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Synergistic silver-mediated and palladium-catalyzed nondirected olefination of aryl C–H bond: quick access to multi-substituted aryl olefins

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Science China Chemistry 2024年第3期67卷 882-889页

作者： jian Yao Lili shao Xiaohong Huo Xiaoming Wang Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Frontiers Science Center for Transformative MoleculesSchool of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Organometallic Chemistry Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 20032China School of Chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China

Transition metal-catalyzed olefination of aryl C-H bond is a powerful tool for the synthesis of alkenes. While the Pd-catalyzed oxidative C-H olefination of arenes, also known as Fujiwara-Moritani reaction, has been established as one of the most efficient methods, the substrates are largely limited to terminal olefins with electron-withdrawing group(s). Herein, we report a synergistic silver-mediated and palladium-catalyzed non-directed C-H olefination of arenes with vinyl(pseudo)halides, which offers a complementary strategy to the typical Fujiwara-Moritani reaction. The reactions proceeded well for a variety of halogenated arenes, heteroarenes, and olefin substrates, providing an efficient access to various multi-substituted aryl olefins, including trisubstituted/tetrasubstituted olefins and several complex olefins derived from medicines or natural products. Mechanistic studies indicated a bimetallic Pd/Ag cooperation is operative in the catalysis, i.e., the reaction is initiated by aryl C-H bond cleavage via ligation with phosphine/Ag species, followed by transferring of the aryl moiety to a vinyl palladium intermediate,which is in turn formed by oxidative addition of vinyl(pseudo)halide to a Pd complex. This method enables the synthesis of a wide range of challenging multi-substituted vinyl products from simple arenes(directing-group free) in a streamlined and controllable fashion.

关键词： direct C–H olefination multi-substituted aryl alkenes bimetallic Pd/Ag cooperation C–H functionalization

The reaction mechanism and interfacial crystallization of Al nanoparticle-embedded Ni under shock loading

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Defence Technology（防务技术） 2024年第3期33卷 114-124页

作者： Yifan Xie jian-Li shao Rui Liu Pengwan Chen State Key Laboratory of Explosion Science and Technology Beijing Institute of TechnologyBeijing100081China Explosion Protection and Emergency Disposal Technology Engineering Research Center of the Ministry of Education Beijing100039China

The shock-induced reaction mechanism and characteristics of Ni/Al system,considering an Al nanoparticle-embedded Ni single crystal,are investigated through molecular dynamics simulation.For the shock melting of Al nanoparticle,interfacial crystallization and dissolution are the main characteristics.The reaction degree of Al particle first increases linearly and then logarithmically with time driven by rapid mechanical mixing and following dissolution.The reaction rate increases with the decrease of particle diameter,however,the reaction is seriously hindered by interfacial crystallization when the diameter is lower than 9 nm in our simulations.Meanwhile,we found a negative exponential growth in the fraction of crystallized Al atoms,and the crystallinity of B2-NiAl(up to 20%)is positively correlated with the specific surface area of Al particle.This can be attributed to the formation mechanism of B2-NiAl by structural evolution of finite mixing layer near the collapsed interface.For shock melting of both Al particle and Ni matrix,the liquid-liquid phase inter-diffusion is the main reaction mechanism that can be enhanced by the formation of internal jet.In addition,the enhanced diffusion is manifested in the logarithmic growth law of mean square displacement,which results in an almost constant reaction rate similar to the mechanical mixing process.

关键词： Shock-induced reaction Molecular dynamics simulations Interfacial crystallization Reaction mechanism

Mirizzi syndrome:Problems and strategies

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Hepatobiliary & Pancreatic Diseases International 2024年第3期23卷 234-240页

作者： Jun Wu Shuang-Yong cai Xu-Liang Chen Zhi-Tao Chen shao-Hua Shi Department of Hepatobiliary and Pancreatic Surgery People’s Hospital of Jiulongpo DistrictChongqing 400050China Department of Hepatobiliary and Pancreatic Surgery Shulan(Hangzhou)Hospital Affiliated to Zhejiang Shuren University Shulan International Medical CollegeHangzhou 310003China

Mirizzi syndrome is a serious complication of gallstone disease.It is caused by the impacted stones in the gallbladder neck or cystic duct.One of the features of Mirizzi syndrome is severe inflammation or dense fibrosis at the Calot’s triangle.In our clinical practice,bile duct,branches of right hepatic artery and right portal vein clinging to gallbladder infundibulum are often observed due to gallbladder infundibulum adhered to right hepatic hilum.The intraoperative damage of branches of right hepatic artery occurs more easily than that of bile duct,all of which are hidden pitfalls for surgeons.Magnetic resonance cholangiopancreatography(MRCP)and endoscopic retrograde cholangiopancreatography(ERCP)are the preferable tools for the diagnosis of Mirizzi syndrome.Anterograde cholecystectomy in Mirizzi syndrome is easy to damage branches of right hepatic artery and bile duct due to gallbladder infundibulum adhered to right hepatic hilum.Subtotal cholecystectomy is an easy,safe and definitive approach to Mirizzi syndrome.When combined with the application of ERCP,a laparoscopic management of Mirizzi syndrome by well-trained surgeons is feasible and safe.The objective of this review was to highlight its existing problems:(1)low preoperative diagnostic rate,(2)easy to damage bile duct and branches of right hepatic artery,and(3)high concomitant gallbladder carcinoma.Meanwhile,the review aimed to discuss the possible therapeutic strategies:(1)to enhance its preoperative recognition by imaging findings,and(2)to avoid potential pitfalls during surgery.

关键词： Mirizzi syndrome Bile duct injury Artery injury Surgical treatment Subtotal cholecystectomy

What benefit can be obtained from magnetic resonance imaging diagnosis with artificial intelligence in prostate cancer compared with clinical assessments?

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Military Medical Research 2024年第2期11卷 268-286页

作者： Li-Tao Zhao Zhen-Yu Liu Wan-Fang Xie Li-Zhi shao jian Lu Jie Tian jian-Gang Liu School of Engineering Medicine Beihang UniversityBeijing 100191China School of Biological Science and Medical Engineering Beihang UniversityBeijing 100191China CAS Key Laboratory of Molecular Imaging Institute of AutomationBeijing 100190China University of Chinese Academy of Sciences Beijing 100080China Department of Urology Peking University Third HospitalPeking UniversityBeijing 100191China Key Laboratory of Big Data‑Based Precision Medicine(Beihang University) Ministry of Industry and Information Technology of the People's Republic of ChinaBeijing 100191China Beijing Engineering Research Center of Cardiovascular Wisdom Diagnosis and Treatment Beijing 100029China

The present study aimed to explore the potential of artificial intelligence(AI)methodology based on magnetic resonance(MR)images to aid in the management of prostate cancer(PCa).To this end,we reviewed and summarized the studies comparing the diagnostic and predictive performance for PCa between AI and common clinical assessment methods based on MR images and/or clinical characteristics,thereby investigating whether AI methods are generally superior to common clinical assessment methods for the diagnosis and prediction fields of PCa.First,we found that,in the included studies of the present study,AI methods were generally equal to or better than the clinical assessment methods for the risk assessment of PCa,such as risk stratification of prostate lesions and the prediction of therapeutic outcomes or PCa progression.In particular,for the diagnosis of clinically significant PCa,the AI methods achieved a higher summary receiver operator characteristic curve(SROC-AUC)than that of the clinical assessment methods(0.87 vs.0.82).For the prediction of adverse pathology,the AI methods also achieved a higher SROC-AUC than that of the clinical assessment methods(0.86 vs.0.75).Second,as revealed by the radiomics quality score(RQS),the studies included in the present study presented a relatively high total average RQS of 15.2(11.0–20.0).Further,the scores of the individual RQS elements implied that the AI models in these studies were constructed with relatively perfect and standard radiomics processes,but the exact generalizability and clinical practicality of the AI models should be further validated using higher levels of evidence,such as prospective studies and open-testing datasets.

关键词： Clinically significant prostate cancer Adverse pathology Radiomics quality score Artificial intelligence Magnetic resonance imaging

MIL-100(V) derived porous vanadium oxide/carbon microspheres with oxygen defects and intercalated water molecules as high-performance cathode for aqueous zinc ion battery

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Journal of Energy Chemistry 2024年第3期90卷 578-589,I0013页

作者： Yuexin Liu jian Huang Xiaoyu Li Jiajia Li Jinhu Yang Kefeng cai Shanghai Key Laboratory of Development and Application for Metal-Functional Materials Key Laboratory of Advanced Civil Engineering MaterialsMinistry of EducationSchool of Materials Science&EngineeringTongji UniversityShanghai 201804China State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 201800China Research Center for Translational Medicine East HospitalTongji University School of MedicineShanghai 200092China

The development of aqueous zinc ion battery cathode materials with high capacity and high magnification is still a challenge.Herein,porous vanadium oxide/carbon(p-VO_(x)@C,mainly VO_(2) with a small amount of V_(2)O_(3)) core/shell microspheres with oxygen vacancies are facilely fabricated by using a vanadium-based metal-organic framework(MIL-100(V)) as a sacrificial template.This unique structure can improve the conductivity of the VO_(x),accelerate electrolyte diffusion,and suppress structural collapse during circulation.Subsequently,H_(2)O molecules are introduced into the interlayer of VO_(x) through a highly efficient in-situ electrochemical activation process,facilitating the intercalation and diffusion of zinc ions.After the activation,an optimal sample exhibits a high specific capacity of 464.3 mA h g^(-1) at0.2 A g^(-1) and 395.2 mA h g^(-1) at 10 A g^(-1),indicating excellent rate performance.Moreover,the optimal sample maintains a capacity retention of about 89.3% after 2500 cycles at 10 A g^(-1).Density functional theory calculation demonstrates that the presence of oxygen vacancies and intercalated water molecules can significantly reduce the diffusion barrier for zinc ions.In addition,it is proved that the storage of zinc ions in the cathode is achieved by reversible intercalation/extraction during the charge and discharge process through various ex-situ analysis technologies.This work demonstrates that the p-VO_(x)@C has great potential for applications in aqueous ZIBs after electrochemical activation.

关键词： Metal-organic frameworks Vanadium oxide Carbon Zn-ion batteries Electrochemical activation

Changes of China’s Status in the Global System and Its Influencing Factors:A Multiple Contact Networks Perspective

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Chinese Geographical Science 2024年第2期34卷 265-279页

作者： LIU jian LIU Jibin YANG Qingshan cai Sikai LIU Jie School of Geographical Sciences Northeast Normal UniversityChangchun 130024China Key Laboratory of Geographical Processes and Ecological Security of Changbai Mountains Ministry of EducationChangchun 130024China School of Architecture and Planning Jilin Jianzhu UniversityChangchun 130118China School of Geographical Sciences Liaoning Normal UniversityDalian 116029China

Clarifying China’s position in the global system is an important logical basis for developing national diplomacy.Although much research has been done on China’s development status,most studies have been based on country comparisons or institutional en-vironment.In today’s networked era in which the global economy,trade,personnel,and information are closely connected,studies on China’s global position and its status changes and influencing factors in multiple contact networks are still insufficient.In this study,from the perspective of diverse global contact networks,we constructed economic,cultural,and political influence indices to explore the changes and influencing factors on China’s status in the global system from 2005 to 2018.The results show that during the study period,China’s global influence in the fields of economic ties,cultural exchanges,and political contacts increased significantly,but its influ-ence in the fields of cultural exchanges and political contacts lagged far economic ties.The pattern of China’s economic influence on various economies around the world has shown a transformation from an‘upright pyramid’to an‘inverted pyramid’structure.The proportion of these economies in low-influence zones has decreased from more than 60%in 2005 to less than 20%in 2018.China’s cultural and political influence on various economies around the world has increased significantly;however,for the former,the percentage of high-influence areas is still less than 20%,whereas for the latter the percentage of these economies in medium-and high-influence areas is still less than 50%.Analyses such as a scatter plot matrix show that geographical proximity,economic globalization,close cooperation with developing countries,and a proactive and peaceful foreign policy are important factors in improving China’s status in the diverse global network system.

关键词： global system economic ties cultural exchanges political contacts multiple contact networks China’s status

Safety and efficacy of transcatheter arterial embolization in autosomal dominant polycystic kidney patients with gross hematuria: Six case reports

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World Journal of Clinical Cases 2024年第11期12卷 1954-1959页

作者： Wei-Fan Sui Yun-Xin Duan jian-Yun Li Wei-Bin shao jian-Hua Fu Department of Interventional Radiology Zhenjiang First People's HospitalZhenjiang 212000Jiangsu ProvinceChina Department of Nephrology Zhenjiang First People’s HospitalZhenjiang 212000Jiangsu ProvinceChina

BACKGROUND To retrospectively report the safety and efficacy of renal transcatheter arterial embolization for treating autosomal dominant polycystic kidney disease(ADPKD)patients with gross hematuria.CASE SUMMARY The purpose of this study is to retrospectively report the safety and efficacy of renal transcatheter arterial embolization for treating ADPKD patients with gross hematuria.Materials and methods:During the period from January 2018 to December 2019,renal transcatheter arterial embolization was carried out on 6 patients with polycystic kidneys and gross hematuria.Renal arteriography was performed first,and then we determined the location of the hemorrhage and performed embolization under digital subtraction angiography monitoring.Improvements in routine blood test results,routine urine test results,urine color and postoperative reactions were observed and analyzed.Results:Renal transcatheter arterial embolization was successfully conducted in 6 patients.The indices of 5 patients and the color of gross hematuria improved after surgery compared with before surgery.No severe complication reactions occurred.CONCLUSION For autosomal dominant polycystic kidney syndrome patients with gross hematuria,transcatheter arterial embolization was safe and effective.

关键词： Renal artery Autosomal dominant polycystic kidney disease Gross hematuria Interventional radiology Embolization Case report

Application of neoadjuvant chemoradiotherapy and neoadjuvant chemotherapy in curative surgery for esophageal cancer:A metaanalysis

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World Journal of Gastrointestinal Oncology 2024年第1期16卷 214-233页

作者： Mao-Xiu Yuan Qi-Gui cai Zhen-Yang Zhang jian-Zhong Zhou cai-Yun Lan jiang-Bo Lin The Graduate School Fujian Medical UniversityFuzhou 350000Fujian ProvinceChina Department of Thoracic Surgery Affiliated Hospital of Jinggangshan UniversityJi’an 343000Jiangxi ProvinceChina Department of Thoracic Surgery Fujian Medical University Union HospitalFuzhou 350000Fujian ProvinceChina

BACKGROUND The effectiveness of neoadjuvant therapy in esophageal cancer(EC)treatment is still a subject of debate.AIM To compare the clinical efficacy and toxic side effects between neoadjuvant chemoradiotherapy(nCRT)and neoadjuvant chemotherapy(nCT)for locally advanced EC(LAEC).METHODS A comprehensive search was conducted using multiple databases,including PubMed,EMBASE,MEDLINE,Science Direct,The Cochrane Library,China National Knowledge Infrastructure,Wanfang Database,Chinese Science and Technology Journal Database,and Chinese Biomedical Literature Database Article.Studies up to December 2022 comparing nCRT and nCT in patients with EC were selected.RESULTS The analysis revealed significant differences between nCRT and nCT in terms of disease-free survival.The results indicated that nCRT provided better outcomes in terms of the 3-year overall survival rate(OSR)[odds ratio(OR)=0.95],complete response rate(OR=3.15),and R0 clearance rate(CR)(OR=2.25).However,nCT demonstrated a better 5-year OSR(OR=1.02)than nCRT.Moreover,when compared to nCRT,nCT showed reduced risks of cardiac complications(OR=1.15)and pulmonary complications(OR=1.30).CONCLUSION Overall,both nCRT and nCT were effective in terms of survival outcomes for LAEC.However,nCT exhibited better performance in terms of postoperative complications.

关键词： Esophageal cancer Neoadjuvant chemoradiotherapy Radical resection for esophageal cancer Neoadjuvant chemotherapy Meta-analysis

Interface strengthening for thermal sprayed WC-10Co4Cr coating subjected to pulsed magnetic treatment

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Rare Metals 2024年第2期43卷 780-795页

作者： Cheng-Kai Qian Qu Liu Heng Wang Ke-jian Li Zhi-Peng cai Department of Mechanical Engineering Tsinghua UniversityBeijing100084China Tianjin Research Institute for Advanced Equipment Tsinghua UniversityTianjin300304China State Key Laboratory of Tribology in Advanced Equipment Tsinghua UniversityBeijing100084China

The reliability of the coated industry components demands ideal fatigue properties of the coating,and it is mainly determined by the performance of the interfaces.In this study,pulsed magnetic treatment(PMT)was applied to the thermal sprayed WC-10Co4Cr coating,and the fatigue lifetime of the coated bolt increased by 219.82%under an imitation of the operating mode condition.Scratch tests further proved that both the adhesion and cohesion strength were improved after PMT,and they benefit from the interface strengthening effects.The formation of coherent WC/Co interfaces was characterized by in-situ transmission electron microscopy(TEM),and the molecular dynamic simulations indicate that the work of separation of these interfaces is much higher than the original disordered ones.Residual stress was relaxed and distributed more homogeneously after PMT,and it mainly contributes to the coating/substrate strengthening.This work provides a new post-treatment method focusing on the interfaces in the WC-based coating and gives insight into its mechanism so that it is hopeful to be applied to other kinds of coatings.

关键词： Cemented carbide coating Pulsed magnetic treatment Interface strengthening Fatigue properties Adhesion strength