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Structural insight into palladium-nickel clusters over mordenite zeolite for carbene-insertion reaction

Frontiers of Chemical Science and Engineering 2024年第9期18卷 89-99页

作者： Guangchao Li ping-Luen Baron Ho Bryan Kit Yue ng Tai-Sing Wu Pawel Rymarz Shik chi Edman Tsang Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHong Kong 999077China Department of Chemistry University of OxfordOxford OX13QRUK Synchrotron Radiation Research Center Hsinchu 30076China

The advancement of heterogeneous catalysts incorporating metal clusters in the nanometric size range has garnered significant attention due to their extraordinary catalytic activity and *** detailed characterization and understanding of the atomic structure of these metal clusters within catalysts is crucial for elucidating the underlying reaction *** the present study,a distinctive three-atom PdNi cluster,characterized by two Pd atoms at terminal positions and a central Ni atom,was synthesized over mordenite *** presence of atomic PdNi clusters within the eight-membered ring side pocket area was confirmed by multiple advanced analytical techniques,including magic-angle spinning nuclear magnetic resonance spectroscopy,synchrotron X-ray powder diffraction,extended X-ray absorption fine structure spectroscopy,and high-angle annular dark-field scanning transmission electron *** catalytic activity of the confined active species was examined by the carbene-mediated reactions of ethyl-2-diazoacetate to ethyl-2-methoxyacetate as a model *** to the Pd-mordenite and Ni-mordenite,the PdNi-mordenite catalyst incorporates a PdNi cluster,which demonstrates a superior performance,achieving 100%conversion and high selectivity under the same reaction *** study elucidates the potential of constructing bimetallic clusters in zeolites,providing valuable insights for developing new heterogeneous catalysts applicable to a wide range of catalytic processes.

关键词： zeolite metal cluster synchrotron X-ray diffraction carbene-mediated reaction

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Ligand-controlled NiH-catalyzed regiodivergent hydroalkylation of 2-alkenylazaarenes

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Science china Chemistry 2024年第6期67卷 1935-1940页

作者： Ya-ping Shao Zhuo-Min chi Yong-Min Liang State Key Laboratory of Applied Organic Chemistry School of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000China

A nickel-hydride(Ni H)-catalyzed migratory and nonmigratory hydroalkylation reaction of 2-alkenyl azaarenes with alkyl iodines has been established through strategic modulation of N-or P-donor *** method enables the synthesis of diverseβ-orγ-branched aromatic *** mild regiodivergent protocols exhibit wide substrate scope,excellent functional tolerance,and great reaction yield with remarkable ***,deuterium labeling studies reveal Ni H-catalyzed interrupted chain-walking mode as the mechanism behind remotedβ-selective hydroalkylation reaction—an interesting phenomenon mediated through aromatic imine directing groups.

关键词： NiH regiodivergent hydroalkylation azaarenes interrupted chain-walking

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Doping engineering of iron oxide nanoparticles towards high performance and biocompatible T_(1)-weighted MRI contrast agents

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Rare Metals 2024年第1期43卷 298-308页

作者： Xue Xu ping-Li Dong Yu-Yun Chai Run Yang Zhen-Hui Ma chi-Chong Lu Department of Chemistry College of Chemistry and Materials EngineeringBeijing Technology and Business UniversityBeijing 100048China Department of Physics Beijing Technology and Business UniversityBeijing 100048China

Extremely small-sized iron oxide nanoparticles(IONPs) are of great interest in magnetic resonance imaging(MRI) due to their biosafety as an alternative to clinical gadolinium(Ⅲ) complexes-based contrast *** when the particle size is less than 10 nm,it has strong diffusion ability and deep penetration distance in tumor *** doping can significantly enhance the T_(1)contrast effect of nanoparticles by regulating the surface exposed ***,the nucleation and growth processes of multi-component synthesis systems are complex and difficult to be accurately controlled,leading to great challenges in the synthesis of ultra-small-sized nanoparticles with different components and ***,extremely smallsized superparamagnetic gadolinium-doped iron oxide nanoparticles(GdIONPs,Gd_(x)Fe_(3-x)O_(4) NPs) with adjustable doping amount and controllable size in the range of 3.5-7.5 nm were synthesized by thermal ***,as-synthesized GdIONPs were surface modified with a highly water-soluble and biocompatible carboxyl-polyethylene glycol-phosphoric acid ligand with high binding ***_(0.65)Fe_(2.35)O_(4) NPs exhibited very high r_(1) relaxivity of 10.6 mmol^(-1)·L·s^(-1) in terms of all metal concentrations and 49.0 mmol^(-1)·L·s^(-1) in terms of gadolinium alone,respectively,3 and 14 times higher than clinical T_(1) contrast agents(Gd-DTPA).GdIONPs can continuously obtain high resolution images of blood vessels,and can be used as an efficient and multifunctional contrast agent for MR T_(1)*** stable and efficient doping strategy provides an easy and effective method to individually optimize the magnetic properties of complex oxides and their relaxation effects for a variety of biomedical applications.

关键词： Iron oxide nanoparticles Small size Magnetic resonance imaging Substitutional doping Gd dopant

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Federated Dynamic Client Selection for Fairness Guarantee in Heterogeneous Edge Computing

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Journal of Computer Science & Technology 2024年第1期39卷 139-158页

作者：毛莺池沈莉娟吴俊平萍吴杰 Key Laboratory of Water Big Data Technology of Ministry of Water Resources Hohai UniversityNanjing 211100China College of Computer and Information Hohai UniversityNanjing 211100China Center of Networked Computing Temple UniversityPhiladelphiaPA 19122-6096U.S.A

Federated learning has emerged as a distributed learning paradigm by training at each client and aggregat-ing at a parameter *** heterogeneity hinders stragglers from responding to the server in time with huge com-munication *** client grouping in federated learning can solve the straggler problem,the stochastic selection strategy in client grouping neglects the impact of data distribution within each ***,current client grouping ap-proaches make clients suffer unfair participation,leading to biased performances for different *** order to guaran-tee the fairness of client participation and mitigate biased local performances,we propose a federated dynamic client selec-tion method based on data representativity(FedSDR).FedSDR clusters clients into groups correlated with their own lo-cal computational *** estimate the significance of client datasets,we design a novel data representativity evalua-tion scheme based on local data ***,the two most representative clients in each group are selected to optimize the global ***,the DYNAMIC-SELECT algorithm updates local computational efficiency and data representativity states to regroup clients after periodic average *** on real datasets show that FedS-DR improves client participation by 27.4%,37.9%,and 23.3%compared with FedAvg,TiFL,and FedSS,respectively,tak-ing fairness into account in federated *** addition,FedSDR surpasses FedAvg,FedGS,and FedMS by 21.32%,20.4%,and 6.90%,respectively,in local test accuracy variance,balancing the performance bias of the global model across clients.

关键词： federated learning fairness computational efficiency data distribution client selection client grouping

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Mesenchymal-epithelial transition factor amplification correlates with adverse pathological features and poor clinical outcome in colorectal cancer

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World Journal of Gastrointestinal Surgery 2024年第5期16卷 1395-1406页

作者： Qiu-Xiao Yu ping-Ying Fu chi Zhang Li Li Wen-Ting Huang Department of Pathology National Cancer Center/National Clinical Research Center for Cancer/Cancer Hospital&Shenzhen HospitalChinese Academy of Medical Sciences and Peking Union Medical CollegeShenzhen 518116Guangdong ProvinceChina

BACKGROUND Colorectal cancer(CRC)is the third most common cancer and the second most common cause of cancer-related mortality ***-epithelial transition factor(MET)gene participates in multiple tumor biology and shows clinical potential for pharmacological manipulation in tumor *** amplification has been reported in CRC,but data are very *** pathological values of MET in CRC may provide new therapeutic and genetic screening options in future clinical *** To determine the pathological significance of MET amplification in CRC and to propose a feasible screening *** A number of 205 newly diagnosed CRC patients undergoing surgical resection without any preoperative therapy at Shenzhen Cancer Hospital of chinese Academy of Medical Sciences were *** patients were without RAS/RAF mutation or microsatellite *** amplification and c-MET protein expression were analyzed using fluorescence in situ hybridization(FISH)and immunohistochemistry(IHC),*** between MET aberration and pathological features were detected using the chi-squared *** free survival(PFS)during the two-year follow-up was detected using the Kaplan-Meier method and log rank *** results of MET FISH and IHC were com pared using one-way *** Polysomy-induced MET amplification was observed in 14.4%of cases,and focal MET amplification was not ***-induced MET amplification was associated with a higher frequency of lymph node metastasis(LNM)(Png grade(P=0.02).In the survival analysis,significant difference was detected between patients with amplified-and non-amplified MET in a two-year follow-up after the first diagnosis(P=0.001).C-MET scores of 0,1+,2+,and 3+were observed in 1.4%,24.9%,54.7%,and 19.0%of tumors,respectively.C-MET overexpression correlated with higher frequency of LNM(P=0.002),but no significant difference of PFS was dete

关键词： Colorectal cancer MET Amplification Pathological features Prognosis Fluorescence in situ hybridization

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The anthocyanin formation of purple leaf is associated with the activation of LfiHY5 and LfiMYB75 in crape myrtle

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Horticultural Plant Journal 2024年第5期10卷 1230-1246页

作者： Lu Feng ping Shen Xiufeng chi Yang Zhou Jieru Liu Tangren Cheng Jia Wang Qixiang Zhang Ming Cai Huitang Pan State Key Laboratory of Efficient Production of Forest Resources Beijing Key Laboratory of Ornamental Plants Germplasm Innovation&Molecular BreedingNational Engineering Research Center for FloricultureBeijing Laboratory of Urban and Rural Ecological EnvironmentKey Laboratory of Genetics and Breeding in Forest Trees and Ornamental Plants of Ministry of Education and College of Landscape ArchitectureBeijing Forestry UniversityBeijing 100083China

Purple-leafed plants not only have a higher resistance to biotic and abiotic stresses,but also have higher ornamental *** are vital for leaf color formation,growth and development of purple ***,the molecular mechanism underlying purple leaf formation in Lagerstroemia indica remains *** and transcriptomic analysis of purple-leafed cultivar‘Ebony Embers’and greenleafed cultivar‘Arapahoe’showed that the high expression of anthocyanin structure genes induced hyperaccumulation of cyanidin and pelargonidin derivatives,making the leaves ***5,LfiMYB75 and LfibHLH1 were identified using correlation analysis and weighted gene co-expression network ***‘Arapahoe’‘Ebony Embers’population,LfiHY5 and LfiMYB75 showed significant positive correlation with leaf anthocyanin *** expression of LfiMYB75 and LfiHY5 in tobacco and purple-leafed crape myrtle indicated that the two genes activated anthocyanin *** two-hybrid analysis showed that LfiMYB75 and LfibHLH1 could form a complex that enhanced anthocyanin *** monohybrid and dual-luciferase assays confirmed that LfiHY5 activated the expression of LfiMYB75,to activate the transcription of anthocyanin structural genes LfiCHS and ***,there were three alleles of LfiHY5 in crape myrtle,and the different sequences had different activation effects on *** conclusion,the results showed that LfiHY5 led to upregulate the transcription of LfiMYB75,and LfiMYB75 formed a complex with LfibHLH1,which increased the transcription level of LfiCHS and LfiANS to affect anthocyanin synthesis in crape myrtle.

关键词： Lagerstroemia indica Leaf color Anthocyanin HY5 MYB bHLH

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NHE7 upregulation potentiates the uptake of small extracellular vesicles by enhancing maturation of macropinosomes in hepatocellular carcinoma

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Cancer Communications 2024年第2期44卷 251-272页

作者： Yue Yao Yi Xu Liang Yu Ting-Mao Xue Zhi-Jie Xiao Pui-chi Tin Hiu-Ling Fung Hoi-Tang Ma Jing-ping Yun Judy Wai ping Yam Department of Pathology School of Clinical MedicineLi Ka Shing Faculty of MedicineThe University of Hong KongHong KongP.R.China Department of Endocrinology and Metabolism Second Affiliated Hospital of Harbin Medical UniversityHarbinHeilongjingP.R.China Department of Hepatopancreatobiliary Surgery Second Affiliated Hospital of Harbin Medical UniversityHarbinHeilongjingP.R.China State Key Laboratory of Oncology in South china Cancer Center of Sun Yat-sen UniversityGuangzhouGuangdongP.R.China Department of Hepatobiliary Surgery II Zhujiang HospitalSouthern Medical UniversityGuangzhouGuangdongP.R.China Scientific Research Center The Seventh Affiliated HospitalSun Yat-sen UniversityShenzhenGuangdongP.R.China State Key Laboratory of Liver Research The University of Hong KongHong KongP.R.China Department of Pathology Cancer Center of Sun Yat-sen UniversityGuangzhouGuangdongP.R.China

Background:Small extracellular vesicles(sEVs)mediate intercellular commu-nication that contributes to hepatocellular carcinoma(HCC)progression via multifaceted *** success of cell entry determines the effect of sEV on recipient ***,we aimed to delineate the mechanisms underlying the uptake of sEV in ***:AF,Alexa Fluor;ANOVA,analysis of variance;ATP9A,ATPase Phospholipid Transporting 9A;BCECF-AM,2’,7’-bis-(2-barboxyethyl)-5-(and-6)-carboxyfluorescein,acetoxymethyl ester;BSA,bovine serum albumin;CCMR,Centre for Comparative Medicine Research;CRISPR,clustered regularly interspaced short palindromic repeats;CTL,ctrl;CXCR4,C-X-C Chemokine Receptor Type 4;DAPI,4′,6-diamidino-2-phenylindole;DFS,disease-free survival;DMEM,Dulbecco’s Modified Eagle Medium;DMSO,dimethyl sulfoxide;Dox,doxycycline;EEA1,early endosome antigen 1;EIPA,5-(N-ethyl-N-isopropyl)-amiloride;FBS,fetal bovine serum;FITC,fluorescein isothiocyanate;GAPDH,glyceraldehyde-3-phosphate dehydrogenase;GM130,Golgi matrix protein 130;HCC,hepatocellular carcinoma;HEPES,4-(2-hydroxyethyl)-1-piperazineethanesulfonic acid;HPRT1,hypoxanthine phosphoribosyltransferase 1;H-score,histoscore;IAA,indole-3-acetic acid;KD,knockdown;KO,knockout;mAID,mini-auxin-inducible degron;MTT,3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide;NHE7,Na(+)/H(+)exchanger 7;ns,non-significant;OD,optical density;OS,overall survival;PBS,phosphate-buffered saline;PCR,polymerase chain reaction;pHe,endosomal pH;pHi,intracellular pH;PKH67,Paul Karl Horan 67;Rab21,Ras-associated binding protein 21;RIPA,radioimmunoprecipitation assay;SAM,synergistic activation mediator;SEMs,standard error of the means;sEVs,small extracellular vesicles;sgRNA,single-guide RNA;shRNA,short-hairpin RNA;SLC9,solute carrier gene 9;SLiCE,Seamless Ligation Cloning Extract;TCGA,The Cancer Genome Atlas;TCL,total cell lysates;TGN,trans-Golgi network;TMA,tissue microarray;TMR,tetramethyl rhodamine;TSG101,tumor susceptibility gene *** Yao an

关键词： hepatocellular carcinoma small extracellular vesicles macropinocytosis pH regulation sodium-hydrogen exchanger

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ABC/2 formula for"bedside"postoperative pneumocephalus volume measurement

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chinese Neurosurgical Journal 2022年第4期8卷 284-291页

作者： David Yuen Chung Chan Eric Yuk Hong Cheung Ka Ho Hui Cecelia Mei Sze Leung Stephanie chi ping ng Wai Kit Mak George Kwok Chu Wong Tat Ming Danny Chan Wai Sang Poon Division of Neurosurgery Department of SurgeryFaculty of MedicinePrince of Wales HospitalThe Chinese University of Hong KongHong KongSARChina

Background:Postoperative pneumocephalus is associated with a higher risk of recurrence of chronic subdural hematoma(cSDH).However,there is no verified simple way to measure the pneumocephalus volume at the bedside for daily clinical *** ABC/2 method was shown to be a simple and reliable technique to estimate volumes of intracranial lesions,such as intracranial *** study aims to evaluate the accuracy of the ABC/2 formula in estimating volumes of pneumocephalus,as compared to the gold standard with computer-assisted volumetric ***:A total of 141 postoperative computed tomographic(CT)brain scans of cSDH patients with burr-hole drainage were *** volume was measured independently by both the ABC/2 formula and the computer-assisted volumetric *** the computer-assisted measurement,the volume of the air was semiautomatically segmented and calculated by computer *** regression was used to determine the correlation between the ABC/2 method and computer-assisted ***:The postoperative pneumocephalus volume after bilateral burr-hole drainage was significantly larger than that of unilateral burr-hole drainage(29.34 ml versus 12.21 ml,png positive correlation,and it is statistically ***:An excellent correlation is observed between the ABC/2 method and the computer-assisted *** study verified that the ABC/2 method is an accurate and simple"bedside"technique to estimate pneumocephalus volume.

关键词： ABC/2 Chronic subdural haematoma Burr-hole Pneumocephalus

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Efficient C-N coupling in electrocatalytic urea generation on copper carbonate hydroxide electrocatalysts

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Journal of Energy Chemistry 2024年第6期93卷 289-298,I0008页

作者： Yinuo Wang Yian Wang Qinglan Zhao Hongming Xu Shangqian Zhu Fei Yang Ernest P.Delmo Xiaoyi Qiu chi Song Juhee Jang Tiehuai Li ping Gao MDanny Gu Minhua Shao Advanced Materials Thrust The Hong Kong University of Science and Technology(Guangzhou)Guangzhou 511400GuangdongChina Department of Chemical and Biological Engineering The Hong Kong University of Science and TechnologyClear Water BayKowloonHong KongChina Department of Materials Science and Engineering Southern University of Science and Technology of Chin11088 Xueyuan BoulevardShenzhen 518055GuangdongChina Energy Institute and Chinese National Engineering Research Center for Control&Treatment of Heavy Metal PollutionThe Hong Kong University of Science and TechnologyKowloonHong KongChina Department of Chemistry City University of Hong KongTat Chee AvenueKowloonHong KongChina

Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of ***,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen *** thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~**** work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.

关键词： Copper carbonate hydroxide Co-reduction Urea generation C-N coupling DFT calculation

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Umbilical Cord Blood Mononuclear Cell Treatment for Neonatal Rats with Hypoxic Ischemia

Umbilical Cord Blood Mononuclear Cell Treatment for Neonatal...

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第十六届中国医师协会神经外科医师年会

作者： Hao LYU Dong Ming SUN chi ping ng Wendy S CHEng Jun Fan CHEN Yu Zhong HE Sin Yu LAM Zhi Yuan ZHEng Guo Dong HUAng chi chiu WAng Wise Young Wai Sang POON Division of Neurosurgery Department of SurgeryFaculty of MedicineThe Chinese University of Hong Kong Department of Neurosurgery Shenzhen Key Laboratory of Neurosurgerythe Shenzhen Second People's HospitalFirst Affiliated Hospital of Shenzhen University W.M.Keck Center for Collaborative Neuroscience RutgersState University of New Jersey Department of Neurosurgery Hainan Hospital of People's Liberation Army General Hospital Department of Obstetrics and Gynecology The Chinese University of Hong Kong

Background:Hypoxic-Ischemic Encephalopathy(HIE) occurs when an infant’s brain has not received adequate oxygen and blood supply,resulting in ischemic and hypoxic ***,supportive care and hypothermia therapy have been the standard treatment for ***,there are still over 20% of treated infants died and 19-30% survived with significant *** animal model was first established by Vannucci et al,involving the ligation of one common carotid artery followed by *** this study,we investigated human umbilical cord blood(HUCB) and its two components mononuclear cell(MNC) and red cell fraction(RCF) in both short and long term study using a modified HIE rat ***:In this modified HIE model,both common carotid arteries were occluded,breathing 8% oxygen in a hypoxic chamber for 60-minute,followed by the release of the common carotid arteries ligature,mimicking reperfusion *** cell therapeutic study,cells were intravenously injected to HIE rat pups,and both behavioral and histological changes were assessed at selected time ***:Statistically significant behavioral improvements were demonstrated on Day 7 and 1 month between saline treated HIE rats and UCB/MNC treated ***,at 3 months,the therapeutic improvements were only showed between saline treated HIE animals and MNC treated HIE *** histological analysis one month after cell injection,the number of functional neurons were statistically increased between saline treated HIE and UCB/MNC/RCF treated HIE *** 3 months,the significant increase in functional neurons was only present in MNC treated HIE ***:We have used a bilateral temporary occlusion of 60 minutes,a moderately brain damaged model,for cell therapeutic *** umbilical cord blood(HUCB) mononuclear cell(MNC) therapy showed benefits in neonatal HIE rats in both short and long term behavioral and histological assessments.

关键词： Hypoxic Ischemic Encephalopathy animal model cell therapeutic

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