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Copper-catalyzed C(sp)-H aryl amination enables modular synthesis of quinolines and 2-quinolinones

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Science China chemistry 2024年第2期67卷 595-603页

作者： Yang Gao Haixia Li Simin Yang Yanping Huo Qian Chen Xianwei Li Zhe Wang Xiao-Qiang Hu school of Chemical engineering and Light Industry Guangdong University of TechnologyGuangzhou510006China Jieyang Branch of chemistry and Chemical engineering Guangdong Laboratory Jieyang515200China Key Laboratory of Catalysis and Energy materials chemistry of Ministry of Education&Hubei Key Laboratory of Catalysis and materials Science School of Chemistry and Materials ScienceSouth-Central University for NationalitiesWuhan430074China

Herein,we disclose a novel copper-catalyzed C(sp)-H aryl amination of terminal alkynes with anthranils,enabling the rapid generation of highly reactive secondary N-aryl ynamines for the modular synthesis of structurally diverse C2-substituted quinolines and *** in-situ formed carbonyl-ynamines are prone to tautomerize to carbonyl-ketenimines,which can efficiently react with a series of nucleophiles,including amines,alcohols,phenols,thiols,thiophenols,active-methylene compounds,and even water to produce various quinoline derivatives with the generation of H_(2)O as a sole and green *** method also unlocks a practical route to create various quinoline-fused heterocycles and can be successfully applied to the late-stage modification of complex molecules and the concise synthesis of bioactive *** studies reveal a coppercatalyzed inner-sphere nitrene transfer process by using anthranils as novel aryl nitrene precursors.

关键词： copper catalysis anthranils C(sp)-H aryl amination carbonyl-ketenimines quinolines

Manipulating Na occupation and constructing protective film of P2-Na_(0.67)Ni_(0.33)Mn_(0.67)O_(2) as long-term cycle stability cathode for sodium-ion batteries

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Journal of Energy chemistry 2024年第1期88卷 603-611,I0013页

作者： Yiran Sun Pengfei Zhou Siyu Liu Zhongjun Zhao Yihao Pan Xiangyan Shen Xiaozhong Wu Jinping Zhao Junying Weng Jin Zhou school of chemistry and Chemical engineering Shandong University of TechnologyZibo 0255000ShandongChina school of materials Science and engineering Shandong University of TechnologyZibo 255049ShandongChina

P2-Na_(0.67)Ni_(0.33)Mn_(0.67)O_(2)(NNMO)is promising cathode material for sodium-ion batteries(SIBs)due to its high specific capacity and fast Na+diffusion ***,the irreversible P2-O_(2)phase transformation,Na+/vacancy ordering,and transition metal(TM)dissolution seriously damage its cycling stability and restrict its commercialization ***,Na occupation manipulation and interface stabilization are proposed to strengthen the phase structure of NNMO by synergistic Zn/Ti co-doping and introducing lithium difluorophosp(LiPO_(2)F_(2))film-forming electrolyte *** Zn/Ti co-doping regulates the occupancy ratio of Nae/Nafat Na sites and disorganizes the Na+/vacancy ordering,resulting in a faster Na+diffusion kinetics and reversible P2-Z phase transition for P2-Na_(0.67)Ni_(0.28)Zn_(0.05)Mn_(0.62)Ti_(0.05)O_(2)(NNZMTO).Meanwhile,the LiPO_(2)F_(2)additive can form homogeneous and ultrathin cathode-electrolyte interphase(CEI)on NNZMTO surface,which can stabilize the NNZMTO-electrolyte interface to prevent TM dissolution,surface structure transformation,and micro-crack *** studies of in situ and ex situ characterizations and theoretical calculations were used to elucidate the storage mechanism of NNZMTO with Li PO_(2)F_(2)*** a result,the NNZMTO displays outstanding capacity retention of 94.44%after 500 cycles at 1C with 0.3 wt%Li PO_(2)F_(2),excellent rate performance of 92.5 mA h g^(-1)at 8C with 0.1 wt%Li PO_(2)F_(2),and remarkable full cell *** work highlights the important role of manipulating Na occupation and constructing protective film in the design of layered materials,which provides a promising direction for developing high-performance cathodes for SIBs.

关键词： Layered cathode Zn/Ti co-doping Na occupation Electrolyte additive Sodium-ion batteries

Emerging two-dimensional Mo-based materials for rechargeable metal-ion batteries:Advances and perspectives

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Journal of Energy chemistry 2024年第2期89卷 487-518,I0012页

作者： Qingqing Ruan Yuehua Qian Mengda Xue Lingyun Chen Qichun Zhang Department of Applied chemistry School of Chemistry and Chemical EngineeringChongqing UniversityChongqing 401331China Department of materials Science and engineering City University of Hong Kong999077Hong KongChina

With the rapid development of rechargeable metal-ion batteries(MIBs)with safety,stability and high energy density,significant efforts have been devoted to exploring high-performance electrode *** recent years,two-dimensional(2D)molybdenum-based(Mo-based)materials have drawn considerable attention due to their exceptional characteristics,including low cost,unique crystal structure,high theoretical capacity and controllable chemical ***,like other transition metal compounds,Mo-based materials are facing thorny challenges to overcome,such as slow electron/ion transfer kinetics and substantial volume changes during the charge and discharge *** this review,we summarize the recent progress in developing emerging 2D Mo-based electrode materials for MIBs,encompassing oxides,sulfides,selenides,*** introducing the crystal structure and common synthesis methods,this review sheds light on the charge storage mechanism of several 2D Mo-based materials by various advanced characterization *** latest achievements in utilizing 2D Mo-based materials as electrode materials for various MIBs(including lithium-ion batteries(LIBs),sodium-ion batteries(SIBs)and zinc-ion batteries(ZIBs))are discussed in ***,the modulation strategies for enhancing the electrochemical performance of 2D Mo-based materials are highlighted,focusing on heteroatom doping,vacancies creation,composite coupling engineering and nanostructure ***,we present the existing challenges and future research directions for 2D Mo-based materials to realize high-performance energy storage systems.

关键词： Molybdenum-based materials Two-dimensional materials Lithium-ion batteries Sodium-ion batteries Zinc-ion batteries

B and Fe co-doped Co_(2)P hollow nanocubes for nitrate electroreduction to ammonia

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Chinese Chemical Letters 2024年第2期35卷 278-282页

作者： Jing Miao Qingling Hong Liping Liang Guomin Li Zhihong Liu Shibin Yin Yu Chen school of materials Science and engineering Taiyuan University of Science and TechnologyTaiyuan 030024China school of materials Science and engineering Shaanxi Normal UniversityXi'an 710062China school of chemistry and Chemical engineering Shaanxi Normal UniversityXi'an 710062China Guangxi Key Laboratory of Electrochemical Energy materials School of Chemistry and Chemical EngineeringGuangxi UniversityNanning 530004China

Nitrate(NO_(3)^(−))electroreduction reaction(NO_(3)^(−)RR)provides an attractive and sustainable route for NO_(3)^(−)pollution mitigation or energy-saved ammonia(NH3)*** this work,high-quality B and Fe co-doped Co_(2) P hollow nanocubes(B/Fe-Co_(2) P HNCs)are successfully synthesized though simultaneous boronation-phosphorization treatment,which reveal outstanding selectivity,activity,stability for the NO_(3)^(−)to NH_(3) conversion in neutral electrolyte because of big surface area,fast mass transport,superhydrophilic surface,and optimized electronic structure.B/Fe-Co_(2) P HNCs can achieve the high NH3 yield rate(22.67 mg h^(−1) mg_(cat)^(−1))as well as Faradaic efficiency(97.54%)for NO_(3)^(−)RR,greatly outperforming most of non-precious metal based NO_(3)^(−)RR electrocatalysts.

关键词： Nitrate electroreduction reaction Ammonia synthesis Transition metal phosphides Hollow nanocubes

Stretchable and self-healing conductive fibers from hierarchical silver nanowires-assembled network

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Nano Research 2024年第2期17卷 763-770页

作者： Ying-Ying Wu Hong Chen Fan Zhang Pan Guo Haili Qin Huai-Ping Cong Anhui Province Key Laboratory of Advanced Catalytic materials and Reaction engineering School of Chemistry and Chemical EngineeringHefei University of TechnologyHefei 230009China

Conductive fibers(CFs)with features of high conductivity,stretchability,self-healability,and electromechanical stability are key components of the increasingly popular wearable ***,since the lack of structural design of conductive network and interfacial interaction between soft polymer and conductive additives,it is still hard to enable CFs to meet above ***,we describe a facial drawing method from a hydrogel reservoir which is remolded into ultrathin and stretchable CFs with excellent multi-responsive *** hydrogel reservoir was fabricated in synergy of an ice-templating method and in situ polymerization using the assembled framework as a *** on the effective fabrication mechanism,the diameter of CFs could be well-tuned from 90 to 400μm by adjusting the dipping depth of the glass rod,accompanied with conductivity increased from 0.75 to 2.5 S/*** the hierarchical network structure was well maintained in the CFs,professional performances have been proved on the stretchability and electromechanical *** presence of massive hydrogen bonding and Ag–S bond enabled the CFs with excellent self-healability under the conditions of contact,electric field,and near infrared light,***,the CFs with high sensing property could be integrated into an advanced textile sensor through an effective healing-induced integration strategy,demonstrating its great potentials as superior two-dimensional(2D)electronic skins.

关键词： conductive fibers self-assembled silver nanowires Ag–S coordination self-healing flexible sensors

Universal synthesis of metallophthalocyanine covalent organic frameworks as ultra-sensitive multifaceted electrochemical sensor

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Science China chemistry 2024年第6期67卷 2092-2101页

作者： Qi Liu Qiqi Sun Yuming Zhang Hao Li Wenmiao Chen Yuexing Zhang Sirong Yu Yanli Chen Jianzhuang Jiang school of materials Science and engineering China University of Petroleum(East China)Qingdao266580China Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline materials School of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing100083China College of chemistry and Chemical engineering Dezhou UniversityDezhou253023China

The universal synthesis of highly stable covalent organic frameworks(COFs)for ultra-sensitive and multi-component electrochemical detection in different scenarios remains a great ***,a series of metallophthalocyanine-based twodimensional(2D)dioxin(DXI)-linked metalophthalocyanine(MPc)-n DXI-COFs(M=Ni,Zn;n=1,2)are afforded in high yield(80%-96%)by a facile trace-quinoline assisted one-pot condensation of tetracarbonitrile *** X-ray diffraction and electron microscopy investigations disclose their lamellar texture 2D network with AA stacking *** and calculation results elucidate that the 2DXI-linked MPc-2DXI-COFs provide the stronger built-in electronic field and more electrostatic/hydrogen bonding adsorption sites than DXI-linked MPc-DXI-COFs,and the lower electrode reaction Gibbs free energy and stronger adsorption of analytes at Ni Pc than Zn Pc unit,which grants Ni Pc-2DXI-COF excellent sensing properties for various analytes including neurotransmitters,organic pollutants,and heavy metal ions,with high sensitivity and low detection limit of 0.53 to 25.66 *** in binary and ternary systems and even in real-world conditions,simultaneous multi-component detection could be achieved.

关键词： covalent organic framework metallophthalocyanine 2D materials electrochemical sensors multi-component detection

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Designing metal sulfide-based cathodes and separators for suppressing polysulfide shuttling in lithium-sulfur batteries

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Nano Research 2024年第4期17卷 2574-2591页

作者： Guoyin Zhu Qingzhu Wu Xianghua Zhang Yuwen Bao Xuan Zhang Zhuoyao Shi Yizhou Zhang Lianbo Ma Institute of Advanced materials and Flexible Electronics(IAMFE) School of Chemistry and Materials ScienceNanjing University of Information Science&TechnologyNanjing 210044China school of materials Science and engineering Anhui University of TechnologyMaanshan 243002China school of Mechanical engineering Jiangsu University of TechnologyChangzhou 213001China

Lithium-sulfur(Li-S)batteries,known for their high energy density,are attracting extensive research interest as a promising next-generation energy storage ***,their widespread use has been hampered by certain issues,including the dissolution and migration of polysulfides,along with sluggish redox *** sulfides present a promising solution to these obstacles regarding their high electrical conductivity,strong chemical adsorption with polysulfides,and remarkable electrocatalytic capabilities for polysulfide *** this review,the recent progress on the utilization of metal sulfide for suppressing polysulfide shuttling in Li-S batteries is systematically summarized,with a special focus on sulfur hosts and functional *** critical roles of metal sulfides in realizing high-performing Li-S batteries have been comprehensively discussed by correlating the materials’structure and electrochemical ***,the remaining issues/challenges and future perspectives are *** offering a detailed understanding of the crucial roles of metal sulfides,this review dedicates to contributing valuable knowledge for the pursuit of high-efficiency Li-S batteries based on metal sulfides.

关键词： lithium-sulfur batteries metal sulfides polysulfide shuttling sulfur hosts separator coating layers

Bridging molecular photosensitizer and catalyst on carbon nanotubes toward enhanced selectivity and durability for CO_(2)photoreduction

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Journal of Environmental Sciences 2024年第6期140卷 157-164页

作者： Xiaofeng Cui Xueting Wang Lijun Zhao Jixin Wang Tingting Kong Yujie Xiong Anhui engineering Research Center of Carbon Neutrality The Key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Laboratory of Molecular-Based MaterialsCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China school of chemistry and Chemical engineering Anqing Normal UniversityAnqing 246011China school of chemistry and materials Science University of Science and Technology of ChinaHefei 230026China

Homogenous molecular photocatalysts for CO_(2)reduction,especially metal complex-based photosensitizer-catalyst assemblages,have been attracting extensive research interests due to their efficiency and ***,their low durability and recyclability limit practical *** this work,we immobilized the catalysts of metal terpyridyl complexes and the photosensitizer of[Ru(bpy)3]Cl2onto the surface of carbon nanotubes through covalent bonds and electrostatic interactions,respectively,transforming the homogeneous system into a heterogeneous *** characterizations prove that these metal complexes are well dispersed on CNTs with a high loading(ca.12 wt.%).Photocatalytic measurements reveal that catalytic activity is remarkably enhanced when the molecular catalysts are anchored,which is three times higher than that of homogeneous molecular ***,when the photosensitizer of[Ru(bpy)3]Cl2is immobilized,the side reaction of hydrogen evolution is completely suppressed and the selectivity for CO production reaches 100%,with its durability also significantly *** work provides an effective pathway for constructing heterogeneous photocatalysts based on rational assembly of efficient molecular photosensitizers and catalysts.

关键词： durability selectivity catalyst

Open-Shell Oligomers and Polymers: Theory, Characterization Methods, Molecular Design, and Applications

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Chinese Journal of Polymer Science 2024年第4期42卷 417-436页

作者： Xue-Qing Wang Cheng Song Ting Lei Key Laboratory of Polymer chemistry and Physics(Ministry of Education) School of Materials Science and EngineeringPeking UniversityBeijing100871China

Open-shell oligomers and polymers have exhibited intriguing electronic and magnetic properties, making them highly desirable for a wide range of applications, including ambipolar organic field-effect transistors (OFETs), photodetectors, organic thermoelectrics, and spintronics. Although open-shell ground states have been observed in certain small molecules and doped organic semiconductors, the exploration of open-shell ground-state conjugated polymers is still limited, and the strategies for designing these polymers remain obscure. This review aims to briefly introduce the theory and characterization methods of open-shell conjugated polymers, along with an overview of recent progress and applications. The objective is to stimulate further advancements and investigations in this promising area by shedding light on the potential of open-shell conjugated polymers and the challenges that lie ahead.

关键词： Conjugated polymers Open-shell molecules High-spin ground state Donor-acceptor(D-A)polymers Optoelectronic and magnetic properties