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Spin effect on redox acceleration and regioselectivity in Fe-catalyzed alkyne hydrosilylation

National Science Review 2024年第2期11卷 155-167页

作者： Peng He Meng-Yang Hu Jin-hong Li Tian-Zhang Qiao yi-Lin lu Shou-Fei Zhu Frontiers Science Center for New Organic Matter State Key Laboratory and Institute of Elemento-Organic Chemistry Nankai University

Iron catalysts are ideal transition metal catalysts because of the Earths abundant, cheap, biocompatible features of iron salts. Iron catalysts often have unique open-shell structures that easily undergo spin crossover in chemical transformations, a feature rarely found in noble metal catalysts. Unfortunately, little is known currently about how the open-shell structure and spin crossover affect the reactivity and selectivity of iron catalysts, which makes the development of iron catalysts a low efficient trial-and-error program. In this paper, a combination of experiments and theoretical calculations revealed that the iron-catalyzed hydrosilylation of alkynes is typical spin-crossover catalysis. Deep insight into the electronic structures of a set of well-defined open-shell active formal Fe(0) catalysts revealed that the spin-delocalization between the iron center and the 1,10-phenanthroline ligand effectively regulates the iron center's spin and oxidation state to meet the opposite electrostatic requirements of oxidative addition and reductive elimination, respectively,and the spin crossover is essential for this electron transfer process. The triplet transition state was essential for achieving high regioselectivity through tuning the nonbonding interactions. These findings provide an important reference for understanding the effect of catalyst spin state on reaction. It is inspiring for the development of iron catalysts and other Earth-abundant metal catalysts, especially from the point of view of ligand development.

关键词： spin effect spin-delocalization spin crossover iron-catalysis alkyne hydrosilylation

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Percutaneous transhepatic cholangioscopy-assisted biliary polypectomy for local palliative treatment of intraductal papillary neoplasm of the bile duct

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World Journal of Gastrointestinal Oncology 2024年第5期16卷 1821-1832页

作者： Xu Ren Yong-Ping Qu Chun-Lan Zhu Xiao-hong Xu hong Jiang yi-Xia lu hong-Peng Xue Digestive Disease Hospital of Heilongjiang Provincial Hospital Heilongjiang Provincial Clinical Medical Research Center for Minimally Invasive Diagnosis and Treatment of Pancreaticobiliary DiseasesHarbin 150001Heilongjiang ProvinceChina Digestive Endoscopy Center of Heilongjiang Provincial Hospital Heilongjiang Provincial Clinical Medical Research Center for Minimally Invasive Diagnosis and Treatment of Pancreaticobiliary DiseasesHarbin 150001Heilongjiang ProvinceChina Second Department of Gastroenterology Digestive Disease Hospital of Heilongjiang Provincial Hospitaland Heilongjiang Provincial Clinical Medical Research Center for Minimally Invasive Diagnosis and Treatment of Pancreaticobiliary DiseasesHarbin 150001Heilongjiang ProvinceChina Department of Pathology Heilongjiang Provincial HospitalHarbin 150001Heilongjiang ProvinceChina

BACKGROUND Intraductal papillary neoplasm of the bile duct(IPNB)is a premalignant biliarytype epithelial neoplasm with intraductal papillary or villous growth.Currently reported local palliative therapeutic modalities,including endoscopic nasobiliary drainage,stenting and biliary curettage,endoscopic biliary polypectomy,percutaneous biliary drainage,laser ablation,argon plasma coagulation,photodynamic therapy,and radiofrequency ablation to relieve mechanical obstruction are limited with weaknesses and disadvantages.We have applied percutaneous transhepatic cholangioscopy(PTCS)-assisted biliary polypectomy(PTCS-BP)technique for the management of IPNB including mucin-hypersecreting cast-like and polypoid type tumors since 2010.AIM To assess the technical feasibility,efficacy,and safety of PTCS-BP for local palliative treatment of IPNB.METHODS Patients with mucin-hypersecreting cast-like or polypoid type IPNB and receiving PTCS-BP between September 2010 and December 2019 were included.PTCS-BP was performed by using a half-moon type snare with a soft stainless-steel wire,and the tumor was snared and resected with electrocautery.The primary outcome was its feasibility,indicated by technical success.The secondary outcomes were efficacy,including therapeutic success,curative resection,and clinical success,and safety.RESULTS Five patients(four with mucin-hypersecreting cast-like type and one with polypoid type IPNB)were included.Low-and high-grade intraepithelial neoplasia(HGIN)and recurrent IPNB with invasive carcinoma were observed in one,two,and two patients,respectively.Repeated cholangitis and/or obstructive jaundice were presented in all four patients with mucin-hypersecreting cast-like type IPNB.All five patients achieved technical success of PTCS-BP.Four patients(three with mucin-hypersecreting cast-like type and one with polypoid type IPNB)obtained therapeutic success;one with mucin-hypersecreting cast-like type tumors in the intrahepatic small bile duct and HGIN had residual tumors.All four patients with mucin-

关键词： Intraductal papillary neoplasm of the bile duct Percutaneous transhepatic cholangioscopy Biliary polypectomy Feasibility Efficacy

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Ex vivo liver resection and auto-transplantation as an alternative for the treatment of liver malignancies: Progress and challenges

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Hepatobiliary & Pancreatic Diseases International 2024年第2期23卷 117-122页

作者： Xin Yang lu lu Wen-Wei Zhu yi-Feng Tao Cong-Huan Shen Jin-hong Chen Zheng-Xin Wang lun-Xiu Qin Hepatobiliary Surgery and Liver Transplantation Centers Department of General SurgeryHuashan Hospital&Cancer Metastasis InstituteFudan UniversityShanghai 200040China

Hepatectomy is still the major curative treatment for patients with liver malignancies.However,it is still a big challenge to remove the tumors in the central posterior area,especially if their location involves the retrohepatic inferior vena cava and hepatic veins.Ex vivo liver resection and auto-transplantation(ELRA),a hybrid technique of the traditional liver resection and transplantation,has brought new hope to these patients and therefore becomes a valid alternative to liver transplantation.Due to its technical difficulty,ELRA is still concentrated in a few hepatobiliary centers that have experienced surgeons in both liver resection and liver transplantation.The efficacy and safety of this technique has already been demonstrated in the treatment of benign liver diseases,especially in the advanced alveolar echinococcosis.Recently,the application of ELRA for liver malignances has gained more attention.However,standardization of clinical practice norms and international consensus are still lacking.The prognostic impact in these oncologic patients also needs further evaluation.In this review,we summarized the principles and recent progresses on ELRA.

关键词： Ex vivo liver resection Liver auto-transplantation Oncology Liver malignancies

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Photocatalytic in situ H2O2 production and activation for enhanced ciprofloxacin degradation over CeO2-Co3O4/g-C3N4:key role of CeO2

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Rare Metals 2024年第6期43卷 2695-2707页

作者： hong-Jie Zhu yi-Kai Yang Ming-Hui Li lu-Ning Zou Hai-Tao Zhao Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology School of Chemistry and Chemical EngineeringLiaocheng University College of Ecology and Environment Anhui Normal University Liaocheng yilu Advanced Materials Co. Ltd

The abused ciprofloxacin antibiotics have caused significant environmental damage.Although oxidative degradation of ciprofloxacin exhibits promising efficacy,it often entails excessive energy consumption.Hence,it is necessary to explore an effective and ecologically sustainable degradation strategy.Herein,we demonstrated that g-C3N4decorated with the coordinated CeO2and Co3O4（CeO2-Co3O4/CN） exhibited effective ciprofloxacin photodegradation via in situ H2O2production and activation mechanism.Results indicate that the introduced CeO2enhances the transference of photogenerated electrons to O2by adjusting the oxygen vacancy of photocatalyst,thereby increasing the generation of superoxide radicals,which in turn generate H2O2,resulting in a 22.4-fold increase in H2O2generation over g-C3N4.Moreover,the in situ H2O2generation facilitated by CeO2is confirmed to be essential for ciprofloxacin degradation via CeO2-Co3O4/CN,as it provides enough oxidant for Co3O4to activate into hydroxyl radicals for the pollutants degradation.Ultimately,CeO2-Co3O4/CN achieves a ciprofloxacin degradation ratio of 97.7% within 80 min.This study introduces a novel approach that combines H2O2generation and activation,offering an innovative perspective for achieving clean and efficient purification of antibiotic-contaminated water.

关键词： CeO 2 In situ H 2 O 2 generation Ciprofloxacin degradation Photocatalyst

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Total-factor energy efficiency of ten major global energy-consuming countries

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Journal of Environmental Sciences 2024年第3期137卷 41-52页

作者： Xuan Wang Yonglong lu Chunci Chen Xiaojie yi Haotian Cui State Key Laboratory of Urban and Regional Ecology Research Centre for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China State Key Laboratory of Marine Environmental Science and Key Laboratory of the Ministry of Education for Coastal Wetland Ecosystems College of the Environment and EcologyXiamen UniversityFujian 361102China University of Chinese Academy of Sciences Beijing 100049China

Improving energy efficiency is regarded as a key path to tackling global warming and achieving the Sustainable Development Goals(SDGs).In 2020,the energy consumption of the world's ten major energy-consuming countries accounted for 66.8%of the global total.This paper applied data envelopment analysis(DEA)to calculate these ten major energyconsuming countries'total-factor energy efficiency(TFEE)at national and sectoral levels from 2001-2020,and explored the infuencing factors of total-factor energy efficiency with the Tobit regression model.The results showed significant difference in the ten countries'energy efficiency.The United States and Germany topped the list for total-factor energy efficiency,while China and India were at the bottom.Meanwhile,the energy efficiency of the industrial subsector has increased significantly over the past two decades,while that of the other subsectors has been relatively fat.The industrial structure upgrading,per capita GDP,energy consumption structure,and foreign direct investment had significant impacts on energy efficiency with national heterogeneity.Energy consumption structure and GDP per capita were determinative factors of energy efficiency.

关键词： Total-factor energy efficiency SBM-UN model Major energy-consuming country Carbon emission reduction

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A nanoplatform with oxygen self-supplying and heat-sensitizing capabilities enhances the efficacy of photodynamic therapy in eradicating multidrug-resistant biofilms

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Journal of Materials Science & Technology 2024年第2期169卷 209-219页

作者： Haixin Zhang yi Zou Kunyan lu Yan Wu Yuancheng Lin Jingjing Cheng Chunxia Liu hong Chen Yanxia Zhang Qian Yu State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials College of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China Department of Cardiovascular Surgery of the First Affiliated Hospital and Institute for Cardiovascular Science Suzhou Medical College of Soochow UniversitySoochow UniversitySuzhou 215007China

Bacterial biofilms,especially those caused by multidrug-resistant bacteria,have emerged as one of the greatest dangers to global public health.The acceleration of antimicrobial resistance to conventional an-tibiotics and the severe lack of new drugs necessitates the development of novel agents for biofilm eradication.Photodynamic therapy(PDT)is a promising non-antibiotic method for treating bacterial infections.However,its application in biofilm eradication is hampered by the hypoxic microenvironment of biofilms and the physical protection of extracellular polymeric substances.In this study,we develop a composite nanoplatform with oxygen(O_(2))self-supplying and heat-sensitizing capabilities to improve the PDT efficacy against biofilms.CaO_(2)/ICG@PDA nanoparticles(CIP NPs)are fabricated by combining calcium peroxide(CaO_(2))with the photosensitizer indocyanine green(ICG)via electrostatic interactions,followed by coating with polydopamine(PDA).The CIP NPs can gradually generate O_(2)in response to the acidic microenvironment of the biofilm,thereby alleviating its hypoxic state.Under near-infrared(NIR)irradiation,the nanoplatform converts O_(2)into a significant amount of singlet oxygen(^(1)O_(2))and heat to eradicate biofilm.The generated heat enhances the release of O_(2),accelerates the generation of^(1)O_(2)in PDT,increases cell membrane permeability,and increases bacterial sensitivity to^(1)O_(2).This nanoplatform significantly improves the efficacy of PDT in eradicating biofilm-dwelling bacteria without fostering drug resistance.Experiments on biofilm eradication demonstrate that this nanoplatform can eradicate over 99.9999%of methicillin-resistant Staphylococcus aureus(MRSA)biofilms under 5-min NIR irradiation.Notably,these integrated advantages enable the system to promote the healing of MRSA biofilm-infected wounds with negligible toxicity in vivo,indicating great promise for overcoming the obstacles associated with bacterial biofilm eradication.

关键词： Bacterial biofilm Multidrug-resistant bacteria Photodynamic therapy Oxygen supplying Photothermal therapy

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Effects of the urban landscape on heatwave-mortality associations in hong Kong: comparison of different heatwave definitions

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Frontiers of Environmental Science & Engineering 2024年第1期18卷 145-156页

作者： Jinglu Song yi lu Thomas Fischer Kejia Hu Department of Urban Planning and Design Xi’an Jiaotong-Liverpool UniversitySuzhou 215123China Department of Architecture and Civil Engineering City University of Hong KongKowloon TongHong Kong 999077China Environmental Assessment and Management Research Centre School of Environmental SciencesUniversity of LiverpoolLiverpool L35TRUK Research Unit for Environmental Sciences and Management Faculty of Natural and Agricultural SciencesNorth West UniversityPotchefstroom 31750South Africa Institute of Big Data in Health Science School of Public HealthZhejiang UniversityZijingang CampusHangzhou 310058China

Despite increased attention given to potential modifiers of temperature-mortality associations, evidence for variations between different urban landscape characteristics remains limited. It is in this context that in this paper effect modifications of multiple urban landscape characteristics are explored under different heatwave definitions for different age groups and gender in hong Kong, China. Daily meteorological data and heatwave-related mortality counts from 2008 to 2017 were collected from the hong Kong Census and Statistics Department, China. A case-only design was adopted, combined with logistic regression models to examine the modification effects of five urban landscape characteristics under six heatwave definitions. Stratified analyses were conducted to investigate age- and gender-specific effect modifications. It is found that individuals living in greener areas experienced lower levels of mortality during or immediately after heatwaves. In contrast, a higher building density and nighttime land surface temperature (LST) were associated with a higher heatwave-related mortality risk. Pronounced effect modifications of these urban landscape characteristics were observed under hotter and longer heatwaves, and in older adults (age ≥ 65 years) and males. The findings provide a scientific basis for policymakers and practitioners when considering measures for coping with hotter, longer, and more frequent heatwaves in the context of global climate change.

关键词： Urban landscape Heatwave Mortality Effect modification Intra-urban differences Health risk reduction

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A Degree Condition for Graphs Having All(a,b)-parity Factors

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Acta Mathematicae Applicatae Sinica 2024年第3期40卷 656-664页

作者： Hao-dong LIU hong-liang lu School of Mathematics and Statistics Xi'an Jiaotong UniversityXi'an 710049China

Let a and b be positive integers such that a≤b and a≡b(mod 2).We say that G has all(a,b)-parity factors if G has an h-factor for every function h:V(G)→{a,a+2,…,b-2,b} with b|V(G)| even and h(v)≡b(mod 2) for all v∈V(G).In this paper,we prove that every graph G with n≥2(b+1)(a+b) vertices has all(a,b)-parity factors if δ(G)≥(b^(2)-b)/a,and for any two nonadjacent vertices u,v ∈V(G),max{d_(G)(u),d_(G)(v)}≥bn/a+b.Moreover,we show that this result is best possible in some sense.

关键词： degree condition all(a,b)-factors

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Application of total keratometry in ten intraocular lens power calculation formulas in highly myopic eyes

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Eye and Vision 2024年第2期10卷 22-30页

作者： Ling Wei Kaiwen Cheng Wenwen He Xiangjia Zhu yi lu Department of Ophthalmology and Eye Institute Eye and ENT Hospital of Fudan UniversityShanghai 200031China Key Laboratory of Myopia(Fudan University)Key Laboratory of MyopiaShanghai Key Laboratory of Visual Impairment and Restoration National Health CommissionChinese Academy of Medical ScienceShanghai 200031China State Key Laboratory of Medical Neurobiology Fudan UniversityShanghai 200031China

Background:The accuracy of using total keratometry(TK)value in recent IOL power calculation formulas in highly myopic eyes remained unknown.Methods:Highly myopic patients who underwent uneventful cataract surgery were prospectively enrolled in this prospective comparative study.At one month postoperatively,standard deviation(SD)of the prediction errors(PEs),mean and median absolute error(MedAE)of 103 highly myopic eyes were back-calculated and compared among ten formulas,including XGboost,RBF 3.0,Kane,Barrett Universal II,Emmetropia Verifying Optical 2.0,Cooke K6,Haigis,SRK/T,and Wang-Koch modifications of Haigis and SRK/T formulas,using either TK or standard keratometry(K)value.Results:In highly myopic eyes,despite good agreement between TK and K(P>0.05),larger differences between the two were associated with smaller central corneal thickness(Plue,the XGboost calculator was comparable with the RBF 3.0 formula(P>0.05),which both presented smaller MedAEs than others(all P0.05),and statistically larger percentages than the other eight formulas(Plusions:Highly myopic eyes with thinner corneas tend to have larger differences between TK and K.The XGboost enhancement calculator and RBF 3.0 formula using TK showed the most promising outcomes in highly myopic eyes.

关键词： High myopia Total keratometry Cataract surgery IOL power calculation

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Can the integration between urban and rural areas be realized?A new theoretical analytical framework

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Journal of Geographical Sciences 2024年第1期34卷 3-24页

作者： WANG yi lu Yuqi ZHU yingming Research Base of Jiangsu Industrial Cluster School of Economics and ManagementNanjing University of Science and TechnologyNanjing 210094China School of Geography Nanjing Normal UniversityNanjing 210023China

Urban-rural integration is an advanced form resulting from the future evolution of urban-rural relationships.Nevertheless,little research has explored whether urban and rural areas can move from dual segmentation to integrated development from a theoretical or empirical perspective.Based on the research framework of welfare economics,which offers an appealing paradigm to frame the underlying game between cities and villages,this study clarifies the ideal state of urban-rural integration.It then proposes a series of basic assumptions,and constructs a corresponding objective function and its constraints.Moreover,it assesses the possibility of seeing the transmutation from division to integration between urban and rural areas with continuous socio-economic development.The authors argue that the ideal state of urban-rural integration should be a Pareto-driven optimal allocation of urban-rural resources and outputs,and the maximization of social welfare in the entire region.Based on a systematic demonstration using mathematical models,the study proposes that urban and rural areas can enter this ideal integrated development pattern when certain parameter conditions are met.In general,this study demonstrates the theoretical logic and scientific foundations of urban-rural integration,enriches theoretical studies about urban-rural relationships,and provides basic theoretical support for large developing countries to build a coordinated and orderly urban-rural community with a shared future.

关键词： urban-rural integration development ideal state parameter conditions welfare economics theoretical framework

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