Objective:Placement of human placenta derived grafts during robotic-assisted radical prostatectomy(RARP)hastens the return of continence and potency.The long-term impact on the oncologic outcomes remains to be investi...Objective:Placement of human placenta derived grafts during robotic-assisted radical prostatectomy(RARP)hastens the return of continence and potency.The long-term impact on the oncologic outcomes remains to be investigated.Our objective was to determine the oncologic outcomes of patients with dehydrated human amnion chorion membrane(dHACM)at RARP compared to a matched cohort.Methods:In a referral centre,from August 2013 to October 2019,599 patients used dHACM in bilateral nerve-sparing RARP.We excluded patients with less than 12 months follow-up,simple prostatectomy,and unilateral nerve-sparing.Patients with dHACM(amnio group)were 529,and were propensity score matched 1:1 to 2465 patients without dHACM(non-amnio group)and a minimum follow-up of 36 months.At the time of RARP,dHACM was placed around the neurovascular bundle in the amnio group.Continuous and categorical variables in matched groups was tested by two-sample Kolmogorov-Smirnov test and Fisher's exact test respectively.Outcomes measured were biochemical recurrence(BCR),adjuvant and salvage therapy rates.Results:Propensity score matching resulted in two groups of 444 patients.Cumulative incidence functions for BCR did not show a difference between the groups(p=0.3).Patients in the non-amnio group required salvage therapy more frequently than the amnio group,particularly after partial nerve-sparing RARP(6.3%vs.2.3%,p=0.001).Limitations are the absence of prospective randomization.Conclusion:The data suggest that using dHACM does not have a negative impact on BCR in patients.Outcomes of cancer specific and overall survival will require follow-up study to increase our understanding of these grafts’impact on prostate cancer biology.展开更多
Chile,a pioneer and benchmark partner for China's free trade.cooperation in Latin America,holds a special position in China-Latin America economic and trade relations.It was the first Latin American country to sig...Chile,a pioneer and benchmark partner for China's free trade.cooperation in Latin America,holds a special position in China-Latin America economic and trade relations.It was the first Latin American country to sign a bilateral free trade agreement with China and the first to reach an upgraded protocol.Chile also established mutual recognition of Authorized Economic Operators(AEO)with China,the first country in South America to do so.展开更多
BACKGROUND The risk factors and prediction models for diabetic foot(DF)remain incompletely understood,with several potential factors still requiring in-depth investigations.AIM To identify risk factors for new-onset D...BACKGROUND The risk factors and prediction models for diabetic foot(DF)remain incompletely understood,with several potential factors still requiring in-depth investigations.AIM To identify risk factors for new-onset DF and develop a robust prediction model for hospitalized patients with type 2 diabetes.METHODS We included 6301 hospitalized patients with type 2 diabetes from January 2016 to December 2021.A univariate Cox model and least absolute shrinkage and selection operator analyses were applied to select the appropriate predictors.Nonlinear associations between continuous variables and the risk of DF were explored using restricted cubic spline functions.The Cox model was further employed to evaluate the impact of risk factors on DF.The area under the curve(AUC)was measured to evaluate the accuracy of the prediction model.RESULTS Seventy-five diabetic inpatients experienced DF.The incidence density of DF was 4.5/1000 person-years.A long duration of diabetes,lower extremity arterial disease,lower serum albumin,fasting plasma glucose(FPG),and diabetic nephropathy were independently associated with DF.Among these risk factors,the serum albumin concentration was inversely associated with DF,with a hazard ratio(HR)and 95%confidence interval(CI)of 0.91(0.88-0.95)(P<0.001).Additionally,a U-shaped nonlinear relationship was observed between the FPG level and DF.After adjusting for other variables,the HRs and 95%CI for FPG<4.4 mmol/L and≥7.0 mmol/L were 3.99(1.55-10.25)(P=0.004)and 3.12(1.66-5.87)(P<0.001),respectively,which was greater than the mid-range level(4.4-6.9 mmol/L).The AUC for predicting DF over 3 years was 0.797.CONCLUSION FPG demonstrated a U-shaped relationship with DF.Serum albumin levels were negatively associated with DF.The prediction nomogram model of DF showed good discrimination ability using diabetes duration,lower extremity arterial disease,serum albumin,FPG,and diabetic nephropathy(Clinicaltrial.gov NCT05519163).展开更多
Approximately 350 million people are estimated to be persistently infected with hepatitis B virus(HBV) worldwide. HBV maintains persistent infection by employing covalently closed circular DNA(ccc DNA), a template for...Approximately 350 million people are estimated to be persistently infected with hepatitis B virus(HBV) worldwide. HBV maintains persistent infection by employing covalently closed circular DNA(ccc DNA), a template for all HBV RNAs. Chronic hepatitis B(CHB) patients are currently treated with nucleos(t)ide analogs such as lamivudine, adefovir, entecavir, and tenofovir. However, these treatments rarely cure CHB because they are unable to inhibit ccc DNA transcription and inhibit only a late stage in the HBV life cycle(the reverse transcription step in the nucleocapsid). Therefore, an understanding of the factors regulating ccc DNA transcription is required to stop this process. Among numerous factors, hepatocyte nuclear factors(HNFs) play the most important roles in ccc DNA transcription, especially in the generation of viral genomic RNA, a template for HBV replication. Therefore, proper control of HNF function could lead to the inhibition of HBV replication. In this review, we summarize and discuss the current understanding of the roles of HNFs in the HBV life cycle and the upstream factors that regulate HNFs. This knowledge will enable the identification of new therapeutic targets to cure CHB.展开更多
Drought has become a problem that is universally faced by global terrestrial ecosystems. Northeast China is located in a region sensitive to global climate changes, and one of the main impacts of climate changes in No...Drought has become a problem that is universally faced by global terrestrial ecosystems. Northeast China is located in a region sensitive to global climate changes, and one of the main impacts of climate changes in Northeast China is manifested as drought in growing seasons. This study analyzes the spatio-temporal evolution law of the water use efficiency(WUE) of the main natural vegetation(i.e., cold-temperate coniferous forests, temperate pine-broad-leaved mixed forests, warm-temperate deciduous broad-leaved forests, and grasslands) in Northeast China based on public MODIS data products, including MCD12 Q1, MOD15 A2 H, MOD16 A2, and MOD17 A3 H, and meteorological data from 2002 to 2013. The influence of drought events on the WUE of different vegetation types and their response to drought events are also investigated. The study findings are as follows:(1) drought in Northeast China frequently occurs in the regions stretching from 114.55°E to 120.90°E, and the percentage of drought area among the forests is lower than that among the grasslands during these years;(2) the annual average WUE of the natural vegetation ranges from 0.82 to 1.08 C/kg^(-1) H_2O, and the WUE of forests(0.82 to 1.08 C/kg^(-1) H_2O) is universally higher than that of grasslands(0.84 to 0.99 C/kg^(-1) H_2O);(3) in 2008, the regions where the WUE in drought conditions is higher than that in normal water conditions account for 86.11% of the study area, and a significant linear positive correlation is found between the WUE in drought conditions and the WUE in normal water conditions, whereas the degree of drought does not influence the WUE of the natural vegetation in an obviously linear manner; and(4) the WUE for the cold-temperate coniferous forests and temperate pine-broad-leaved mixed forests with a high ET or low NPP is more likely to rise in drought conditions; the WUE for the grasslands with a low Evapotranspiration(ET), Net Primary Production(NPP), and Leaf Area Index(LAI) is more likely to rise in drought conditions; and the ET, NPP, and LAI have no significant influence on the WUE for the warm-temperate deciduous broad-leaved forests in drought conditions. This study contributes to improving the evaluation of the influence of drought on natural ecosystems.展开更多
Electrocatalytic oxygen reduction reaction (ORR) via two-electron pathway is a promising approach to decentralized and on-site hydrogen peroxide (H_(2)O_(2)) production beyond the traditional anthraquinone process.In ...Electrocatalytic oxygen reduction reaction (ORR) via two-electron pathway is a promising approach to decentralized and on-site hydrogen peroxide (H_(2)O_(2)) production beyond the traditional anthraquinone process.In recent years,electrochemical H_(2)O_(2) production in acidic media has attracted increasing attention owing to its stronger oxidizing capacity,superior stability,and higher compatibility with various applications.Here,recent advances of H_(2)O_(2) electrosynthesis in acidic media are summarized.Specifically,fundamental aspects of two-electron ORR mechanism are firstly presented with an emphasis on the pH effect on catalytic performance.Major categories of promising electrocatalysts are then reviewed,including noble-metal-based materials,non-noble-metal single-atom catalysts,non-noblemetal compounds,and metal-free carbon-based materials.The innovative development of electrochemical devices and in situ/on-site application of electrogenerated H_(2)O_(2) are also highlighted to bridge the gap between laboratory-scale fundamental research and practically relevant H_(2)O_(2) electrosynthesis.Finally,critical perspectives on present challenges and promising opportunities for future research are provided.展开更多
The demand for efficient and environmentally-benign electrocatalysts that help availably harness the renewable energy resources is growing rapidly. In recent years, increasing insights into the design of water electro...The demand for efficient and environmentally-benign electrocatalysts that help availably harness the renewable energy resources is growing rapidly. In recent years, increasing insights into the design of water electrolysers, fuel cells, and metal–air batteries emerge in response to the need for developing sustainable energy carriers, in which the oxygen evolution reaction and the oxygen reduction reaction play key roles. However, both reactions suffer from sluggish kinetics that restricts the reactivity. Therefore, it is vital to probe into the structure of the catalysts to exploit high-performance bifunctional oxygen electrocatalysts. Spinel-type catalysts are a class of materials with advantages of versatility, low toxicity, low expense, high abundance, flexible ion arrangement, and multivalence structure. In this review, we afford a basic overview of spinel-type materials and then introduce the relevant theoretical principles for electrocatalytic activity, following that we shed light on the structure–property relationship strategies for spinel-type catalysts including electronic structure, microstructure, phase and composition regulation,and coupling with electrically conductive supports. We elaborate the relationship between structure and property, in order to provide some insights into the design of spinel-type bifunctional oxygen electrocatalysts.展开更多
To satisfy the rapid development of gas-involving electrocatalysis(O2, CO2, N2, etc.), nanostructured electrocatalysts with favorably regulated electronic structure and surface nanostructures are urgently required. He...To satisfy the rapid development of gas-involving electrocatalysis(O2, CO2, N2, etc.), nanostructured electrocatalysts with favorably regulated electronic structure and surface nanostructures are urgently required. Herein, we highlighted a core-branch hydroxysulfide as a significantly enhanced oxygen evolution reaction electrocatalyst. This hydroxysulfide was facilely fabricated via a versatile interfacial reaction in S2- inorganic solution at room temperature for a designed period. The moderative growth kinetics contributed to the growth of interconnected hydroxysulfide nanosheets with high-sulfur contents on the hydroxide precursor substrates, resulting in a hierarchical nanostructure with multifunctional modifications, including regulated electronic structure, rapid electron highway, excellent accessibility, and facilitated mass transfer. Such synthetic methodology can be generalized and facilely governed by regulating the temperature, concentration, duration, and solvent for targeted nanostructures. Contributed to the favorably regulated electronic structure and surface nanostructure, the as-obtained core-branch Co2NiS2.4(OH)1.2 sample exhibits superior OER performance, with a remarkably low overpotential(279 m V required for 10.0 m A c^m-2), a low Tafel slope(52 m V dec^-1), and a favorable long-term stability. This work not only presents a promising nanostructured hydroxysulfide for excellent OER electrocatalysis, but also shed fresh lights on the further rational development of efficient electrocatalysts.展开更多
The solubility data of compounds in supercritical fluids and the correlation between the experimental solubility data and predicted solubility data are crucial to the development of supercritical technologies. In the ...The solubility data of compounds in supercritical fluids and the correlation between the experimental solubility data and predicted solubility data are crucial to the development of supercritical technologies. In the present work, the solubility data of silymarin(SM) in both pure supercritical carbon dioxide(SCCO2) and SCCO2 with added cosolvent was measured at temperatures ranging from 308 to 338 K and pressures from 8 to 22 MPa. The experimental data were fit with three semi-empirical density-based models(Chrastil, Bartle and Mendez-Santiago and Teja models) and a back-propagation artificial neural networks(BPANN) model. Interaction parameters for the models were obtained and the percentage of average absolute relative deviation(AARD%) in each calculation was determined. The correlation results were in good agreement with the experimental data. A comparison among the four models revealed that the experimental solubility data were more fit with the BPANN model with AARDs ranging from 1.14% to 2.15% for silymarin in pure SCCO2 and with added cosolvent. The results provide fundamental data for designing the extraction of SM or the preparation of its particle using SCCO2 techniques.展开更多
Nowadays,Cu-based materials have attracted extensive attention as electrocatalysts,while the inherent reason of the filling of high anti-bonding state of Cu d band(3 d^(10)4 s^(1))makes it difficult to hybridize with ...Nowadays,Cu-based materials have attracted extensive attention as electrocatalysts,while the inherent reason of the filling of high anti-bonding state of Cu d band(3 d^(10)4 s^(1))makes it difficult to hybridize with O2 p band of oxygen intermediates during the adsorption process of oxygen evolution reaction(OER).To increase the efficiency of Cu-based electrocatalysts,efforts have been made to optimize the electronic structures and to create surface defects and hierarchical nanostructures with more exposed accessible active sites.Herein,we report a facile method for preparing CuO electrocatalysts with hierarchical nanostructures using the Cu-alanine complex as a precursor through room-temperature chemical precipitation and subsequent calcination in air.Investigations of products obtained at different calcination temperatures reveal the relationship between OER activities and the material characteristics such as specific surface areas,crystal growth orientations,and element components.The product obtained at 500℃exhibits the smallest overpotential of 290 mV in 1.0 mol/L KOH for electrocatalyzing OER.Combining with various characterizations of CuO electrocatalysts after OER activities,the possible catalytic mechanism and the influence factors of their OER performance are also discussed.展开更多
Recent studies have shown that mutation at Ser522 causes inhibition of collapsin response mediator protein 2(CRMP2) phosphorylation and induces axon elongation and partial recovery of the lost sensorimotor function af...Recent studies have shown that mutation at Ser522 causes inhibition of collapsin response mediator protein 2(CRMP2) phosphorylation and induces axon elongation and partial recovery of the lost sensorimotor function after spinal cord injury(SCI).We aimed to reveal the intracellular mechanism in axotomized neurons in the CRMP2 knock-in(CRMP2KI) mouse model by performing transcriptome analysis in mouse sensorimotor cortex using micro-dissection punching system.Prior to that, we analyzed the structural pathophysiology in axotomized or neighboring neurons after SCI and found that somatic atrophy and dendritic spine reduction in sensorimotor cortex were suppressed in CRMP2KI mice.Further analysis of the transcriptome has aided in the identification of four hemoglobin genes Hba-a1, Hba-a2, Hbb-bs, and Hbb-bt that are significantly upregulated in wild-type mice with concomitant upregulation of genes involved in the oxidative phosphorylation and ribosomal pathways after SCI.However, we observed substantial upregulation in channel activity genes and downregulation of genes regulating vesicles, synaptic function, glial cell differentiation in CRMP2KI mice.Moreover, the transcriptome profile of CRMP2KI mice has been discussed wherein energy metabolism and neuronal pathways were found to be differentially regulated.Our results showed that CRMP2KI mice displayed improved SCI pathophysiology not only via microtubule stabilization in neurons, but also possibly via the whole metabolic system in the central nervous system, response changes in glial cells, and synapses.Taken together, we reveal new insights on SCI pathophysiology and the regenerative mechanism of central nervous system by the inhibition of CRMP2 phosphorylation at Ser522.All these experiments were performed in accordance with the guidelines of the Institutional Animal Care and Use Committee at Waseda University, Japan(2017-A027 approved on March 21, 2017;2018-A003 approved on March 25, 2018;2019-A026 approved on March 25, 2019).展开更多
BACKGROUND Artificial intelligence in colonoscopy is an emerging field,and its application may help colonoscopists improve inspection quality and reduce the rate of missed polyps and adenomas.Several deep learning-bas...BACKGROUND Artificial intelligence in colonoscopy is an emerging field,and its application may help colonoscopists improve inspection quality and reduce the rate of missed polyps and adenomas.Several deep learning-based computer-assisted detection(CADe)techniques were established from small single-center datasets,and unrepresentative learning materials might confine their application and generalization in wide practice.Although CADes have been reported to identify polyps in colonoscopic images and videos in real time,their diagnostic performance deserves to be further validated in clinical practice.AIM To train and test a CADe based on multicenter high-quality images of polyps and preliminarily validate it in clinical colonoscopies.METHODS With high-quality screening and labeling from 55 qualified colonoscopists,a dataset consisting of over 71000 images from 20 centers was used to train and test a deep learning-based CADe.In addition,the real-time diagnostic performance of CADe was tested frame by frame in 47 unaltered full-ranged videos that contained 86 histologically confirmed polyps.Finally,we conducted a selfcontrolled observational study to validate the diagnostic performance of CADe in real-world colonoscopy with the main outcome measure of polyps per colonoscopy in Changhai Hospital.RESULTS The CADe was able to identify polyps in the test dataset with 95.0%sensitivity and 99.1%specificity.For colonoscopy videos,all 86 polyps were detected with 92.2%sensitivity and 93.6%specificity in frame-by-frame analysis.In the prospective validation,the sensitivity of CAD in identifying polyps was 98.4%(185/188).Folds,reflections of light and fecal fluid were the main causes of false positives in both the test dataset and clinical colonoscopies.Colonoscopists can detect more polyps(0.90 vs 0.82,P<0.001)and adenomas(0.32 vs 0.30,P=0.045)with the aid of CADe,particularly polyps<5 mm and flat polyps(0.65 vs 0.57,P<0.001;0.74 vs 0.67,P=0.001,respectively).However,high efficacy is not realized in colonoscopies with inadequate bowel preparation and withdrawal time(P=0.32;P=0.16,respectively).CONCLUSION CADe is feasible in the clinical setting and might help endoscopists detect more polyps and adenomas,and further confirmation is warranted.展开更多
Secondary metabolites are important for various industrial applications. The production of secondary metabolites is often improved by the activation of substrate supply pathways for biosynthesis. However, many importa...Secondary metabolites are important for various industrial applications. The production of secondary metabolites is often improved by the activation of substrate supply pathways for biosynthesis. However, many important pathways have remained unclear. In this study, we explored possible pathways related to substrate supply for the biosynthesis of the antifungal agent FR901469 which is a nonribosomal peptide and a fungal secondary metabolite. To clarify the unknown activated pathways, we utilized the Comprehensive Pathway Model (CPM) which was developed in our previous study. We verified that the overexpression of the hypothetical beta-alanine-aminotransferase (BAL-AT), which was included in the explored pathways, improved the FR901469 productivity. The genes encoding the BAL metabolic enzymes are considered to be important for improving the FR901469 productivity.展开更多
Age-related mitochondrial dysfunction leads to defects in cellular energy metabolism and oxidative stress defense systems,which can contribute to tissue damage and disease development.Among the key regulators responsi...Age-related mitochondrial dysfunction leads to defects in cellular energy metabolism and oxidative stress defense systems,which can contribute to tissue damage and disease development.Among the key regulators responsible for mitochondrial quality control,peroxisome proliferator-activated receptor gamma coactivator 1-alpha(PGC-1α)is an important target for mitochondrial dysfunction.We have previously reported that bioactive polyphenols extracted from sugarcane top(ST)ethanol extract(STEE)could activate neuronal energy metabolism and increase astrocyte PGC-1αtranscript levels.However,their potential impact on the mitochondria activity in muscle and liver cells has not yet been investigated.To address this gap,our current study examined the effects of STEE and its polyphenols on cultured myotubes and hepatocytes in vitro.Rhodamine 123 assay revealed that the treatment with STEE and its polyphenols resulted in an increase in mitochondrial membrane potential in C2C12 myotubes.Furthermore,a comprehensive examination of gene expression patterns through transcriptome-wide microarray analysis indicated that STEE altered gene expressions related to mitochondrial functions,fatty acid metabolism,inflammatory cytokines,mitogen-activated protein kinase(MAPK)signaling,and cAMP signaling in both C2C12 myotubes and HepG2 hepatocytes.Additionally,protein-protein interaction analysis identified the PGC-1αinteractive-transcription factors-targeted regulatory network of the genes regulated by STEE,and the quantitative polymerase chain reaction results confirmed that STEE and its polyphenols upregulated the transcript levels of PGC-1αin both C2C12 and HepG2 cells.These findings collectively suggest the potential beneficial effects of STEE on muscle and liver tissues and offer novel insights into the potential nutraceutical applications of this material.展开更多
Fluorescence microscopy enables the visualization of cellular morphology,molecular distribution,ion distribution,and their dynamic behaviors during biological processes.Enhancing the signal-to-noise ratio(SNR)in fluor...Fluorescence microscopy enables the visualization of cellular morphology,molecular distribution,ion distribution,and their dynamic behaviors during biological processes.Enhancing the signal-to-noise ratio(SNR)in fluorescence imaging improves the quantification accuracy and spatial resolution;however,achieving high SNR at fast image acquisition rates,which is often required to observe cellular dynamics,still remains a challenge.In this study,we developed a technique to rapidly freeze biological cells in milliseconds during optical microscopy observation.Compared to chemical fixation,rapid freezing provides rapid immobilization of samples while more effectively preserving the morphology and conditions of cells.This technique combines the advantages of both live-cell and cryofixation microscopy,i.e.,temporal dynamics and high SNR snapshots of selected moments,and is demonstrated by fluorescence and Raman microscopy with high spatial resolution and quantification under low temperature conditions.Furthermore,we also demonstrated that intracellular calcium dynamics can be frozen rapidly and visualized using fluorescent ion indicators,suggesting that ion distribution and conformation of the probe molecules can be fixed both spatially and temporally.These results confirmed that our technique can time-deterministically suspend and visualize cellular dynamics while preserving molecular and ionic states,indicating the potential to provide detailed insights into sample dynamics with improved spatial resolution and temporal accuracy in observations.展开更多
Two-dimensional(2D)metal-organic frameworks(MOFs)are promising for electrocatalysis with high performance,as they possess large surface areas and high densities of exposed active sites.It attracts tremendous attention...Two-dimensional(2D)metal-organic frameworks(MOFs)are promising for electrocatalysis with high performance,as they possess large surface areas and high densities of exposed active sites.It attracts tremendous attention to obtain 2D nanostructures via simple preparation methods.Herein,a facile pyridine-modulated solvothermal synthesis of Ni/Co bimetallic MOF nanoplates(NixCoy-bpy(PyM))is reported with well-defined 2D morphology with a thickness as thin as 20 nm and an aspect ratio larger than 50.These nanoplates possess oxygen evolution reaction activity as electrocatalysts in alkaline conditions.Specifically,Ni0.5Co1.5-bpy(PyM)exhibits excellent OER electrocatalytic activity with a low overpotential of 256 mV at 10 m A cm-2 and a small Tafel slope of 81.8 mV dec-1 in 1.0 mol L-1 KOH with long-term electrochemical stability for 3000 cyclic voltammetry cycles.The high catalytic activity of Ni0.5Co1.5-bpy(PyM)can be attributed to the in situ formed active hydroxide and oxyhydroxide species within the inherited 2D morphology and the optimized bimetallic ratio.展开更多
Through partial deligandation of metal-organic frameworks(MOFs),quasi-MOFs with a transition structure between MOFs and metal compounds(such as metal oxides,nitrides,sulfides,and phosphides)can be fabricated.Quasi-MOF...Through partial deligandation of metal-organic frameworks(MOFs),quasi-MOFs with a transition structure between MOFs and metal compounds(such as metal oxides,nitrides,sulfides,and phosphides)can be fabricated.Quasi-MOFs can not only retain the porous structure of MOFs to a certain extent,but also expose the inorganic nodes to the vip species(e.g.,metal nanoparticles)to show enhanced metal-support interaction for synergistic catalysis.This concept was first demonstrated by our group through calcining Au/MIL-101 at different temperatures under Ar flow to adjust the interface between Au nanoparticles and the inorganic Cr–O nodes.The obtained Au/quasi-MIL-101 showed superior enhanced catalytic activity in the oxidation of carbon monoxide.This study has inspired further research interest to fabricate other quasi-MOFs through controlled deligandation of mono-and bimetallic MOFs and their composites for the design of efficient catalysts.展开更多
Carb on nanospheres(XC-72R)were functionalized by boron-oxygen(B-O)through coannealing with boric acid,to which highly dispersed palladium nanoparticles(Pd NPs)(-1.7 nm)were immobilized by a wet chemical reduction for...Carb on nanospheres(XC-72R)were functionalized by boron-oxygen(B-O)through coannealing with boric acid,to which highly dispersed palladium nanoparticles(Pd NPs)(-1.7 nm)were immobilized by a wet chemical reduction for the first time.The resultant Pd/OB-C catalystexhibits significantly improved activity for the dehydrogenation from formic acid(FA)compared to pristine XC-72R supported Pd NPs(Pd/C).Impressively,by adding melamine precursor,the B-0 and nitrogen(N)-functionalized product OB-C-N displays an extremely high B content,ca.34 times higher than OB-C.The Pd/OB-C-N catalyst with an ultrafine Pd particle size of-1.4 nm shows a superb activity,with a turnoverfrequency(TOF)as high as 5,354 h^-1 at 323 K,owing to the uniform ultrafine Pd NPs and the effect from B-0 and N functionalities.展开更多
The hydrogen evolution reaction(HER)as a fundamental process in electrocatalysis plays a significant role in clean energy technologies.For an energy-efficient HER,it demands an effective,durable,and low-cost catalyst ...The hydrogen evolution reaction(HER)as a fundamental process in electrocatalysis plays a significant role in clean energy technologies.For an energy-efficient HER,it demands an effective,durable,and low-cost catalyst to trigger proton reduction with minimal overpotential and fast kinetics.Here,we successfully fabricate a highly efficient HER catalyst of N-C/Co/Mo_(2)C holey nanorods with Co/b-Mo_(2)C nanoparticles uniformly embedded in nitrogen-doped carbon(N-C/Co/Mo_(2)C)by pyrolyzing the molybdate-coordinated zeolitic imidazolate framework(ZIF-67/MoO_(4)^(2-))holey nanorods,which result from the reaction between CoMoO_(4)and Me IM in a methanol/water/triethylamine mixed solution.The uniform distribution of MoO_(4)^(2-)in the ZIF-67/MoO_(4)^(2-)enables Co/β-Mo_(2)C nanoparticles to be welldistributed within nitrogen-doped carbon holey nanorods.This synthetic strategy endows the N-C/Co/Mo_(2)C catalyst with uniformly decorated bimetal,thus attaining excellent HER electrocatalytic activities with a small overpotential of 142.0 m V at 10 m A cm^(-2)and superior stability in 1.0 mol L^(-1)KOH aqueous solution.展开更多
Porous metal phosphide cubes with exposed vertices and edges containing abundant catalytically active sites are promising electrocatalysts.Herein,by integrating the advantages of the phosphorus-rich cobalt phosphides ...Porous metal phosphide cubes with exposed vertices and edges containing abundant catalytically active sites are promising electrocatalysts.Herein,by integrating the advantages of the phosphorus-rich cobalt phosphides and bimetallic oxides to form hybrid architectures,we prepared CoP_(3)/CoSnO_(2)via phosphating CoSn(OH)_(6)nanocubes,which has unique porous nanocubic structure.The optimized CoP_(3)/CoSnO_(2)porous nanaocubes showed excellent electrocatalytic activity for OER/ORR.What’s more,the electrochemical performances of CoP_(3)/CoSnO_(2)porous nanaocubes as air cathode catalyst for zinc air batteries were better than that of commercial RuO_(2)and 20 wt%Pt/C with a mass ratio of 1:1 as the air cathode catalyst.This work offers a new strategy to fabricate metal phosphide with porous nanocubic structures.展开更多
文摘Objective:Placement of human placenta derived grafts during robotic-assisted radical prostatectomy(RARP)hastens the return of continence and potency.The long-term impact on the oncologic outcomes remains to be investigated.Our objective was to determine the oncologic outcomes of patients with dehydrated human amnion chorion membrane(dHACM)at RARP compared to a matched cohort.Methods:In a referral centre,from August 2013 to October 2019,599 patients used dHACM in bilateral nerve-sparing RARP.We excluded patients with less than 12 months follow-up,simple prostatectomy,and unilateral nerve-sparing.Patients with dHACM(amnio group)were 529,and were propensity score matched 1:1 to 2465 patients without dHACM(non-amnio group)and a minimum follow-up of 36 months.At the time of RARP,dHACM was placed around the neurovascular bundle in the amnio group.Continuous and categorical variables in matched groups was tested by two-sample Kolmogorov-Smirnov test and Fisher's exact test respectively.Outcomes measured were biochemical recurrence(BCR),adjuvant and salvage therapy rates.Results:Propensity score matching resulted in two groups of 444 patients.Cumulative incidence functions for BCR did not show a difference between the groups(p=0.3).Patients in the non-amnio group required salvage therapy more frequently than the amnio group,particularly after partial nerve-sparing RARP(6.3%vs.2.3%,p=0.001).Limitations are the absence of prospective randomization.Conclusion:The data suggest that using dHACM does not have a negative impact on BCR in patients.Outcomes of cancer specific and overall survival will require follow-up study to increase our understanding of these grafts’impact on prostate cancer biology.
文摘Chile,a pioneer and benchmark partner for China's free trade.cooperation in Latin America,holds a special position in China-Latin America economic and trade relations.It was the first Latin American country to sign a bilateral free trade agreement with China and the first to reach an upgraded protocol.Chile also established mutual recognition of Authorized Economic Operators(AEO)with China,the first country in South America to do so.
基金Supported by National Natural Science Foundation of China,No.81972947Academic Promotion Programme of Shandong First Medical University,No.2019LJ005.
文摘BACKGROUND The risk factors and prediction models for diabetic foot(DF)remain incompletely understood,with several potential factors still requiring in-depth investigations.AIM To identify risk factors for new-onset DF and develop a robust prediction model for hospitalized patients with type 2 diabetes.METHODS We included 6301 hospitalized patients with type 2 diabetes from January 2016 to December 2021.A univariate Cox model and least absolute shrinkage and selection operator analyses were applied to select the appropriate predictors.Nonlinear associations between continuous variables and the risk of DF were explored using restricted cubic spline functions.The Cox model was further employed to evaluate the impact of risk factors on DF.The area under the curve(AUC)was measured to evaluate the accuracy of the prediction model.RESULTS Seventy-five diabetic inpatients experienced DF.The incidence density of DF was 4.5/1000 person-years.A long duration of diabetes,lower extremity arterial disease,lower serum albumin,fasting plasma glucose(FPG),and diabetic nephropathy were independently associated with DF.Among these risk factors,the serum albumin concentration was inversely associated with DF,with a hazard ratio(HR)and 95%confidence interval(CI)of 0.91(0.88-0.95)(P<0.001).Additionally,a U-shaped nonlinear relationship was observed between the FPG level and DF.After adjusting for other variables,the HRs and 95%CI for FPG<4.4 mmol/L and≥7.0 mmol/L were 3.99(1.55-10.25)(P=0.004)and 3.12(1.66-5.87)(P<0.001),respectively,which was greater than the mid-range level(4.4-6.9 mmol/L).The AUC for predicting DF over 3 years was 0.797.CONCLUSION FPG demonstrated a U-shaped relationship with DF.Serum albumin levels were negatively associated with DF.The prediction nomogram model of DF showed good discrimination ability using diabetes duration,lower extremity arterial disease,serum albumin,FPG,and diabetic nephropathy(Clinicaltrial.gov NCT05519163).
文摘Approximately 350 million people are estimated to be persistently infected with hepatitis B virus(HBV) worldwide. HBV maintains persistent infection by employing covalently closed circular DNA(ccc DNA), a template for all HBV RNAs. Chronic hepatitis B(CHB) patients are currently treated with nucleos(t)ide analogs such as lamivudine, adefovir, entecavir, and tenofovir. However, these treatments rarely cure CHB because they are unable to inhibit ccc DNA transcription and inhibit only a late stage in the HBV life cycle(the reverse transcription step in the nucleocapsid). Therefore, an understanding of the factors regulating ccc DNA transcription is required to stop this process. Among numerous factors, hepatocyte nuclear factors(HNFs) play the most important roles in ccc DNA transcription, especially in the generation of viral genomic RNA, a template for HBV replication. Therefore, proper control of HNF function could lead to the inhibition of HBV replication. In this review, we summarize and discuss the current understanding of the roles of HNFs in the HBV life cycle and the upstream factors that regulate HNFs. This knowledge will enable the identification of new therapeutic targets to cure CHB.
基金Foundation of Northeast China Innovation and Opening Laboratory of Eco-Meteorology,CMA,No.stqx2017zd01Special Projects of Climate Change of CMA,No.CCSF201512+1 种基金Foundation of Institute of Atmospheric Environment in Shenyang,CMA,No.2016SYIAE11National Natural Science Foundation of China,No.41165005
文摘Drought has become a problem that is universally faced by global terrestrial ecosystems. Northeast China is located in a region sensitive to global climate changes, and one of the main impacts of climate changes in Northeast China is manifested as drought in growing seasons. This study analyzes the spatio-temporal evolution law of the water use efficiency(WUE) of the main natural vegetation(i.e., cold-temperate coniferous forests, temperate pine-broad-leaved mixed forests, warm-temperate deciduous broad-leaved forests, and grasslands) in Northeast China based on public MODIS data products, including MCD12 Q1, MOD15 A2 H, MOD16 A2, and MOD17 A3 H, and meteorological data from 2002 to 2013. The influence of drought events on the WUE of different vegetation types and their response to drought events are also investigated. The study findings are as follows:(1) drought in Northeast China frequently occurs in the regions stretching from 114.55°E to 120.90°E, and the percentage of drought area among the forests is lower than that among the grasslands during these years;(2) the annual average WUE of the natural vegetation ranges from 0.82 to 1.08 C/kg^(-1) H_2O, and the WUE of forests(0.82 to 1.08 C/kg^(-1) H_2O) is universally higher than that of grasslands(0.84 to 0.99 C/kg^(-1) H_2O);(3) in 2008, the regions where the WUE in drought conditions is higher than that in normal water conditions account for 86.11% of the study area, and a significant linear positive correlation is found between the WUE in drought conditions and the WUE in normal water conditions, whereas the degree of drought does not influence the WUE of the natural vegetation in an obviously linear manner; and(4) the WUE for the cold-temperate coniferous forests and temperate pine-broad-leaved mixed forests with a high ET or low NPP is more likely to rise in drought conditions; the WUE for the grasslands with a low Evapotranspiration(ET), Net Primary Production(NPP), and Leaf Area Index(LAI) is more likely to rise in drought conditions; and the ET, NPP, and LAI have no significant influence on the WUE for the warm-temperate deciduous broad-leaved forests in drought conditions. This study contributes to improving the evaluation of the influence of drought on natural ecosystems.
基金The University of Adelaide for Early Career Researcher Seed Funding(15128587)the University of Electronic Science and Technology of China(UESTC)for Startup funding(A1098531023601264)the National Natural Science Foundation of China(NSFC 22102018 and 52171201)。
文摘Electrocatalytic oxygen reduction reaction (ORR) via two-electron pathway is a promising approach to decentralized and on-site hydrogen peroxide (H_(2)O_(2)) production beyond the traditional anthraquinone process.In recent years,electrochemical H_(2)O_(2) production in acidic media has attracted increasing attention owing to its stronger oxidizing capacity,superior stability,and higher compatibility with various applications.Here,recent advances of H_(2)O_(2) electrosynthesis in acidic media are summarized.Specifically,fundamental aspects of two-electron ORR mechanism are firstly presented with an emphasis on the pH effect on catalytic performance.Major categories of promising electrocatalysts are then reviewed,including noble-metal-based materials,non-noble-metal single-atom catalysts,non-noblemetal compounds,and metal-free carbon-based materials.The innovative development of electrochemical devices and in situ/on-site application of electrogenerated H_(2)O_(2) are also highlighted to bridge the gap between laboratory-scale fundamental research and practically relevant H_(2)O_(2) electrosynthesis.Finally,critical perspectives on present challenges and promising opportunities for future research are provided.
基金supported by the Natural Scientific Foundation of China (21825501)National Key Research and Development Program (2016YFA0202500 and 2016YFA0200102)+1 种基金Australian Research Council (DP160103107, FT170100224)Tsinghua University Initiative Scientific Research Program。
文摘The demand for efficient and environmentally-benign electrocatalysts that help availably harness the renewable energy resources is growing rapidly. In recent years, increasing insights into the design of water electrolysers, fuel cells, and metal–air batteries emerge in response to the need for developing sustainable energy carriers, in which the oxygen evolution reaction and the oxygen reduction reaction play key roles. However, both reactions suffer from sluggish kinetics that restricts the reactivity. Therefore, it is vital to probe into the structure of the catalysts to exploit high-performance bifunctional oxygen electrocatalysts. Spinel-type catalysts are a class of materials with advantages of versatility, low toxicity, low expense, high abundance, flexible ion arrangement, and multivalence structure. In this review, we afford a basic overview of spinel-type materials and then introduce the relevant theoretical principles for electrocatalytic activity, following that we shed light on the structure–property relationship strategies for spinel-type catalysts including electronic structure, microstructure, phase and composition regulation,and coupling with electrically conductive supports. We elaborate the relationship between structure and property, in order to provide some insights into the design of spinel-type bifunctional oxygen electrocatalysts.
基金supported by the National Key Research and Development Program(2016YFA0202500 and 2016YFA0200101)the Natural Scientific Foundation of China(21825501)
文摘To satisfy the rapid development of gas-involving electrocatalysis(O2, CO2, N2, etc.), nanostructured electrocatalysts with favorably regulated electronic structure and surface nanostructures are urgently required. Herein, we highlighted a core-branch hydroxysulfide as a significantly enhanced oxygen evolution reaction electrocatalyst. This hydroxysulfide was facilely fabricated via a versatile interfacial reaction in S2- inorganic solution at room temperature for a designed period. The moderative growth kinetics contributed to the growth of interconnected hydroxysulfide nanosheets with high-sulfur contents on the hydroxide precursor substrates, resulting in a hierarchical nanostructure with multifunctional modifications, including regulated electronic structure, rapid electron highway, excellent accessibility, and facilitated mass transfer. Such synthetic methodology can be generalized and facilely governed by regulating the temperature, concentration, duration, and solvent for targeted nanostructures. Contributed to the favorably regulated electronic structure and surface nanostructure, the as-obtained core-branch Co2NiS2.4(OH)1.2 sample exhibits superior OER performance, with a remarkably low overpotential(279 m V required for 10.0 m A c^m-2), a low Tafel slope(52 m V dec^-1), and a favorable long-term stability. This work not only presents a promising nanostructured hydroxysulfide for excellent OER electrocatalysis, but also shed fresh lights on the further rational development of efficient electrocatalysts.
基金supported financially by the Subject Chief Scientist Program (10XD14303900) from Science and Technology Commission of Shanghai Municipalitythe Special Research Fund for the Doctoral Program of Higher Education of China (20123107110005)
文摘The solubility data of compounds in supercritical fluids and the correlation between the experimental solubility data and predicted solubility data are crucial to the development of supercritical technologies. In the present work, the solubility data of silymarin(SM) in both pure supercritical carbon dioxide(SCCO2) and SCCO2 with added cosolvent was measured at temperatures ranging from 308 to 338 K and pressures from 8 to 22 MPa. The experimental data were fit with three semi-empirical density-based models(Chrastil, Bartle and Mendez-Santiago and Teja models) and a back-propagation artificial neural networks(BPANN) model. Interaction parameters for the models were obtained and the percentage of average absolute relative deviation(AARD%) in each calculation was determined. The correlation results were in good agreement with the experimental data. A comparison among the four models revealed that the experimental solubility data were more fit with the BPANN model with AARDs ranging from 1.14% to 2.15% for silymarin in pure SCCO2 and with added cosolvent. The results provide fundamental data for designing the extraction of SM or the preparation of its particle using SCCO2 techniques.
基金supported by the National Natural Science Foundation of China(NSFC,Nos.U1904215,21671170,21673203,21805192 and 21875207)the Top-notch Academic Programs Project of Jiangsu Higher Education Institutions(TAPP)+5 种基金the Six Talent Plan(No.2015-XCL-030)the Guangdong Basic and Applied Basic Research Foundation(No.2019A1515110735)China Postdoctoral Science Foundation(No.2020M671612)Jiangsu Province Postdoctoral Science Foundation(No.2020Z082)Excellent Doctoral Dissertation of Yangzhou University and Undergraduate Scientific Research Innovation Projects in Jiangsu Province(No.201911117036Z)the Priority Academic Program Development of Jiangsu Higher Education Institutions。
文摘Nowadays,Cu-based materials have attracted extensive attention as electrocatalysts,while the inherent reason of the filling of high anti-bonding state of Cu d band(3 d^(10)4 s^(1))makes it difficult to hybridize with O2 p band of oxygen intermediates during the adsorption process of oxygen evolution reaction(OER).To increase the efficiency of Cu-based electrocatalysts,efforts have been made to optimize the electronic structures and to create surface defects and hierarchical nanostructures with more exposed accessible active sites.Herein,we report a facile method for preparing CuO electrocatalysts with hierarchical nanostructures using the Cu-alanine complex as a precursor through room-temperature chemical precipitation and subsequent calcination in air.Investigations of products obtained at different calcination temperatures reveal the relationship between OER activities and the material characteristics such as specific surface areas,crystal growth orientations,and element components.The product obtained at 500℃exhibits the smallest overpotential of 290 mV in 1.0 mol/L KOH for electrocatalyzing OER.Combining with various characterizations of CuO electrocatalysts after OER activities,the possible catalytic mechanism and the influence factors of their OER performance are also discussed.
基金supported by Grants-in-Aid for Scientific Research on Priority Areas from The Ministry of Education, Culture, Sports, Science and Technology(No.26430043to TO)。
文摘Recent studies have shown that mutation at Ser522 causes inhibition of collapsin response mediator protein 2(CRMP2) phosphorylation and induces axon elongation and partial recovery of the lost sensorimotor function after spinal cord injury(SCI).We aimed to reveal the intracellular mechanism in axotomized neurons in the CRMP2 knock-in(CRMP2KI) mouse model by performing transcriptome analysis in mouse sensorimotor cortex using micro-dissection punching system.Prior to that, we analyzed the structural pathophysiology in axotomized or neighboring neurons after SCI and found that somatic atrophy and dendritic spine reduction in sensorimotor cortex were suppressed in CRMP2KI mice.Further analysis of the transcriptome has aided in the identification of four hemoglobin genes Hba-a1, Hba-a2, Hbb-bs, and Hbb-bt that are significantly upregulated in wild-type mice with concomitant upregulation of genes involved in the oxidative phosphorylation and ribosomal pathways after SCI.However, we observed substantial upregulation in channel activity genes and downregulation of genes regulating vesicles, synaptic function, glial cell differentiation in CRMP2KI mice.Moreover, the transcriptome profile of CRMP2KI mice has been discussed wherein energy metabolism and neuronal pathways were found to be differentially regulated.Our results showed that CRMP2KI mice displayed improved SCI pathophysiology not only via microtubule stabilization in neurons, but also possibly via the whole metabolic system in the central nervous system, response changes in glial cells, and synapses.Taken together, we reveal new insights on SCI pathophysiology and the regenerative mechanism of central nervous system by the inhibition of CRMP2 phosphorylation at Ser522.All these experiments were performed in accordance with the guidelines of the Institutional Animal Care and Use Committee at Waseda University, Japan(2017-A027 approved on March 21, 2017;2018-A003 approved on March 25, 2018;2019-A026 approved on March 25, 2019).
基金the National Key R&D Program of China,No.2018YFC1313103the National Natural Science Foundation of China,No.81670473 and No.81873546+1 种基金the“Shu Guang”Project of Shanghai Municipal Education Commission and Shanghai Education Development Foundation,No.19SG30the Key Area Research and Development Program of Guangdong Province,China,No.2018B010111001.
文摘BACKGROUND Artificial intelligence in colonoscopy is an emerging field,and its application may help colonoscopists improve inspection quality and reduce the rate of missed polyps and adenomas.Several deep learning-based computer-assisted detection(CADe)techniques were established from small single-center datasets,and unrepresentative learning materials might confine their application and generalization in wide practice.Although CADes have been reported to identify polyps in colonoscopic images and videos in real time,their diagnostic performance deserves to be further validated in clinical practice.AIM To train and test a CADe based on multicenter high-quality images of polyps and preliminarily validate it in clinical colonoscopies.METHODS With high-quality screening and labeling from 55 qualified colonoscopists,a dataset consisting of over 71000 images from 20 centers was used to train and test a deep learning-based CADe.In addition,the real-time diagnostic performance of CADe was tested frame by frame in 47 unaltered full-ranged videos that contained 86 histologically confirmed polyps.Finally,we conducted a selfcontrolled observational study to validate the diagnostic performance of CADe in real-world colonoscopy with the main outcome measure of polyps per colonoscopy in Changhai Hospital.RESULTS The CADe was able to identify polyps in the test dataset with 95.0%sensitivity and 99.1%specificity.For colonoscopy videos,all 86 polyps were detected with 92.2%sensitivity and 93.6%specificity in frame-by-frame analysis.In the prospective validation,the sensitivity of CAD in identifying polyps was 98.4%(185/188).Folds,reflections of light and fecal fluid were the main causes of false positives in both the test dataset and clinical colonoscopies.Colonoscopists can detect more polyps(0.90 vs 0.82,P<0.001)and adenomas(0.32 vs 0.30,P=0.045)with the aid of CADe,particularly polyps<5 mm and flat polyps(0.65 vs 0.57,P<0.001;0.74 vs 0.67,P=0.001,respectively).However,high efficacy is not realized in colonoscopies with inadequate bowel preparation and withdrawal time(P=0.32;P=0.16,respectively).CONCLUSION CADe is feasible in the clinical setting and might help endoscopists detect more polyps and adenomas,and further confirmation is warranted.
文摘Secondary metabolites are important for various industrial applications. The production of secondary metabolites is often improved by the activation of substrate supply pathways for biosynthesis. However, many important pathways have remained unclear. In this study, we explored possible pathways related to substrate supply for the biosynthesis of the antifungal agent FR901469 which is a nonribosomal peptide and a fungal secondary metabolite. To clarify the unknown activated pathways, we utilized the Comprehensive Pathway Model (CPM) which was developed in our previous study. We verified that the overexpression of the hypothetical beta-alanine-aminotransferase (BAL-AT), which was included in the explored pathways, improved the FR901469 productivity. The genes encoding the BAL metabolic enzymes are considered to be important for improving the FR901469 productivity.
基金partially funded by Nippo Co.,Ltd.,Japan Science and Technology Agency(JST COI-NEXT,grant no.JPMJPF2017).
文摘Age-related mitochondrial dysfunction leads to defects in cellular energy metabolism and oxidative stress defense systems,which can contribute to tissue damage and disease development.Among the key regulators responsible for mitochondrial quality control,peroxisome proliferator-activated receptor gamma coactivator 1-alpha(PGC-1α)is an important target for mitochondrial dysfunction.We have previously reported that bioactive polyphenols extracted from sugarcane top(ST)ethanol extract(STEE)could activate neuronal energy metabolism and increase astrocyte PGC-1αtranscript levels.However,their potential impact on the mitochondria activity in muscle and liver cells has not yet been investigated.To address this gap,our current study examined the effects of STEE and its polyphenols on cultured myotubes and hepatocytes in vitro.Rhodamine 123 assay revealed that the treatment with STEE and its polyphenols resulted in an increase in mitochondrial membrane potential in C2C12 myotubes.Furthermore,a comprehensive examination of gene expression patterns through transcriptome-wide microarray analysis indicated that STEE altered gene expressions related to mitochondrial functions,fatty acid metabolism,inflammatory cytokines,mitogen-activated protein kinase(MAPK)signaling,and cAMP signaling in both C2C12 myotubes and HepG2 hepatocytes.Additionally,protein-protein interaction analysis identified the PGC-1αinteractive-transcription factors-targeted regulatory network of the genes regulated by STEE,and the quantitative polymerase chain reaction results confirmed that STEE and its polyphenols upregulated the transcript levels of PGC-1αin both C2C12 and HepG2 cells.These findings collectively suggest the potential beneficial effects of STEE on muscle and liver tissues and offer novel insights into the potential nutraceutical applications of this material.
基金supported by JST-CREST and JST COI-NEXT program under Grant number JPMJCR1925 and JPMJPF2009supported by JST SPRING under Grant number JPMJSP2138,Deutsche Forschungsgemeinschaft SFB1278(TP C04)+1 种基金the Leibniz Association(Leibniz Science Campus,InfectoOptics,HotAim 2.0)supported by Janelia Research Campus,Howard Hughes Medical Institute.
文摘Fluorescence microscopy enables the visualization of cellular morphology,molecular distribution,ion distribution,and their dynamic behaviors during biological processes.Enhancing the signal-to-noise ratio(SNR)in fluorescence imaging improves the quantification accuracy and spatial resolution;however,achieving high SNR at fast image acquisition rates,which is often required to observe cellular dynamics,still remains a challenge.In this study,we developed a technique to rapidly freeze biological cells in milliseconds during optical microscopy observation.Compared to chemical fixation,rapid freezing provides rapid immobilization of samples while more effectively preserving the morphology and conditions of cells.This technique combines the advantages of both live-cell and cryofixation microscopy,i.e.,temporal dynamics and high SNR snapshots of selected moments,and is demonstrated by fluorescence and Raman microscopy with high spatial resolution and quantification under low temperature conditions.Furthermore,we also demonstrated that intracellular calcium dynamics can be frozen rapidly and visualized using fluorescent ion indicators,suggesting that ion distribution and conformation of the probe molecules can be fixed both spatially and temporally.These results confirmed that our technique can time-deterministically suspend and visualize cellular dynamics while preserving molecular and ionic states,indicating the potential to provide detailed insights into sample dynamics with improved spatial resolution and temporal accuracy in observations.
基金supported by the National Natural Science Foundation of China(U1904215,21671170 and 21875207)the Top-notch Academic Programs Project of Jiangsu Higher Education Institutions(TAPP)+4 种基金the Program for New Century Excellent Talents of the University in China(NCET-13-0645)the Six Talent Plan(2015XCL-030)Qinglan Projectthe Priority Academic Program Development of Jiangsu Higher Education Institutionsthe support from the postdoctoral fund of Yangzhou University。
文摘Two-dimensional(2D)metal-organic frameworks(MOFs)are promising for electrocatalysis with high performance,as they possess large surface areas and high densities of exposed active sites.It attracts tremendous attention to obtain 2D nanostructures via simple preparation methods.Herein,a facile pyridine-modulated solvothermal synthesis of Ni/Co bimetallic MOF nanoplates(NixCoy-bpy(PyM))is reported with well-defined 2D morphology with a thickness as thin as 20 nm and an aspect ratio larger than 50.These nanoplates possess oxygen evolution reaction activity as electrocatalysts in alkaline conditions.Specifically,Ni0.5Co1.5-bpy(PyM)exhibits excellent OER electrocatalytic activity with a low overpotential of 256 mV at 10 m A cm-2 and a small Tafel slope of 81.8 mV dec-1 in 1.0 mol L-1 KOH with long-term electrochemical stability for 3000 cyclic voltammetry cycles.The high catalytic activity of Ni0.5Co1.5-bpy(PyM)can be attributed to the in situ formed active hydroxide and oxyhydroxide species within the inherited 2D morphology and the optimized bimetallic ratio.
基金This work was supported by the National Institute of Advanced Industrial Science and Technology,and the National Natural Science Foundation of China(NSFC-21875207).
文摘Through partial deligandation of metal-organic frameworks(MOFs),quasi-MOFs with a transition structure between MOFs and metal compounds(such as metal oxides,nitrides,sulfides,and phosphides)can be fabricated.Quasi-MOFs can not only retain the porous structure of MOFs to a certain extent,but also expose the inorganic nodes to the vip species(e.g.,metal nanoparticles)to show enhanced metal-support interaction for synergistic catalysis.This concept was first demonstrated by our group through calcining Au/MIL-101 at different temperatures under Ar flow to adjust the interface between Au nanoparticles and the inorganic Cr–O nodes.The obtained Au/quasi-MIL-101 showed superior enhanced catalytic activity in the oxidation of carbon monoxide.This study has inspired further research interest to fabricate other quasi-MOFs through controlled deligandation of mono-and bimetallic MOFs and their composites for the design of efficient catalysts.
文摘Carb on nanospheres(XC-72R)were functionalized by boron-oxygen(B-O)through coannealing with boric acid,to which highly dispersed palladium nanoparticles(Pd NPs)(-1.7 nm)were immobilized by a wet chemical reduction for the first time.The resultant Pd/OB-C catalystexhibits significantly improved activity for the dehydrogenation from formic acid(FA)compared to pristine XC-72R supported Pd NPs(Pd/C).Impressively,by adding melamine precursor,the B-0 and nitrogen(N)-functionalized product OB-C-N displays an extremely high B content,ca.34 times higher than OB-C.The Pd/OB-C-N catalyst with an ultrafine Pd particle size of-1.4 nm shows a superb activity,with a turnoverfrequency(TOF)as high as 5,354 h^-1 at 323 K,owing to the uniform ultrafine Pd NPs and the effect from B-0 and N functionalities.
基金National Institute of Advanced Industrial Science and Technology(AIST)the Japan Society for the Promotion of Science(JSPS)for financial support。
文摘The hydrogen evolution reaction(HER)as a fundamental process in electrocatalysis plays a significant role in clean energy technologies.For an energy-efficient HER,it demands an effective,durable,and low-cost catalyst to trigger proton reduction with minimal overpotential and fast kinetics.Here,we successfully fabricate a highly efficient HER catalyst of N-C/Co/Mo_(2)C holey nanorods with Co/b-Mo_(2)C nanoparticles uniformly embedded in nitrogen-doped carbon(N-C/Co/Mo_(2)C)by pyrolyzing the molybdate-coordinated zeolitic imidazolate framework(ZIF-67/MoO_(4)^(2-))holey nanorods,which result from the reaction between CoMoO_(4)and Me IM in a methanol/water/triethylamine mixed solution.The uniform distribution of MoO_(4)^(2-)in the ZIF-67/MoO_(4)^(2-)enables Co/β-Mo_(2)C nanoparticles to be welldistributed within nitrogen-doped carbon holey nanorods.This synthetic strategy endows the N-C/Co/Mo_(2)C catalyst with uniformly decorated bimetal,thus attaining excellent HER electrocatalytic activities with a small overpotential of 142.0 m V at 10 m A cm^(-2)and superior stability in 1.0 mol L^(-1)KOH aqueous solution.
基金supported by the National Natural Science Foundation of China(NSFC-21671170,21673203,21875207,21201010)the Top-notch Academic Programs Project of Jiangsu Higher Education Institutions(TAPP)+4 种基金Program for New Century Excellent Talents of the University in China(NCET-13-0645)Postgraduate Research&Practice Innovation Program of Jiangsu Province(XSJCX17-015)the Priority Academic Program Development of Jiangsu Higher Education InstitutionsYangzhou University Graduate Student International Academic Exchange Special Fund Projectthe Technical Support we received at the Testing Center of Yangzhou University.
文摘Porous metal phosphide cubes with exposed vertices and edges containing abundant catalytically active sites are promising electrocatalysts.Herein,by integrating the advantages of the phosphorus-rich cobalt phosphides and bimetallic oxides to form hybrid architectures,we prepared CoP_(3)/CoSnO_(2)via phosphating CoSn(OH)_(6)nanocubes,which has unique porous nanocubic structure.The optimized CoP_(3)/CoSnO_(2)porous nanaocubes showed excellent electrocatalytic activity for OER/ORR.What’s more,the electrochemical performances of CoP_(3)/CoSnO_(2)porous nanaocubes as air cathode catalyst for zinc air batteries were better than that of commercial RuO_(2)and 20 wt%Pt/C with a mass ratio of 1:1 as the air cathode catalyst.This work offers a new strategy to fabricate metal phosphide with porous nanocubic structures.
