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Difluoromethyl phenoxathiinium salt: A new general and versatile difluoromethylating reagent with divergent ·CF_(2)H, CF_(2)H^(+), and :CF_(2) reactivities

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Science China Chemistry 2024年第3期67卷 953-962页

作者： Yuan-Qing Gu Hong-Xin Long dan-dan Zhang Mei-Feng ruan Guo-Kai Liu School of Pharmacy Shenzhen University Medical SchoolShenzhen UniversityShenzhen 518055China

Development of practical and versatile electrophilic difluoromethylating reagent is still a grand challenge so far due to its inherent instability or low reactivity.Herein,we report the design and synthesis of difluoromethyl phenoxathiinium tetrafluoroborate(PT-CF_(2)H^(+)BF_(4)^(-)) as a novel difluoromethylating reagent,which proves to be a bench-stable,general,powerful and versatile reagent with divergent·CF_(2)H,CF_(2)H^(+),and:CF_(2) reactivities.Making use of this reagent,we demonstrated a vast array of difluoromethyl radical transfer reactions via diverse pathways involving photocatalyst-free visible-light induction,visible-light photoredox catalysis and visible-light mediation single electron transfer of EDA complex.Moreover,the green and highly effective CF_(2)H^(+) and:CF_(2) transfer reactions were also readily accomplished.

关键词： difluoromethyl phenoxathiinium salt versatile difluoromethylating reagent difluoromethyl radical difluoromthyl cation difluorocarbene

Assembly of peptide nanostructures with controllable sizes

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Nano Research 2024年第1期17卷 151-161页

作者： dan Cheng Fan Jia yun-Bao Jiang Vincent P.Conticello Tao Jiang The MOE Key Laboratory of Spectrochemical Analysis and Instrumentation Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361005China Department of Chemistry Emory UniversityAtlanta 30033USA

Controlled peptide assembly offers significant promise to develop synthetic supramolecular nanostructures to display material and biological properties that mimic protein assemblies in nature.Despite the progress in forming peptide nanostructures of various morphology,there exists a distinct gap between natural and synthetic assembly systems in terms of size control.Constructing nanostructures with a narrow size distribution that can be tuned over a wide range of length-scales is essential for applications that require precise spacing between objects.This approach provides the opportunity to correlate materials and biological properties of interest with assembly size.In this review,we discuss representative endeavors over the past two decades for design of size-controllable peptide nanostructures using tunable building blocks.Other mechanisms for size control,e.g.,molecular frustration,template-directed peptide assembly,and multi-component peptide co-assembly,will also be discussed.We also demonstrate the applicable scopes of these strategies and suggest potential future avenues for scientific advances in this field.

关键词： peptide assembly controllable size template multi-component

Recent progress on mechanisms,principles,and strategies for high-activity and high-stability non-PGM fuel cell catalyst design

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Carbon Energy 2024年第5期6卷 25-52页

作者： Yuping Yuan yun Zheng dan Luo Weibin Qiu Jiantao Wang Xin Wang Zhongwei Chen GRINM(Guangdong)Institute of New Materials Technology FoshanChina Department of Chemical Engineering Waterloo Institute for NanotechnologyWaterloo Institute for Sustainable EnergyUniversity of WaterlooWaterlooOntarioCanada Guangdong Provincial Key Laboratory of Nanophotonic Functional Materials and Devices School of Information and Optoelectronic Science and EngineeringSouth China Normal UniversityGuangdongChina National Power Battery Innovation Center GRINM Group Co.Ltd.BeijingChina

The commercialization of a polymer membrane H2-O2 fuel cell and its widespread use call for the development of cost-effective oxygen reduction reaction(ORR)nonplatinum group metal(NPGM)catalysts.Nevertheless,to meet the requests for the real-world fuel cell application and replacing platinum catalysts,it still needs to address some challenges for NPGM catalysts regarding the sluggish ORR kinetics in the cathode and their poor durability in acidic environment.In response to these issues,numerous efforts have been made to study NPGM catalysts both theoretically and experimentally,developed these into the atomically dispersed coordinated metal-nitrogen-carbon(M-N-C)form over the past decades.In this review,we present a comprehensive summary of recent advancements on NPGM catalysts with high activity and durability.Catalyst design strategies in terms of optimizing active-site density and enhancing catalyst stability against demetalization and carbon corrosion are highlighted.It is also emphasized the importance of understanding the mechanisms and principles behind those strategies through a combination of theoretical modeling and experimental work.Especially,further understanding the mechanisms related to the active-site structure and the formation process of the single-atom active site under pyrolysis conditions is critical for active-site engineering.Optimizing the active-site distance is the basic principle for improving catalyst activity through increasing the catalyst active-site density.Theoretical studies for the catalyst deactivation mechanism and modeling stable active-site structures provide both mechanisms and principles to improve the NPGM catalyst durability.Finally,currently remained challenges and perspectives in the future on designing high-performance atomically dispersed NPGM catalysts toward fuel cell application are discussed.

关键词： batteries electrocatalysis energy storage and conversion fuel cells

Impact of short-term ambient air pollution exposure on the risk of severe COVID-19

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Journal of Environmental Sciences 2024年第1期135卷 610-618页

作者： Baihuan Feng Jiangshan Lian Fei Yu dan Zhang Weizhen Chen QiWang Yifei Shen Guoliang Xie Ruonan Wang yun Teng Bin Lou Shufa Zheng Yida Yang Yu Chen Department of Laboratory Medicine The First Affiliated HospitalZhejiang University School of MedicineHangzhou 310000China Key Laboratory of Clinical In Vitro Diagnostic Techniques of Zhejiang Province Hangzhou 310000China Institute of Laboratory Medicine Zhejiang UniversityHangzhou 310000China Department of Infectious Diseases The First Affiliated HospitalZhejiang University School of MedicineHangzhou 310000China State Key Laboratory for Diagnosis and Treatment of Infectious Diseases National Clinical Research Center for Infectious DiseasesCollaborative Innovation Center for Diagnosis and Treatment of Infectious Diseasesthe First Affiliated HospitalZhejiang University School of MedicineHangzhou 310000China

Ecological studies suggested a link between air pollution and severe COVID-19 outcomes,while studies accounting for individual-level characteristics are limited.In the present study,we aimed to investigate the impact of short-term ambient air pollution exposure on disease severity among a cohort of 569 laboratory confirmed COVID-19 patients admitted to designated hospitals in Zhejiang province,China,from January 17 to March 3,2020,and elucidate the possible biological processes involved using transcriptomics.Compared with mild cases,severe cases had higher proportion of medical conditions as well as unfavorable results in most of the laboratory tests,and manifested higher air pollution exposure levels.Higher exposure to air pollutants was associated with increased risk of severe COVID-19 with odds ratio(OR)of 1.89(95%confidence interval(CI):1.01,3.53),2.35(95%CI:1.20,4.61),2.87(95%CI:1.68,4.91),and 2.01(95%CI:1.10,3.69)for PM_(2.5),PM_(10),NO_(2)and CO,respectively.OR for NO_(2)remained significant in two-pollutant models after adjusting for other pollutants.Transcriptional analysis showed 884 differentially expressed genes which mainly were enriched in virus clearance related biological processes between patients with high and low NO_(2)exposure levels,indicating that compromised immune response might be a potential underlying mechanistic pathway.These findings highlight the impact of shortterm air pollution exposure,particularly for NO_(2),on COVID-19 severity,and emphasize the significance in mitigating the COVID-19 burden of commitments to improve air quality.

关键词： Air pollution COVID-19 Severity Transcriptomics Immune response

Frequency and associated factors of accommodation and non-strabismic binocular vision dysfunction among medical university students

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International Journal of Ophthalmology(English edition) 2024年第2期17卷 374-379页

作者： Jie Cai Wen-Wen Fan yun-Hui Zhong Cai-Lan Wen Xiao-dan Wei Wan-Chen Wei Wan-Yan Xiang Jin-Mao Chen Department of Ophthalmology First Affiliated Hospital of Guangxi Medical UniversityNanning 530021Guangxi Zhuang Autonomous RegionChina Digital and Intelligent Technology Transformation and Application Research Institute of Visual Function Tianjin 300000China Guangxi Medical University Nanning 530021Guangxi Zhuang Autonomous RegionChina

AIM:To investigate the frequency and associated factors of accommodation and non-strabismic binocular vision dysfunction among medical university students.METHODS:Totally 158 student volunteers underwent routine vision examination in the optometry clinic of Guangxi Medical University.Their data were used to identify the different types of accommodation and nonstrabismic binocular vision dysfunction and to determine their frequency.Correlation analysis and logistic regression were used to examine the factors associated with these abnormalities.RESULTS:The results showed that 36.71%of the subjects had accommodation and non-strabismic binocular vision issues,with 8.86%being attributed to accommodation dysfunction and 27.85%to binocular abnormalities.Convergence insufficiency(CI)was the most common abnormality,accounting for 13.29%.Those with these abnormalities experienced higher levels of eyestrain(χ2=69.518,P<0.001).The linear correlations were observed between the difference of binocular spherical equivalent(SE)and the index of horizontal esotropia at a distance(r=0.231,P=0.004)and the asthenopia survey scale(ASS)score(r=0.346,P<0.001).Furthermore,the right eye's SE was inversely correlated with the convergence of positive and negative fusion images at close range(r=-0.321,P<0.001),the convergence of negative fusion images at close range(r=-0.294,P<0.001),the vergence facility(VF;r=-0.234,P=0.003),and the set of negative fusion images at far range(r=-0.237,P=0.003).Logistic regression analysis indicated that gender,age,and the difference in right and binocular SE did not influence the emergence of these abnormalities.CONCLUSION:Binocular vision abnormalities are more prevalent than accommodation dysfunction,with CI being the most frequent type.Greater binocular refractive disparity leads to more severe eyestrain symptoms.

关键词： optometry clinic non-strabismic binocular vision dysfunction college students convergence insufficiency

Application of UiO-66 and its composites for remediation and resource recovery of typical environmental contaminants:a review

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Rare Metals 2024年第6期43卷 2498-2526页

作者： Hui-Min Zhang yun-Long Wang Xin-Feng Zhu Zhen-Zhen Huang dan-dan Pang Kai Wang Chao-Hai Wang Zhong-Xian Song Shi-Qiang Yin Lin-Lin Chang Jin-Hui Zhang School Infirmary Henan University of Urban Construction Faculty of Environmental and Municipal Engineering Henan Key Laboratory of Water Pollution Control and Rehabilitation TechnologyKey Laboratory of Carbon Emission Reduction and Combined Air Pollution Control TechnologyHenan University of Urban Construction School of Resources & Environment Collaborative Innovation Center of Coalbed Methane and Shale Gas for Central Plains Economic RegionHenan Polytechnic University The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of EducationGuangzhou Higher Education Mega CentreSouth China University of Technology

UiO-66 series metal-organic framework materials（MOFs） are typical porous materials assembled by Zr4+with a large mass-to-nucleus ratio and terephthalic acid ligands,which form tetrahedral and octahedral cages arranged in a periodic triangular window pattern.Due to the strong interaction between Zr and O,UiO-66 series MOFs exhibit high thermal stability,structural stability,and chemical stability.This article mainly reviews the applications of UiO-66 and its composites in adsorption,photocatalysis,and resource utilization,while exploring the harm of pollutants to human health and the environment.In the first part,the differences in adsorption and removal mechanisms of liquid organic pollutants,heavy metals,and volatile organic compounds（VOCs） are investigated.The results show that organic pollutants are mainly removed by physical adsorption,electrostatic interactions,hydrogen bonding,and π-π interactions,while heavy metals are mainly removed by chemical adsorption,electrostatic interactions,reduction,and chelation.VOCs are mainly removed by the pore volume and pore size structure of the material.Heterojunction catalysis can achieve non-toxic treatment of pollutants,and this study mainly focuses on UiO-based composite materials constructed by strategies such as semiconductor composites,ion doping,and metal/dye encapsulation.In the second part,the synergistic effect between the components of UiO-based composite materials promotes the oriented and rapid separation and transfer of earriers at the material interface,thereby promoting the generation of active species such as h+,·O2-and ·OH,and achieving rapid degradation of pollutants and detoxification of heavy metals.In the third part,heterojunctions can realize the resource utilization of pollutants in water and air,producing energy-type substances such as hydrogen and methanol while solving environmental problems.In addition,this article also summarizes the harm of common typical pollutants to the environment and human health.Finally,the development prospects and un

关键词： UiO Adsorption Photocatalysis Environmental pollution Resource recovery

Holographic Polymer Nanocomposites with High Refractive Index Modulation by Doping Liquid Crystal E6M

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Chinese Journal of Polymer Science 2024年第7期42卷 926-935,I0006页

作者： Meng-yun Wang Yue Zhang dan Wang Ming Yao Yi-Xuan Wang Xing-Ping Zhou Hai-Yan Peng Xiao-Lin Xie Key Laboratory of Material Chemistry for Energy Conversion and Storage Ministry of EducationSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan430074China State Key Laboratory of Materials Processing and Die&Mould Technology Huazhong University of Science and TechnologyWuhan430074China National Anti-counterfeit Engineering Research Center Huazhong University of Science and TechnologyWuhan430074China

Holographic optical elements(HOEs)based on polymer composites have become a research hot spot in recent years for augmented reality(AR)due to the significant improvement of optical performance,dynamic range,ease of processing and high yield rate.Nevertheless,it remains a formidable challenge to obtain a large field of view(FOV)and brightness due to the limited refractive index modulation.Herein,we report an effective method to tackle the challenge by doping an epoxy liquid crystal termed E6M,which enables a large refractive index modulation of 0.050@633 nm and low haze of 5.0%at a doping concentration of 5 wt%.This achievement may be ascribed to the improved molecular ordering of liquid crystals within the holographic polymer composites.The high refractive index modulation can endow transmission-type holographic polymer composites with a high diffraction efficiency of 96.2%at a small thickness of 5μm,which would promise the design of thin and lightweight AR devices.

关键词： Polymer nanocomposites Holography AR/VR Refractive index modulation Liquid crystal

Epidemiological Surveillance: Genetic Diversity of Rotavirus Group A in the Pearl River Delta, Guangdong, China in 2019

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Biomedical and Environmental Sciences 2024年第3期37卷 278-293页

作者： JIANG Jie Ying LIANG dan WANG Li XIAO yun LIANG Yu Feng KE Bi Xia SU Juan XIAO Hong WANG Tao ZOU Min LI Hong Jian KE Chang Wen School of Public Health Shantou UniversityShantou 515063GuangdongChina Guangdong Provincial Center for Disease Control and Prevention Guangdong Workstation for Emerging Infectious Disease Control and PreventionGuangzhou 511430GuangdongChina Guangdong Provincial Key Laboratory of Virology Institute of Medical MicrobiologyJinan UniversityGuangzhou 510632GuangdongChina School of Public Health Sun Yat-sen UniversityGuangzhou 510275GuangdongChina School of Public Health Southern Medical UniversityGuangzhou 510515GuangdongChina Shantou University Medical College Shantou 515041GuangdongChina

Objective This study aimed to understand the epidemic status and phylogenetic relationships of rotavirus group A(RVA)in the Pearl River Delta region of Guangdong Province,China.Methods This study included individuals aged 28 days–85 years.A total of 706 stool samples from patients with acute gastroenteritis collected between January 2019 and January 2020 were analyzed for 17 causative pathogens,including RVA,using a Gastrointestinal Pathogen Panel,followed by genotyping,virus isolation,and complete sequencing to assess the genetic diversity of RVA.Results The overall RVA infection rate was 14.59%(103/706),with an irregular epidemiological pattern.The proportion of co-infection with RVA and other pathogens was 39.81%(41/103).Acute gastroenteritis is highly prevalent in young children aged 0–1 year,and RVA is the key pathogen circulating in patients 6–10 months of age with diarrhea.G9P[8](58.25%,60/103)was found to be the predominant genotype in the RVA strains,and the 41 RVA-positive strains that were successfully sequenced belonged to three different RVA genotypes in the phylogenetic analysis.Recombination analysis showed that gene reassortment events,selection pressure,codon usage bias,gene polymorphism,and post-translational modifications(PTMs)occurred in the G9P[8]and G3P[8]strains.Conclusion This study provides molecular evidence of RVA prevalence in the Pearl River Delta region of China,further enriching the existing information on its genetics and evolutionary characteristics and suggesting the emergence of genetic diversity.Strengthening the surveillance of genotypic changes and gene reassortment in RVA strains is essential for further research and a better understanding of strain variations for further vaccine development.

关键词： Infectious diarrheal disease Rotavirus Phylogenetic analysis Gene rearrangement Codon usage bias Genetic diversity

Role of deubiquitinase JOSD2 in the pathogenesis of esophageal squamous cell carcinoma

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World Journal of Gastroenterology 2024年第6期30卷 565-578页

作者： Wen-Peng Wang dan Shi Duo yun Jun Hu Jie-Fu Wang Jia Liu Yan-Peng Yang Ming-Rui Li Jun-FengWang Da-Lu Kong Department of Colorectal Oncology Tianjin Medical University Cancer Institute and HospitalNational Clinical Research Center for CancerTianjin’s Clinical Research Center for CancerKey Laboratory of Cancer Prevention and TherapyTianjin 300060China Department of Gastrointestinal Surgery Tianjin Nan Kai HospitalTianjin Medical UniversityTianjin Key Laboratory of Acute Abdomen Disease Associated Organ Injury and ITCWM RepairInstitute of Integrative Medicine for Acute Abdominal DiseasesTianjin 300100China Department of Oncology The First Hospital of HohhotHohhot 010000Inner Mongolia Autonomous RegionChina Department of Endocrinology Dazhou Central HospitalDazhou 635000Sichuan ProvinceChina

BACKGROUND Esophageal squamous cell carcinoma(ESCC)is a deadly malignancy with limited treatment options.Deubiquitinases(DUBs)have been confirmed to play a crucial role in the development of malignant tumors.JOSD2 is a DUB involved in con-trolling protein deubiquitination and influencing critical cellular processes in cancer.AIM To investigate the impact of JOSD2 on the progression of ESCC.METHODS Bioinformatic analyses were employed to explore the expression,prognosis,and enriched pathways associated with JOSD2 in ESCC.Lentiviral transduction was utilized to manipulate JOSD2 expression in ESCC cell lines(KYSE30 and RESULTS )Preliminary research indicated that JOSD2 was highly expressed in ESCC tissues,which was associated with poor prognosis.Further analysis demonstrated that JOSD2 was upregulated in ESCC cell lines compared to normal esophageal cells.JOSD2 knockdown inhibited ESCC cell activity,including proliferation and colony-forming ability.Moreover,JOSD2 knockdown decreased the drug resistance and migration of ESCC cells,while JOSD2 overexpression enhanced these phenotypes.In vivo xenograft assays further confirmed that JOSD2 promoted tumor proliferation and drug resistance in ESCC.Mechanistically,JOSD2 appears to activate the MAPK/ERK and PI3K/AKT signaling pathways.Mass spectrometry was used to identify crucial substrate proteins that interact with JOSD2,which identified the four primary proteins that bind to JOSD2,namely USP47,IGKV2D-29,HSP90AB1,and PRMT5.CONCLUSION JOSD2 plays a crucial role in enhancing the proliferation,migration,and drug resistance of ESCC,suggesting that JOSD2 is a potential therapeutic target in ESCC.

关键词： Esophageal squamous cell carcinoma JOSD2 Ubiquitination Biomarker Targeted therapy Drug resistance