octahedron from the microstructure is still insufficient. Herein, we present a tunable [CoO]6 octahedron microstructure in LiCoO2 by a chemical delithiation process. The c-strained strain of the [CoO]6 octahedron is induced to form higher valence Co ions, and the (003) crystalline layer spacing increases to allow more rapid participation of OH- in the redox reaction. Interestingly, the specific capacity of L0.75CO2 is nearly four times higher than that of LiCoO2 at 10 mA g-1. The enhanced activity originated from the asymmetric strain [CoO]6 octahedra, resulting in enhanced electronic conductivity and Co-O hybridization for accelerated redox kinetics. This finding provides new insights into the modification strategy for pseudocapacitive transition metal oxides.

On the magnetization of the 120° order of the spin-1/2 triangular lattice Heisenberg model: a DMRG revisited.

We revisit the issue about the magnetization of the 120° order in the spin-1/2 triangular lattice Heisenberg model with density matrix renormalization group (DMRG). The accurate determination of the magnetization of this model is challenging for numerical methods and its value exhibits substantial disparities across various methods. We perform a large-scale DMRG calculation of this model by employing bond dimension as large asD=24000and by studying the system with width as large asLy=12. With careful extrapolation with truncation error and suitable finite size scaling, we give a conservative estimation of the magnetization asM0=0.208(8). The ground state energy per site we obtain isEg=-0.5503(8). Our results provide valuable benchmark values for the development of new methods in the future.

An Ultrahigh Modulus Gel Electrolytes Reforming the Growing Pattern of Li Dendrites for Interfacially Stable Lithium-Metal Batteries.

Gel polymer electrolytes (GPEs) have aroused intensive attention for their moderate comprehensive performances in lithium-metal batteries (LMBs). However, GPEs with low elastic moduli of MPa magnitude cannot mechanically regulate the Li deposition, leading to recalcitrant lithium dendrites. Herein, a porous Li7 La3 Zr2 O12 (LLZO) framework (PLF) is employed as an integrated solid filler to address the intrinsic drawback of GPEs. With the incorporation of PLF, the composite GPE exhibits an ultrahigh elastic modulus of GPa magnitude, confronting Li dendrites at a mechanical level and realizing steady polarization at high current densities in Li||Li cells. Benefiting from the compatible interface with anodes, the LFP|PLF@GPE|Li cells deliver excellent rate capability and cycling performance at room temperature. Theoretical models extracted from the topology of solid fillers reveal that the PLF with unique 3D structures can effectively reinforce the gel phase of GPEs at the nanoscale via providing sufficient mechanical support from the load-sensitive direction. Numerical models are further developed to reproduce the multiphysical procedure of dendrite propagation and give insights into predicting the failure modes of LMBs. This work quantitatively clarifies the relationship between the topology of solid fillers and the interface stability of GPEs, providing guidelines for designing mechanically reliable GPEs for LMBs.

Prognostic Significance of Blood Pressure at Rest and After Performing the Six-Minute Walk Test in Patients With Acute Heart Failure.

BACKGROUND: It remains unclear whether systolic (SBP) and diastolic (DBP) pressure and BP response after six-minute walk test (6MWT) are associated with adverse outcomes in patients with acute heart failure (AHF). METHODS: We investigated these associations in 98 AHF patients (24.5% women; mean age, 70.5 years) enrolled in the ROSE trial (The Low-dose Dopamine or Low-dose Nesiritide in Acute Heart Failure with Renal Dysfunction). The primary endpoint consisted of any death or rehospitalization within 6 months after randomization. We computed hazard ratios (HRs) of the risks associated with 1-SD increase in post-exercise BP levels and BP ratios, calculated as BP immediately after 6MWT divided by BP before 6MWT. RESULTS: The BP before and after 6MWT averaged 110.6/117.5 mm Hg for SBP and 61.9/64.7 mm Hg for DBP. In multivariable-adjusted analyses including clinic BP measured at the same day of 6MWT, higher DBP after 6MWT was associated with lower risk of the primary endpoint (HR, 0.49; 95% confidence interval [CI], 0.26-0.95; P = 0.034). Both higher SBP and DBP immediately after 6MWT were associated with lower risk of 6-month mortality (HRs, 0.39/0.16; 95% CI, 0.17-0.90/0.065-0.40; P ≤ 0.026). The post-exercise SBP ratio was associated with the risk of 6-month mortality in multivariable-adjusted analyses (HR, 0.44; P = 0.023). CONCLUSIONS: Higher BP levels and BP ratios immediately after 6MWT conferred lower risk of adverse health outcomes. Our observations highlight that 6MWT-related BP level and response may refine risk estimates in patients hospitalized AHF and may help further investigation for the development of HF preventive strategies.

Greenhouse gas emission inventory of drinking water treatment plants and case studies in China.

The Chinese government claimed to reach carbon dioxide emissions peaking by 2030 and achieve carbon neutralization by 2060. In this context, it's meaningful and urgent to estimate GHG emissions amount in every sectors. The growing concern about reducing GHG emissions has been shared by many water companies. This work aims to identify and estimate GHG emissions from the activities of drinking water treatment plants (DWTPs). According to the GHG protocol, the GHG emission inventory of DWTPs covers the sources of fossil fuel combustion, reservoir emissions, electricity and heat supply, use of chemicals and additives, disposal of waste, transportation, operation and maintenance. The tool was tested by nine DWTPs, which had an average GHG emission intensity of 0.225 kg CO2-eq/m3. The GHG emission intensities range from 0.167 kg CO2-eq/m3 to 0.272 kg CO2-eq/m3. The main source of GHG emissions is electricity supply, followed by the use of chemicals and additives. According to the average emission intensity, the estimated total amount of GHG emissions from DWTPs in China is about 1.82 × 107 t/a, corresponding to 0.15 % of the total GHG emission in China. The proposed GHG sources and emissions help decision-makers and DWTPs companies estimate GHG emissions more accurately and undertake GHG reduction measures.

An improved model for target detection and pose estimation of a teleoperation power manipulator.

Introduction: A hot cell is generally deployed with a teleoperation power manipulator to complete tests, operations, and maintenance. The position and pose of the manipulator are mostly acquired through radiation-resistant video cameras arranged in the hot cell. In this paper, deep learning-based target detection technology is used to establish an experimental platform to test the methods for target detection and pose estimation of teleoperation power manipulators using two cameras. Methods: In view of the fact that a complex environment affects the precision of manipulator pose estimation, the dilated-fully convolutional one-stage object detection (dilated-FCOS) teleoperation power manipulator target detection algorithm is proposed based on the scale of the teleoperation power manipulator. Model pruning is used to improve the real-time performance of the dilated-FCOS teleoperation power manipulator target detection model. To improve the detection speed for the key points of the teleoperation power manipulator, the keypoint detection precision and model inference speed of different lightweight backbone networks were tested based on the SimpleBaseline algorithm. MobileNetv1 was selected as the backbone network to perform channel compression and pose distillation on the upsampling module so as to further optimize the inference speed of the model. Results and discussion: Compared with the original model, the proposed model was experimentally proven to reach basically the same precision within a shorter inference time (only 58% of that of the original model). The experimental results show that the compressed model basically retains the precision of the original model and that its inference time is 48% of that of the original model.

Polymer Chainmail: Steric Hindrance and Charge Compensation of Anion-Doped PEDOT to Boost Stress Deformation of Compressible Supercapacitor.

Conducting polymers with high theoretical capacitance and deformability are among the optimal candidates for compressible supercapacitor electrode materials. However, achieving both mechanical and electrochemical stabilities in a single electrode remains a great challenge. To address this issue, the "Polymer Chainmail" is proposed with reversible deformation capability and enhances stability because of the steric hindrance and charge compensation effect of doped anions. As a proof of concept, four common anions are selected as dopants for Poly(3,4-ethylenedioxythiophene) (PEDOT), and their effects on the adsorption and diffusion of H+ on PEDOT are verified using density functional theory calculations. Owing to the film formation effect, the PF 6 - ${{\rm{PF}}_6^- }$ doped PEDOT/nitrogen-doped carbon foam exhibits good mechanical properties. Furthermore, the composite demonstrates excellent rate performance and stability due to suitable anion doping. This finding provides new insights into the preparation of electrochemically stable conductive polymer-based compressible electrode materials.

Associations of long-term mortality with serum uric acid at admission in acute decompensated heart failure with different phenotypes.

BACKGROUND AND AIMS: It remains unclear whether the long-term prognostic value of serum uric acid (SUA) at admission differs in acute decompensated heart failure (HF) patients across the spectrum of left ventricular ejection fraction (EF). METHODS AND RESULTS: In 2375 patients (38.9% women; mean age, 68.8 years), we assessed the risk of long-term (>1 year) all-cause mortality associated with per 1-SD increase in SUA at admission, using multivariable Cox regression in HF with preserved (HFpEF), mildly reduced (HFmrEF) and reduced (HFrEF) EF. During a median follow-up of 4.1 years, the long-term mortality rate was 39.9%. In all patients, the multivariable-adjusted hazard ratio (HR) expressing the risk of long-term mortality associated with SUA was 1.18 (95% CI, 1.11-1.26; P < 0.001). Compared with the low tertile of the SUA distribution, the sex- and age-adjusted cumulative incidence of long-term mortality was higher in the top tertile. In patients with HFpEF and HFrEF, SUA predicted the risk of long-term mortality with HRs amounting to 1.12 (95% CI, 1.02-1.21; P = 0.012) and 1.28 (95% CI, 1.12-1.47; P < 0.001), respectively. However, there were no associations between the risk of mortality and SUA in HFmrEF. Furthermore, age, sex, NYHA class, and the prevalence of coronary heart disease interacted significantly with SUA for predicting long-term mortality. CONCLUSION: Higher levels of SUA at admission were associated with higher risk of long-term mortality in patients with different HF subtypes. The risk conferred by SUA was age and sex dependent. Our observations highlight that measuring SUA at admission may help to improve risk stratification.

Performance evaluation of a liquid-sodium thermoacoustic engine with magnetohydrodynamic electricity generation based upon the Swift model.

Liquid sodium is an attractive working fluid for thermoacoustic conversion. Herein, a numerical study on a standing-wave thermoacoustic electricity generation system with liquid sodium as the working fluid is presented, based upon the Swift model. The characteristics of the thermoacoustic conversion and the output performance of the system have been investigated. The results show that the sodium engine can reach a power density much higher than the classical gas engine. Due to the strong acoustic coupling between components, the electricity output is significantly affected by the input heating power, the magnetic flux density, and the load ratio. In a typical case, the thermal-to-electric efficiency and the relative Carnot efficiency can reach 4.6% and 7.8%, respectively, with a temperature difference of 563 K and an input heat of 5 kW. More importantly, the output electricity density reaches 150 kW/m3, higher than some commercially available technologies. These results demonstrate the potential of such technology for small-scale electricity generation. Its extremely simple structure without any mechanical moving part endows the system with high reliability and long lifetime, if risks of corrosion and exposure to air and water can be avoided.

The relationship between vitamin K and metabolic dysfunction-associated fatty liver disease among the United States population: National Health and Nutrition Examination Survey 2017-2018.

Background: The effect of vitamin K is associated with several pathological processes in fatty liver. However, the association between vitamin K levels and metabolic dysfunction-associated fatty liver disease (MAFLD) remains unclear. Objective: Here, we investigated the relationship between vitamin K intake and MAFLD risk by employing the American National Health and Nutrition Examination Surveys (NHANES) including 3,571 participants. Methods: MAFLD was defined as hepatic steatosis with one or more of the following: overweight or obesity, type 2 diabetes, or >2 other metabolic risk abnormalities. The total vitamin K was the sum of dietary and supplement dietary intake. The relationship of between log10(vitamin K) and MAFLD was investigated using survey-weighted logistic regression and stratified analysis, with or without dietary supplementation. Results: The MAFLD population had a lower vitamin K intake than the non-MAFLD population (p = 0.024). Vitamin K levels were inversely associated with MAFLD in the fully adjusted model (OR = 0.488, 95% CI: 0.302-0.787, p = 0.006). Consistent results were seen in the group without dietary supplements (OR = 0.373, 95% CI: 0.186-0.751, p = 0.009) but not in the group consuming dietary supplements (OR = 0.489, 95% CI: 0.238-1.001, p = 0.050). Conclusion: Vitamin K intake may be a protective factor for MAFLD, especially for individual not using dietary supplements. Nevertheless, more high-quality prospective studies are needed to clarify the causal relationship between them.

An injectable and active hydrogel induces mutually enhanced mild magnetic hyperthermia and ferroptosis.

Magnetic hyperthermia therapy (MHT) is a promising new modality to deal with solid tumors, yet the low magnetic-heat conversion efficacy, magnetic resonance imaging (MRI) artifacts, easy leakage of magnetic nanoparticles, and thermal resistance are the main obstacles to expand its clinical applications. Herein, a synergistic strategy based on a novel injectable magnetic and ferroptotic hydrogel is proposed to overcome these bottlenecks and boost the antitumor efficacy of MHT. The injectable hydrogel (AAGel) exhibiting a sol-gel transition upon heating is made of arachidonic acid (AA)-modified amphiphilic copolymers. Ferrimagnetic Zn0.4Fe2.6O4 nanocubes with high-efficiency hysteresis loss mechanism are synthesized and co-loaded into AAGel with RSL3, a potent ferroptotic inducer. This system maintains the temperature-responsive sol-gel transition, and provides the capacity of multiple MHT and achieves accurate heating after a single injection owing to the firm anchoring and uniform dispersion of nanocubes in the gel matrix. The high magnetic-heat conversion efficacy of nanocubes coupled with the application of echo limiting effect avoids the MRI artifacts during MHT. Besides the function of magnetic heating, Zn0.4Fe2.6O4 nanocubes combined with multiple MHT can sustain supply of redox-active iron to generate reactive oxygen species and lipid peroxides and accelerate the release of RLS3 from AAGel, thus enhancing the antitumor efficacy of ferroptosis. In turn, the reinforced ferroptosis can alleviate the MHT-triggered thermal resistance of tumors by impairment of the protective heat shock protein 70. The synergy strategy achieves the complete elimination of CT-26 tumors in mice without causing local tumor recurrence and other severe side effects.

Crushing analysis of hierarchical multicellular tubes with gradient character along axial and radial directions under oblique loads.

To overcome the disadvantage of high initial peak crush force (IPCF) in hierarchical and gradient structures, the hierarchical multicellular tubes (HMTs) with gradient character along axial and radial directions are proposed based on the bidirectional structural characters of bamboo stem. Crashworthiness performances of HMTs under oblique loads are systematically studied by using numerical simulation. Results show that compared with the square tube with the same mass, HMTs have higher energy absorption capability under different impact angles. The maximum increases of specific energy absorption (SEA) and crush force efficiency (CFE) reach up to 67.02% and 806%, respectively. Whereas, the maximum decrease of IPCF reaches up to 79.92%. Effects of structural parameters, including hierarchical level, wall thickness and internode space, on the crashworthiness performances of HMTs are also fully investigated.

Semi-hydrogenation of α,ß-unsaturated aldehydes over sandwich-structured nanocatalysts prepared by phase transformation of thin-film Al2O3 to Al-TCPP.

The semi-hydrogenation of α,ß-unsaturated aldehydes to the desired unsaturated alcohols with both high conversion and high selectivity remains a big challenge. Herein, we designed a sandwich-structured nanocatalyst for the highly selective hydrogenation of various α,ß-unsaturated aldehydes (e.g., cinnamaldehyde, furfural, crotonaldehyde, and 3-methyl-2-butenal) to the targeted unsaturated alcohols. Highly accessible platinum nanoparticles were sandwiched between a metal-organic framework (MOF) core (i.e., MIL-88B(Fe)) and a MOF shell (i.e., Al-TCPP). In particular, the growth of the Al-TCPP shell was achieved by atomic layer deposition (ALD) of thin-film Al2O3 followed by phase transformation with a tetrakis(4-carboxyphenyl)porphyrin (H4TCPP) linker. The thickness of the Al-TCPP shell can be finely controlled by adjusting the cycle number of alumina ALD and the concentration of the H4TCPP linker during the phase transformation of Al2O3 to Al-TCPP. It was proven that the permeable MOF shells could serve as selectivity regulators for the activation of the CO bonds in α,ß-unsaturated aldehydes (in preference to the CC bonds), leading to higher selectivity towards unsaturated alcohols as compared to the conventional surface supported Pt catalysts. Mechanistic insights showed that the enhanced catalytic performance was attributed to (i) the modified electronic state of sandwiched Pt nanoparticles by the two MOF layers and (ii) the steric hindrance effect on substrate diffusion through the sandwich-structured catalysts.

RGD Nanoarrays with Nanospacing Gradient Selectively Induce Orientation and Directed Migration of Endothelial and Smooth Muscle Cells.

Directed migration of cells through cell-surface interactions is a paramount prerequisite in biomaterial-induced tissue regeneration. However, whether and how the nanoscale spatial gradient of adhesion molecules on a material surface can induce directed migration of cells is not sufficiently known. Herein, we employed block copolymer micelle nanolithography to prepare gold nanoarrays with a nanospacing gradient, which were prepared by continuously changing the dipping velocity. Then, a self-assembly monolayer technique was applied to graft arginine-glycine-aspartate (RGD) peptides on the nanodots and poly(ethylene glycol) (PEG) on the glass background. Since RGD can trigger specific cell adhesion via conjugating with integrin (its receptor in the cell membrane) and PEG can resist protein adsorption and nonspecific cell adhesion, a nanopattern with cell-adhesion contrast and a gradient of RGD nanospacing was eventually prepared. In vitro cell behaviors were examined using endothelial cells (ECs) and smooth muscle cells (SMCs) as a demonstration. We found that SMCs exhibited significant orientation and directed migration along the nanospacing gradient, while ECs exhibited only a weak spontaneously anisotropic migration. The gradient response was also dependent upon the RGD nanospacing ranges, namely, the start and end nanospacings under a given distance and gradient. The different responses of these two cell types to the RGD nanospacing gradient provide new insights for designing cell-selective nanomaterials potentially used in cell screening, wound healing, etc.

Concentration and distribution of sialic acid in human milk and its correlation with dietary intake.

Purpose: This study evaluates the content, distribution, and changing trend of sialic acid in human milk and the correlation between dietary intake of sialic acid and that in human milk. Methods: The study included 33 mothers of full-term and exclusively breastfed infants. At least 2 ml of milk was collected on the 3rd, 8th, 30th, and 90th day after delivery, and 24-h diet recalls of the lactating mothers were obtained each time. The correlation of human milk sialic acid concentration with lactating women's dietary sialic acid intake during lactation was analyzed by statistical analysis software SPSS. Results: The average concentration of sialic acid in colostrum, transition, and 1 and 3 months were 1,670.74 ± 94.53, 1,272.19 ± 128.74, 541.64 ± 55.2, and 297.65 ± 20.78 mg/L, respectively. The total sialic acid concentration in colostrum was about 5.6 times higher than that at 3 months (P < 0.001). The average dietary sialic acid intake of lactating mothers on the 2nd, 7th, 30th, and 90th day after delivery were 106.06 ± 7.51, 127.64 ± 8.61, 120.34 ± 10.21, and 95.40 ± 6.34 mg/day, respectively. The intake of sialic acid was relatively high on the 7th day, and there was no significant difference in dietary intake of sialic acid on different days (P < 0.05). In addition, there was no correlation between the intake of dietary sialic acid and the content of total sialic acid and various forms of sialic acid in milk (P < 0.05). Conclusion: During the lactation period, the distribution of sialic acid in breast milk is relatively stable and its content fluctuates greatly, which may not be affected by the mother's diet, but mainly depends on the self-regulation oft physiological needs.

The Transitional Wettability on Bamboo-Leaf-like Hierarchical-Structured Si Surface Fabricated by Microgrinding.

Stabilizing the hydrophobic wetting state on a surface is essential in heat transfer and microfluidics. However, most hydrophobic surfaces of Si are primarily achieved through microtexturing with subsequent coating or modification of low surface energy materials. The coatings make the hydrophobic surface unstable and impractical in many industrial applications. In this work, the Si chips' wettability transitions are yielded from the original hydrophilic state to a stable transitional hydrophobic state by texturing bamboo-leaf-like hierarchical structures (BLHSs) through a diamond grinding wheel with one-step forming. Experiments showed that the contact angles (CAs) on the BLHS surfaces increased to 97° and only reduced by 2% after droplet impacts. This is unmatched by the current texturing surface without modification. Moreover, the droplets can be split up and transferred by the BLHS surfaces with their 100% mass. When the BLHS surfaces are modified by the low surface energy materials' coating, the hydrophobic BLHS surfaces are upgraded to be superhydrophobic (CA > 135°). More interestingly, the droplet can be completely self-sucked into a hollow micro-tube within 0.1 s without applying external forces. A new wetting model for BLHS surfaces based on the fractal theory is determined by comparing simulated values with the measured static contact angle of the droplets. The successful preparation of the bamboo-leaf-like Si confirmed that transitional wettability surfaces could be achieved by the micromachining of grinding on the hard and brittle materials. Additionally, this may expand the application potential of the key semiconductor material of Si.

Microorganism-Templated Nanoarchitectonics of Hollow TiO2-SiO2 Microspheres with Enhanced Photocatalytic Activity for Degradation of Methyl Orange.

In this study, hollow SiO2 microspheres were synthesized by the hydrolysis of tetraethyl orthosilicate (TEOS) according to the Stober process, in which Pichia pastoris GS 115 cells were served as biological templates. The influence of the preprocessing method, the TEOS concentration, the ratio of water to ethanol, and the aging time on the morphology of microspheres was investigated and the optimal conditions were identified. Based on this, TiO2-SiO2 microspheres were prepared by the hydrothermal process. The structures and physicochemical properties of TiO2-SiO2 photocatalysts were systematically characterized and discussed. The photocatalytic activity for the degradation of methyl orange (MO) at room temperature under Xe arc lamp acting as simulated sunlight was explored. The result showed that the as-prepared TiO2-SiO2 microspheres exhibited a good photocatalytic performance.