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Chinese Journal of Chemistry 2024年第17期42卷 1993-1998页

作者： Chen Zhou Mengfu Dai Xiaoyu Yin Mingyue Zhang Weijin Gu Liang-An Chen jiangsu Collaborative Innovation Center of Biomedical Functional Materials Jiangsu Key Laboratory of New Power BatteriesSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjingJiangsu 210023China

The stereochemical synthesis of highly substituted Danishefsky-type dienes remains unsolved in organic *** describe a simple and efficient approach for the stereoselective synthesis of Danishefsky-type trisubstituted dienes from readily available propargylic esters via Pd-catalyzed dienylation reaction through the key intermediate metallacyclobutene in a regio-,chemo-and stereoselective *** method facilitates a broad range of challenging trisubstituted dienes with a high level of stereocontrol.

关键词： Propargylic ester Dienylation Diene Stereoselectivity Cycloaddition Palladium β-H elimination Regioselectivity

Selective photosynthesis of Z-olefins through crystalline metal-organic cage-initiated expeditious cascade reactions

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Carbon Energy 2024年第3期6卷 118-131页

作者： Jia-Ni Lu Yunze Huang Yuan-Sheng Xia Long-Zhang Dong Lei Zhang Jing-Jing Liu Lan-Gui Xie Jiang Liu Ya-Qian Lan jiangsu key laboratory of new power batteries School of Chemistry and Materials ScienceJiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNanjingChina School of Chemistry South China Normal UniversityGuangzhouChina

The semi-hydrogenation of alkyne to form Z-olefins with high conversion and high selectivity is still a huge challenge in the chemical ***,flammable and explosive hydrogen as the common hydrogen source of this reaction increases the cost and danger of industrial ***,we connect the photocatalytic hydrogen evolution reaction and the semihydrogenation reaction of alkynes in series and successfully realize the high selective production of Z-alkenes using low-cost,safe,and green water as the proton *** the cascade reaction,a series of isomorphic metal–organic cage catalysts(Co_(x)Zn_(8−x)L_(6),x=0,3,4,5,and 8)are designed and synthesized to improve the yield of the photocatalytic hydrogen *** them,Co_(5)Zn_(3)L_(6) shows the highest photocatalytic activity,with a H_(2) generation rate of 8.81 mmol g^(−1) h^(−1).Then,Co_(5)Zn_(3)L_(6) is further applied in the above tandem reaction to efficiently reduce alkynes to Z-alkenes under ambient conditions,which can reach high conversion of>98%and high selectivity of>99%,and maintain original catalytic activity after multiple ***“one-pot”tandem reaction can achieve a highly selective and safe stepwise conversion from water into hydrogen into Z-olefins under mild reaction conditions.

关键词： alkyne semi-hydrogenation hydrogen evolution reaction metal-organic cages photocatalysis Z-olefins

Synthesis of carbon dots with predictable photoluminescence by the aid of machine learning

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Nano Research 2024年第3期17卷 1984-1989页

作者： Chenyu Xing Gaoyu Chen Xia Zhu Jiakun An Jianchun Bao Xuan Wang Xiuqing Zhou Xiuli Du Xiangxing Xu jiangsu key laboratory of Biofunctional Materials Jiangsu Key Laboratory of New Power BatteriesSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China School of Mathematical Sciences Nanjing Normal UniversityNanjing 210023China State key laboratory of Coordination Chemistry School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210093China

Carbon dots(CDs)have wide application potentials in optoelectronic devices,biology,medicine,chemical sensors,and quantum techniques due to their excellent fluorescent ***,synthesis of CDs with controllable spectrum is challenging because of the diversity of the CD components and *** this report,machine learning(ML)algorithms were applied to help the synthesis of CDs with predictable photoluminescence(PL)under the excitation wavelengths of 365 and 532 *** combination of precursors was used as the *** PL peaks of the strongest intensity(λ_(s))and the longest wavelength(λ_(l))were used as target *** six investigated ML models,the random forest(RF)model showed outstanding)performance in the prediction of the PL peaks.

关键词： carbon dots(CDs) synthesis photoluminescence(PL) machine learning(ML) PL prediction

Alkaline zinc-based flow battery: chemical stability, morphological evolution, and performance of zinc electrode with ionic liquid

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Frontiers of Materials Science 2024年第1期18卷 113-121页

作者： Tianyong Mao Jing Dai Meiqing Xin Deliang Zeng Zhipeng Xie Jiangxi Province key laboratory of power batteries and Materials Jiangxi University of Science and TechnologyGanzhou 341000China

Zinc-based flow battery is an energy storage technology with good application prospects because of its advantages of abundant raw materials,low cost,and environmental *** chemical stability of zinc electrodes exposed to electrolyte is a very important issue for zinc-based *** paper reports on details of chemical stability of the zinc metal exposed to a series of solutions,as well as the relationship between the morphological evolution of zinc electrodes and their properties in an alkaline *** corrosion of zinc electrodes by the electrolyte will change their surface ***,we observed that chemical corrosion is not the main contributor to the evolution of zinc electrode surface morphology,but the main contributor is the Zn/Zn^(2+)electrode *** morphological evolution of zinc electrodes was controlled by using ionic liquids,1-ethyl-3-methylimidazolium acetate(EMIA),and 1-propylsulfonic-3-methylimidazolium tosylate(PSMIT),and the electrode performance was recorded during the morphological evolution *** was observed that the reversible change of zinc electrode morphology was accompanied by better electrode performance.

关键词： alkaline medium morphological evolution zinc-based flow battery new energy

The manipulation of rectifying contact of Co and nitrogen-doped carbon hierarchical superstructures toward high-performance oxygen reduction reaction

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Carbon Energy 2024年第9期6卷 338-349页

作者： Jing Li Tingyu Lu Yu Fang Guangyao Zhou Mingyi Zhang Huan Pang Jun Yang Yawen Tang Lin Xu jiangsu key laboratory of new power batteries School of Chemistry and Materials ScienceJiangsu Collaborative Innovation Center of Biomedical Functional MaterialsNanjing Normal UniversityNanjingJiangsuChina College of Science Jinling Institute of TechnologyNanjingJiangsuChina key laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbinHeilongjiangChina School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhouJiangsuChina State key laboratory of Multiphase Complex Systems Center of MesoscienceInstitute of Process EngineeringChinese Academy of SciencesBeijingChina

Rational design and construction of oxygen reduction reaction(ORR)electrocatalysts with high activity,good stability,and low price are essential for the practical applications of renewable energy conversion devices,such as metal-air *** modification through constructing metal/semiconductor Schottky heterointerface represents a powerful strategy to enhance the electrochemical ***,we demonstrate a concept of Schottky electrocatalyst composed of uniform Co nanoparticles in situ anchored on the carbon nanotubes aligned on the carbon nanosheets(denoted as Co@N-CNTs/NSs hereafter)toward *** experimental findings and theoretical simulation testify that the rectifying contact could impel the voluntary electron flow from Co to N-CNTs/NSs and create an internal electric field,thereby boosting the electron transfer rate and improving the intrinsic *** a consequence,the Co@N-CNTs/NSs deliver outstanding ORR activity,impressive long-term durability,excellent methanol tolerance,and good performance as the air-cathode in the Zn-air *** design concept of Schottky contact may provide the innovational inspirations for the synthesis of advanced catalysts in sustainable energy conversion fields.

关键词： Co-based electrocatalysts oxygen reduction reaction rectifying contact Zn-air batteries

Synthesis and characterization of iron clusters with an icosahedral [Fe@Fe12]16+ Core

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National Science Review 2024年第4期11卷 123-129页

作者： Gan Xu Yun-Shu Cui Xue-Lian Jiang Cong-Qiao Xu Jun Li Xu-Dong Chen jiangsu Collaborative Innovation Center of Biomedical Functional Materials and jiangsu key laboratory of new power batteries School of Chemistry and Materials Science Nanjing Normal University Department of Chemistry and Guangdong Provincial key laboratory of Catalytic Chemistry Southern University of Science and Technology Department of Chemistry and Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education Tsinghua University State key laboratory of Coordination Chemistry Nanjing University

Iron-metal clusters are crucial in a variety of critical biological and material systems,including metalloenzymes,catalysts,and magnetic storage ***,a synthetic high-nuclear iron cluster has been absent due to the extreme difficulty in stabilizing species with direct iron-iron *** this work,we have synthesized,crystallized,and characterized a（Tp*）4W4S12(Fe@Fe12) cluster(Tp*=tris（3,5-dimethyl-1-pyrazolyl）borate（1-）),which features a rare trideca-nuclear,icosahedral[Fe@Fe12] cluster core with direct multicenter iron-iron bonding between the interstitial iron（Fei） and peripheral irons（Fep）,as well as Fep…Fepferromagnetic *** chemistry studies reveal that the stability of the cluster arises from the 18-electron shell-closing of the [Fe@Fe12]16+core,assisted by its bonding interactions with the peripheral tridentate [（Tp*）WS3]4-ligands which possess both S→Fe donation and spin-polarized Fe-Wσ *** ground-state electron spin is theoretically predicted to be S=32/2 for the *** existence of low oxidation-state（OS～+1.23） iron in this compound may find interesting applications in magnetic storage,spintronics,redox chemistry,and cluster catalysis.

关键词： Fe13 cluster iron-sulfur cluster low-valence iron iron−iron bond high spin complex

Stereoselective synthesis of substituted 1,3-dienes from propargylic esters: electrophilic-metal or redox catalysis?

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Science China Chemistry 2024年第5期67卷 1384-1396页

作者： Mengfu Dai Liangliang Song Liang-An Chen jiangsu Collaborative Innovation Center of Biomedical Functional Materials Jiangsu Key Laboratory of New Power BatteriesSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources International Innovation Center for Forest Chemicals and MaterialsCollege of Chemical EngineeringNanjing Forestry UniversityNanjing 210037China

1,3-Diene architectures are not only widely present in natural products, pharmaceuticals, and functional organic materials but also serve as versatile building blocks to furnish important functionalized molecules in synthetic chemistry due to conjugated repeating C=C units. Accordingly, various strategies to access substituted 1,3-dienes in a stereoselective manner have been developed. However, chemo-, regio-and stereoselective synthesis of highly substituted 1,3-dienes still remains elusive and challenging. Readily available propargylic esters have emerged as an appealing class of synthetic intermediates for accessing functionalized 1,3-dienes, especially challenging tri-or tetrasubstituted variants, via transition-metal catalysis, including electrophilic metal and redox neutral catalysis. This review, for the first time, systematically highlights recent advances in transitionmetal catalyzed synthesis of substituted 1,3-dienes from propargylic esters, discusses the mechanisms and synthetic utilities, and gives the remaining challenges and potential opportunities in this field.

关键词： 1 3-diene propargylic ester Lewis acid redox catalysis transition metal

Manipulating d-d orbital hybridization induced by Mo-doped Co_(9)S_(8) nanorod arrays for high-efficiency water electrolysis

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Journal of Energy Chemistry 2024年第6期93卷 592-600,I0015页

作者： Xue Zhou Jing Li Guangyao Zhou Weiran Huang Yucan Zhang Jun Yang Huan Pang Mingyi Zhang Dongmei Sun Yawen Tang Lin Xu jiangsu key laboratory of new power batteries Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023JiangsuChina 'College of Science Jinling Institute of TechnologyNanjing 211169JiangsuChina State key laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Nanjing IPE Institute of Green Manufacturing Industry Nanjing 211100JiangsuChina School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225009JiangsuChina key laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbin 150025HeilongjiangChina

Precisely refining the electronic structure of electrocatalysts represents a powerful approach to further optimize the electrocatalytic ***,we demonstrate an ingenious d-d orbital hybridization concept to construct Mo-doped Co_(9)S_(8) nanorod arrays aligned on carbon cloth(CC)substrate(abbreviated as Mo-Co_(9)S_(8)@CC hereafter)as a high-efficiency bifunctional electrocatalyst toward water *** has experimentally and theoretically validated that the 4d-3d orbital coupling between Mo dopant and Co site can effectively optimize the H_(2)O activation energy and lower H^(*)adsorption energy barrier,thereby leading to enhanced hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)*** to the unique electronic and geometrical advantages,the optimized Mo-Co_(9)S_(8)@CC with appropriate Mo content exhibits outstanding bifunctional performance in alkaline solution,with the overpotentials of 75 and 234 mV for the delivery of a current density of 10 mA cm^(-2),small Tafel slopes of 53.8 and 39.9 mV dec~(-1)and long-term stabilities for at least 32 and 30 h for HER and OER,*** impressively,a water splitting electrolylzer assembled by the self-supported Mo-Co_(9)S_(8)@CC electrode requires a low cell voltage of 1.53 V at 10 mA cm^(-2)and shows excellent stability and splendid reversibility,demonstrating a huge potential for affordable and scalable electrochemical H_(2) *** innovational orbital hybridization strategy for electronic regulation herein provides an inspirable avenue for developing progressive electrocatalysts toward new energy systems.

关键词： d-d orbital hybridization Transition metal sulfides Nanorods arrays Water electrolysis

Biphase-to-monophase structure evolution of Na_(0.766+x)Li_(x)Ni_(0.33-x)Mn_(0.5)Fe_(0.1)Ti_(0.07)O_(2) toward ultradurable Na-ion batteries

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Carbon Energy 2024年第9期6卷 66-79页

作者： Mengting Liu Zhiwei Cheng Xu Zhu Haojie Dong Tianran Yan Liang Zhang Lu Zheng Hu-Rong Yao Xian-Zuo Wang Lianzheng Yu Bing Xiao Yao Xiao Peng-Fei Wang State key laboratory of Electrical Insulation and power Equipment School of Electrical EngineeringCenter of Nanomaterials for Renewable EnergyXi'an Jiaotong UniversityXi'anShaanxiChina jiangsu key laboratory of Advanced Negative Carbon Technologies Institute of Functional Nano&Soft Materials(FUNSOM)Soochow UniversitySuzhouJiangsuChina Fujian Provincial key laboratory of Quantum Manipulation and new Energy Materials College of Physics and EnergyFujian Normal UniversityFuzhouFujianChina Wenzhou key laboratory of Sodium-Ion batteries Institute for Carbon NeutralizationWenzhou University Technology InnovationWenzhouZhejiangChina

Layered composite oxide materials with O3/P2 biphasic crystallographic structure typically demonstrate a combination of high capacities of the O3 phase and high operation voltages of the P2 ***,their practical applications are seriously obstructed by difficulties in thermodynamic phase regulation,complicated electrochemical phase transition,and unsatisfactory cycling ***,we propose an efficient structural evolution strategy from biphase to monophase of Na_(0.766+x)Li_(x)Ni_(0.33-x)Mn_(0.5)Fe_(0.1)Ti_(0.07)O_(2) through Li+*** role of Li+substitution not only simplifies the unfavorable phase transition by altering the local coordination of transition metal(TM)cations but also stabilizes the cathode–electrolyte interphase to prevent the degradation of TM cations during battery *** a result,the thermodynamically robust O_(3)-Na_(0.826)Li_(0.06)Ni_(0.27)Mn_(0.5)Fe_(0.1)Ti_(0.07)O_(2) cathode delivers a high capacity of 139.4 mAh g^(-1) at 0.1 C and shows prolonged cycling life at high rates,with capacity retention of 81.6%at 5 C over 500 *** work establishes a solid relationship between the thermodynamic structure evolution and electrochemistry of layered cathode materials,contributing to the development of long-life sodium-ion batteries.

关键词： electrochemistry Li+substitution Na-ion batteries O_(3)phase phase transition

Design method of multivariable PI controller for turboprop engine based on equivalent transfer function

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Chinese Journal of Aeronautics 2024年第9期37卷 237-260页

作者： Shancheng LI Yong WANG Haibo ZHANG jiangsu Province key laboratory of Aerospace power System College of Energy and Power EngineeringNanjing University of Aeronautics and AstronauticsNanjing 210016China

Traditional centralized Proportional Integral(PI)controller design methods based on Equivalent Transfer Functions(ETFs)have poor decoupling effect in turboprop *** this paper,a centralized PI design method based on dynamic imaginary matrix and equivalent transfer function is ***,a method for solving equivalent transfer functions based on the dynamic imaginary matrix is proposed,which adopts dynamic imaginary matrix to describe the dynamic characteristics of the system,and obtains the equivalent transfer function based on the dynamic imaginary matrix ***,for the equivalent transfer function,a central-ized PI control gain is designed using the Taylor expansion ***,this paper further proves that the centralized PI design method proposed in this paper has integral ***-ering the impact of altitude and Mach number on turboprop engines,a linear feedforward control method based on the transfer function matrix is further proposed based on the centralized PI con-troller,and the stability of the entire comprehensive control method is ***,to ensure the safe and effective operation of the turboprop engine,a temperature and torque limiting protection controller is designed for the turboprop *** results show that the centralized PI con-troller design method and linear feedforward control method proposed can effectively improve the control quality of turboprop engine control systems.

关键词： Multivariable control sys-tems Equivalent transfer function Disturbance compensation control Control parameter design Turboprop engine control