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Tuning Structural and Electronic Configuration of FeN_(4) via External S for Enhanced Oxygen Reduction Reaction

Energy & Environmental Materials 2024年第2期7卷 93-101页

作者： Shidong li lixue xia Jiantao li Zhuo Chen wei Zhang Jiexin Zhu Ruohan Yu Fang liu Sungsik Lee Yan Zhao liang Zhou liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Foshan xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Foshan 528200China Chemical Sciences and Engineering Division Argonne National Laboratory9700 South Cass AvenueLemontIL 60439USA NRC(Nanostructure Research Centre) Wuhan University of TechnologyWuhan 430070China X-ray Science Division Advanced Photon SourcesArgonne National Laboratory9700 South CassAvenueLemontIL 60439USA State Key Laboratory of Silicate Materials for Architectures International School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070China The Institute of Technological Sciences Wuhan UniversityWuhan 430072China Hubei Longzhong Laboratory Xiangyang 441000China

The Fe-N-C material represents an attractive oxygen reduction reaction electrocatalyst,and the FeN_(4)moiety has been identified as a very competitive catalytic active *** tuning of the coordination structure of FeN_(4)has an essential impact on the catalytic ***,we construct a sulfur-modified Fe-N-C catalyst with controllable local coordination environment,where the Fe is coordinated with four in-plane N and an axial external *** external S atom affects not only the electron distribution but also the spin state of Fe in the FeN_(4)active *** appearance of higher valence states and spin states for Fe demonstrates the increase in unpaired *** the above characteristics,the adsorption and desorption of the reactants at FeN_(4)active sites are optimized,thus promoting the oxygen reduction reaction *** work explores the key point in electronic configuration and coordination environment tuning of FeN_(4)through S doping and provides new insight into the construction of M-N-C-based oxygen reduction reaction catalysts.

关键词： coordination structure electronic configuration FeN_(4)moiety oxygen reduction reaction sulfur doping

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Visible-light-Mediated Photocatalyst-Free Hydroacylation of Azodicarboxylic Acid Derivatives with 4-Acyl-1,4-dihydropyridines

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Chinese Journal of Chemistry 2024年第11期42卷 1230-1236页

作者： li liu Jing Wang xiaoying Feng Kun Xu wei liu xia Peng Hongguang Du Jiajing Tan Department of Organic Chemistry College of ChemistryBeijing University of Chemical TechnologyBeijing100029 China Sinopec Beijing Research Institute of Chemical Industry Beijing100013 China Faculty of Environment and life Beijing University of TechnologyBeijing100124 China

A visible-light-enabled,photocatalyst-free hydroacylation reaction of azodicarboxylic acid derivatives was *** radical conjugate addition(RCA)protocol relied on the dual role of 4-acyl-1,4-dihydropyridine(acyl-DHP)reagents that besides being as radical reservoirs,they also enabled the conversion of radical adducts to anion intermediates via ***“catalyst-oxidant-additive free”conditions,a wide range of structurally different acyl hydrazide products were readily obtained in 56%—99%*** utility of this transformation was further demonstrated by the scale-up synthesis and downstream derivatization.

关键词： Azo compounds Radicals Acylation 4-Acyl-1,4-dihydropyridine Photochemistry

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Adiposity in Chinese people with type 1 diabetes

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World Journal of Diabetes 2024年第7期15卷 1404-1408页

作者： Nian-wei Wu xia-Fei Lyu Zhen-Mei An She-Yu li Department of Endocrinology and Metabolism West China HospitalSichuan UniversityChengdu 610041Sichuan ProvinceChina Department of Radiology West China HospitalSichuan UniversityChengdu 610041Sichuan ProvinceChina Department of Guideline and Rapid Recommendation Chinese Evidence-based Medicine CenterCochrane China Center and MAGIC China CenterWest China HospitalSichuan UniversityChengdu 610041Sichuan ProvinceChina

Adiposity,synonymous with obesity,is prevalent among both children and adults with type 1 diabetes in *** literature underscored the pathophysiological and socioeconomic factors associated with adiposity,and consistently highlighted its impact on cardiovascular,kidney,and metabolic diseases among Chinese individuals with type 1 *** and managing adiposity in individuals with type 1 diabetes are complicated and entail comprehensive approaches including lifestyle modifications,cognitive-behavioral therapy,insulin dose titration,and other diabetes treatment *** condition calls for coordination among policymakers,researchers,clinicians,and patients.

关键词： Type 1 diabetes China Metabolic syndrome Obesity Anti-obesity medications

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Evaluation of the clinical effects of atropine in combination with remifentanil in children undergoing surgery for acute appendicitis

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World Journal of Gastrointestinal Surgery 2024年第7期16卷 2065-2072页

作者： Yu-Juan li Yong-Yan Chen xia-Lan lin wei-Zhi Zhang Department of Anesthesiology Shanxi Provincial Children’s HospitalTaiyuan 030013Shanxi ProvinceChina

BACKGROUND Acute appendicitis(AA)is the most common cause of acute abdomen in *** significantly influences the surgical treatment of AA in children,making the scientific and effective selection of anesthetics *** To assess the clinical effect of atropine(ATR)in combination with remifentanil(REMI)in children undergoing surgery for *** In total,108 cases of pediatric AA treated between May 2020 and May 2023 were selected,58 of which received ATR+REMI[research group(RG)]and 50 who received REMI[control group(CG)].Comparative analyses were conducted on the time to loss of eyelash reflex,pain resolution time,recovery time from anesthesia,incidence of adverse events(AEs;respiratory depression,hypoxemia,bradycardia,nausea and vomiting,and hypotension),intraoperative responses(head shaking,limb activity,orientation recovery,safe departure time from the operating room),hemodynamic parameters[oxygen saturation(SPO2),mean arterial pressure,heart rate,and respiratory rate],postoperative sedation score(Ramsay score),and pain level[the Face,Legs,Activity,Cry,Consolability(FLACC)Behavioral Scale].RESULTS Compared with the CG,the RG showed significantly shorter time to loss of eyelash reflex,pain resolution,recovery from anesthesia,and safe departure from the operating ***,the incidence rates of overall AEs(head shaking,limb activity,etc.)were lower,and influences on intraoperative hemodynamic parameters and stress response indexes were *** Ramsay score at 30 min after extubation and the FLACC score at 60 min after extubation were significantly lower in the RG than in the *** ATR+REMI is superior to REMI alone in children undergoing AA surgery,with a lower incidence of AEs,fewer influences on hemodynamics and stress responses,and better post-anesthesia recovery.

关键词： Atropine Remifentanil Pediatric acute appendicitis Surgery Clinical efficacy

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X-box binding protein 1 caused an imbalance in pyroptosis and mitophagy in immature rats with di-(2-ethylhexyl)phthalate-induced testis toxicity

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Genes & Diseases 2024年第2期11卷 935-951页

作者： Yifan Hong xiazhu Zhou Qi li Jing Chen Yuexin wei Chunlan Long lianju Shen xiangqin Zheng Dinggang li xia Wang Chenjun Yu Shengde Wu Guanghui wei Department of Urology Children's Hospital of Chongqing Medical UniversityChongqing 400014China Pediatric Research Institute Children's Hospital of Chongqing Medical UniversityChongqing 400014China Chongqing Key Laboratory of Children Urogenital Development and Tissue Engineering Children's Hospital of Chongqing Medical UniversityChongqing 400014China Chongqing Key Laboratory of Pediatrics Children's Hospital of Chongqing Medical UniversityChongqing 400014China ministry of Education Key Laboratory of Child Development and Disorders Children's Hospital of Chongqing Medical UniversityChongqing 400014China National Clinical Research Center for Child Health and Disorders Children's Hospital of Chongqing Medical UniversityChongqing 400014China China International Science and Technology Cooperation Base of Child Development and Critical Disorders Children's Hospital of Chongqing Medical UniversityChongqing 400014China

As a widely used plasticizer,di-(2-ethylhexyl)phthalate(DEHP)is known to induce significant testicular ***,the potential mechanism and effects of pubertal exposure to DEHP on testis development remain *** vivo,postnatal day(PND)21 male rats were gavaged with 0,250,and 500 mg/kg DEHP for ten *** to the seminiferous epithelium and disturbed spermatogenesis were observed after DEHP ***,oxidative stress-induced injury and pyroptosis were *** endoplasmic reticulum(ER)stress and mitophagy were involved in this *** phthalate(MEHP)was used as the biometabolite of DEHP in *** GC-1 and GC-2 cell lines were exposed to 0,100μM,200μM,and 400μM MEHP for 24 *** oxygen species(ROS)generation,oxidative stress damage,ER stress,mitophagy,and pyroptosis were significantly increased after MEHP *** ultrastructure of the ER and mitochondria was destroyed.X-box binding protein 1(XBP1)was observed to be activated and translocated into the *** generation was inhibited by *** levels of antioxidative stress,ER stress,mitophagy,and pyroptosis were decreased as *** the administration of the ER stress inhibitor 4-phenyl-butyric acid,both mitophagy and pyroptosis were ***-induced XBP1 down-regulation decreased the levels of mitophagy and *** equilibrium between pyroptosis and mitophagy was disturbed by XBP1 *** summary,our findings confirmed that DEHP induced a ROS-mediated imbalance in pyroptosis and mitophagy in immature rat testes via ***,XBP1 might be the key target in DEHP-related testis dysfunction.

关键词： DEHP Mitophagy Pyroptosis Testicular development XBP1

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Subnanometric bimetallic Pt-Pd clusters in zeolites for efficient hydrogen production and selective tandem hydrogenation of nitroarenes

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Science China Chemistry 2024年第9期67卷 2911-2917页

作者： Jiafu li Tao Cai Yanran Feng xia.liu Ning Wang Qiming Sun Institute of Sustainable Energy and Resources College of Chemistry and Chemical EngineeringKey Laboratory of Shandong Provincial Universities for Functional Molecules and MaterialsQingdao UniversityQingdao 266071China Innovation Center for Chemical Sciences College of ChemistryChemical Engineering and Materials ScienceJiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123China

The solvolysis of ammonia borane(AB)and the hydrogenation of nitroarenes represent significant reactions for hydrogen generation and value-added chemical *** strategic engineering of the catalysts is imperative for surmounting obstacles associated with their stability and catalytic *** this work,subnanometric bimetallic Pt–Pd clusters were encapsulated within silicalite-1(S-1)zeolites through a ligand-protected in-situ hydrothermal synthesis *** synergetic effect of bimetallic composition and zeolite confinement markedly enhances the catalytic performance of representative Pt_(0.5)Pd_(0.5)@S-1-H catalyst,affording exceptional turnover frequency(TOF)values of 1,043 and 573 mol_(H_(2))mol_(metal)^(-1)min^(-1)for AB hydrolysis and methanolysis at ambient conditions,respectively,surpassing most of the state-of-the-art Pt-based *** and isotopic experiments reveal that the bimetallic catalytic system remarkably boosts the O-H cleavage of water,thereby facilitating the H_(2) production from AB ***,a conspicuous synergistic effect is demonstrated in the shape-selective tandem hydrogenation of nitroarenes,with the bimetallic catalyst facilitating both AB hydrolysis and nitroarene hydrogenation,giving a high TOF value of 1,260 h^(-1)under atmospheric *** study not only demonstrates the effectiveness of bimetallic nanocatalysts encapsulated in zeolites for hydrogen production from chemical hydrogen storage materials,but also paves the way for the design of catalysts with multifunctional active sites capable of synergistically promoting tandem catalytic processes.

关键词： subnanometer bimetallic cluster zeolite synergistic effect ammonia borane solvolysis selective tandem hydrogenation

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Moderate Deviations for Parameter Estimation in the Fractional Ornstein–Uhlenbeck Processes with Periodic Mean

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Acta Mathematica Sinica,English Series 2024年第5期40卷 1308-1324页

作者： Hui JIANG Shi min li wei Gang WANG School of Mathematics Nanjing University of Aeronautics and AstronauticsNanjing 210016P.R.China The People's Bank of China Operations Ofice of Nanjing Branch Nanjing 210016P.R.China School of Statistics and Mathematics Zhejiang Gongshang UniversityHangzhou 310018P.R.China

In this paper,we study the asymptotic properties for the drift parameter estimators in the fractional Ornstein-Uhlenbeck process with periodic mean function and long range *** Cremér-type moderate deviations,as well ... 详细信息

关键词： Cramér-type moderate deviation fractional Ornstein-Uhlenbeck process parameter estimation multiple Wiener-Ito integrals

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Influence of surface acidity and chemical valence on low temperature activity over Pt-HSiW/CeO_(2) for catalytic combustion of chlorobenzene

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Journal of Rare Earths 2024年第9期42卷 1693-1703,I0002页

作者： Zhongxian Song Zepeng liu Xuejun Zhang Yanli Mao wei liu Chunxiang Gao Haiyang li xia Zhang Changrui Han Zhenzhen Huang Key Laboratory of Carbon Emission Reduction and Combined Air Pollution Control Technology Faculty of Environmental and Municipal EngineeringHenan University of Urban ConstructionPingdingshan467036China College of Environmental and Safety Engineering Shenyang University of Chemical TechnologyShenyang110142China

Pt-HSiW/CeO_(2) catalysts were prepared for chlorobenzene(CB) catalytic combustion by hydrothermal method at different calcination temperatures,and the effects of the surface acidity and chemical valence on the catalytic activity were *** results show that the catalyst calcined at 450℃(Cat-B)exhibits the outstanding catalytic performance,and the Cat-B catalyst possesses 90% conversion of CB at148℃.The excellent catalytic activity of Cat-B is attributed to more Ce^(3+)/(Ce^(3+)+Ce^(4+)),Pt~0/(Pt^(0)+Pt^(2+)),O_(ads)/(O_(latt)+O_(ads)) and Lewis acid *** degradation mechanism is proposed based on the analysis of the intermediates with the following reaction pathway:chlorobenzene→phenates/benzoquinone→acetate→maleate→CO_(2)+H_(2)O.

关键词： Pt-HSiW/CeO_(2) Catalytic combustion Chlorobenzene Acid sites Rare earths

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Sequence-Controlled Synthesis of Alternating Poly(ester amide)s using Water as Control Agent in One-Pot

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Chinese Journal of Polymer Science 2024年第8期42卷 1015-1020页

作者： Tao liu Fang-Fang Niu Kan Cheng Yu-min xia Bo-Mou Ma Xue-li Wang Jian-Yong Yu Yong He State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai 201620China Innovation Center for Textile Science and Technology Donghua UniversityShanghai 201620China

Poly(ester amide)s(PEAs)attract much attention as a new kind of biodegradable ***,the synthesis of PEAs with sequence-regulated chain structures is still complicated due to the multistep polymerization,high monomer purity,as well as the usage of organic solvents,which greatly inhibits its development and ***,a one-pot strategy without solvent was developed to synthesize the alternating PEA fromα,ω-amino alcohol and dicarboxylic acid by sequential polycondensation,where water was used as the controlling agent for amidation and ***,the amidation and esterification were controlled to proceed in turn by adding or removing water,realizing the one-pot preparation of alternating *** resultant PEA is characterized by^1H-and^(13)C-NMR,and its chain structure is confirmed to be highly quasi-alternating similar to alternating PEAs prepared by classical methods The evaluations from DSC and DMA demonstrate that the properties of quasi-alternating PEA(T_(m)=102℃,ΔH_(m)=30J·g^(-1))are far superior to those of random PEA(T_(m)=72℃,ΔH_(m)<1 J·g^(-1)).

关键词： Biodegradable macromolecules Polymer architectures Sequence-controlled synthesis One-pot polymerization

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Ru-Ni alloy nanosheets as tandem catalysts for electrochemical reduction of nitrate to ammonia

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Nano Research 2024年第6期17卷 4815-4824页

作者： Xingchao You Jiawei Xu Zechao Zhuang Junkai xia Suwen Wang Haiyan wei Yongfu li Yanjiang Cai Hai xiang Bing Yu State Key Laboratory of Subtropical Silviculture Zhejiang A&F UniversityHangzhou 311300China Ecological-Environment&Health College(EEHC) Zhejiang A&F UniversityHangzhou 311300China Jiangsu Key Laboratory of Numerical Simulation of Large Scale Complex Systems and School of Chemistry and Materials Science Nanjing Normal UniversityNanjing 210023China Department of Chemistry Tsinghua UniversityBeijing 100084China Department of Chemical Engineering Columbia UniversityNew YorkNY 10027USA

Developing electrocatalysts that exhibit both high activity and ammonia selectivity for nitrate reduction is a significant and demanding challenge,primarily due to the complex nature of the multiple-electron reduction process *** encouraging approach involves coupling highly active precious metals with transition metals to enhance catalytic performance through ***,we report a ruthenium-nickel alloy catalyst with nanosheets(Ru-Ni NSs)structure that achieves a remarkable ammonia Faradaic efficiency of approximately 95.93%,alongside a yield rate of up to 6.11 g·h^(−1)·cm^(−2).Moreover,the prepared Ru-Ni NSs exhibit exceptional stability during continuous nitrate reduction in a flow reactor for 100 h,maintaining a Faradaic efficiency of approximately 90%and an ammonia yield of 37.4 mg·L^(−1)·h^(−1)using 0.05 M nitrate alkaline *** studies reveal that the catalytic process follows a two-step pathway,in which HONO serves as a migration *** presence of a partially oxidized Ru(002)surface enhances the adsorption of nitrate and facilitates the release of the migration intermediate by adjusting the strength of the electrostatic and covalent interactions between the adsorbate and the surface,*** the other hand,the Ni(111)surface promotes the utilization of the migration intermediate and requires less energy for NH_(3)*** tandem process contributes to a high catalytic activity of Ru-Ni NSs towards nitrate reduction.

关键词： alloy catalyst nitrate reduction ammonia synthesis Faradaic efficiency

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