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Stepwise assembly to construct stable copper(I) cluster-based circularly polarized luminescent MOFs

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Science china chemistry 2025年

作者： Jing-Wen Xie Meng-Ting Wang yan Jin Si Li Jian-Hua Qin Shuang-Quan Zang Tomas c.W.Mak college of chemistry Henan Key Laboratory of Crystalline Molecular Functional Materials Zhengzhou University college of chemistry and chemical Engineering Luoyang Normal University Department of chemistry The Chinese University of Hong Kong

circularly polarized luminescence （cPL） materials have been extensively studied in recent years owing to their widespread applications in 3D display,optical storage,optical anti-counterfeiting,and biological imaging,***（I） clusters have emerged as a promising candidate for cPL materials,driven by their cost-effectiveness,superior luminescent properties,precise structure,and low ***,the poor environmental stability of copper（I） clusters renders their synthesis and preservation challenging,thereby significantly impeding their ***,we have designed and synthesised a chiral double-coordinated ligand in order to construct copper（I） cluster nodes that can be further *** anticipated,by utilizing stepwise assembly strategy,a cu4cluster node co-modified by chiral alkynyl ligands and triphenylphosphine was further assembled with cd2+ions to obtain 2D layers structure,L/*** L/D-cu4-cd exhibits excellent stability and optical properties,including bright yellow emission,solvent-responsive luminescence,and cPL activity with a maximum glumup to 2.0×10-3,which shows potential applications in the WLED and *** interestingly,the material also exhibits deflection ability towards different wavelengths of linearly polarized light,showing certain potential in the preparation of circular polarizer.

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“Zero‑Strain” NiNb_(2)O_(6) Fibers for All‑climate Lithium Storage

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Nano-Micro Letters 2025年第1期17卷 348-360页

作者： yan Zhao Qiang Yuan Liting yang Guisheng Liang Yifeng cheng Limin Wu chunfu Lin Renchao che college of Physics Donghua UniversityShanghai 201620People’s Republic of China School of Materials Science and Engineering Institute of Materials for Energy and EnvironmentQingdao UniversityQingdao 266071People’s Republic of China Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsAcademy for Engineering&TechnologyFudan UniversityShanghai 200438People’s Republic of China Zhejiang Laboratory Hangzhou 311100People’s Republic of China Inner Mongolia University Hohhot 010021People’s Republic of China

Niobates are promising all-climate Li^(+)-storage anode material due to their fast charge transport,large specific capacities,and resistance to electrolyte ***,their moderate unit-cellvolume expansion(generally 5%–10%)during Li^(+)storage causes unsatisfactory long-term ***,“zero-strain”NiNb_(2)O_(6) fibers are explored as a new anode material with comprehensively good electrochemical *** Li^(+)storage,the expansion of electrochemical inactive NiO_(6) octahedra almost fully offsets the shrinkage of active NbO_(6) octahedra through reversible O *** superior volume-accommodation capability of the NiO_(6) layers guarantees the“zero-strain”behavior of NiNb_(2)O_(6) in a broad temperature range(0.53%//0.51%//0.74%at 25//−10//60℃),leading to the excellent cyclability of the NiNb_(2)O_(6) fibers(92.8%//99.2%//91.1%capacity retention after 1000//2000//1000 cycles at 10c and 25//−10//60℃).This NiNb_(2)O_(6) material further exhibits a large reversible capacity(300//184//318 mAh g−1 at 0.1c and 25//−10//60℃)and outstanding rate performance(10 to 0.5c capacity percentage of 64.3%//50.0%//65.4%at 25//−10//60℃).Therefore,the NiNb_(2)O_(6) fibers are especially suitable for large-capacity,fast-charging,long-life,and all-climate lithium-ion batteries.

关键词： NiNb_(2)O_(6)porous fiber “Zero-strain”mechanism Electrochemical property Harsh-temperature operation Operando characterization

Trinuclear gold-catalyzed site-selective alkylation of peptides

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Science china chemistry 2025年第1期68卷 249-256页

作者： Qing-Yun Fang chengyihan Gu Yinghan chen Wencheng yan Yong Liang Weipeng Li chengjian Zhu Jie Han Jin Xie State key Laboratory of coordination chemistry Jiangsu Key Laboratory of Advanced Organic Materials Chemistry and Biomedicine Innovation Center (Chem BIC) School of Chemistry and Chemical Engineering Nanjing University Green catalysis center College of Chemistry Zhengzhou University State key Laboratory of Natural Medicines China Pharmaceutical University

Selective modification of peptides has always been a challenging issue. The selective alkylation of peptides can alter the biological activity and physical properties of molecules, and it has gained significant research interest. We herein disclose an intriguing gold-catalyzed alkylation of peptides using bench-stable unactivated alkyl bromides under photoredox catalysis. A wide range of structurally diverse primary, secondary and tertiary alkyl bromides serve as effective coupling partners to precisely connect with the α-c(sp3)–H in glycine residue of peptides. This protocol demonstrates an exceptionally broad scope for alkyl halides and excellent tolerance for a wide range of useful functional groups. A series of relay transformations to construct cyclic peptides, to proceed click reaction and to realize peptide fluorescence labeling further enhance its synthetic practicality. In addition, mechanistic studies and density functional theory(DFT) calculations reveal an inner-sphere and subsequent outersphere single electron transfer(SET) mechanism.

关键词： gold catalysis peptide alkylation c-c coupling radical

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Gradient‑Layered MXene/Hollow Lignin Nanospheres Architecture Design for Flexible and Stretchable Supercapacitors

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Nano-Micro Letters 2025年第2期17卷 447-462页

作者： Haonan Zhang cheng Hao Tongtong Fu Dian Yu Jane Howe kaiwen chen Ning yan Hao Ren Huamin Zhai Jiangsu Provincial key Lab of Sustainable Pulp and Paper Technology and Biomass Materials NanJing Forestry UniversityNanjing 210037People’s Republic of China Department of chemical Engineering and Applied chemistry University of Toronto200 College StreetTorontoON M5S 3E5Canada Department of Materials Science and Engineering University of Toronto184 College StreetTorontoON M5S 3E4Canada college of Materials Science and Engineering Nanjing Forestry UniversityNanjing 210037People’s Republic of China

With the rapid development of flexible wearable electronics,the demand for stretchable energy storage devices has *** this work,a novel gradient-layered architecture was design based on single-pore hollow lignin nanospheres(HLNPs)-intercalated two-dimensional transition metal carbide(Ti_(3)c_(2)T_(x) MXene)for fabricating highly stretchable and durable *** depositing and inserting HLNPs in the MXene layers with a bottom-up decreasing gradient,a multilayered porous MXene structure with smooth ion channels was constructed by reducing the overstacking of MXene ***,the micro-chamber architecture of thin-walled lignin nanospheres effectively extended the contact area between lignin and MXene to improve ion and electron accessibility,thus better utilizing the pseudocapacitive property of *** these strategies effectively enhanced the capacitive performance of the *** addition,HLNPs,which acted as a protective phase for MXene layer,enhanced mechanical properties of the wrinkled stretchable electrodes by releasing stress through slip and deformation during the stretch-release cycling and greatly improved the structural integrity and capacitive stability of the *** electrodes and symmetric flexible all-solid-state supercapacitors capable of enduring 600%uniaxial tensile strain were developed with high specific capacitances of 1273 mF cm^(−2)(241 F g^(−1))and 514 mF cm^(−2)(95 F g^(−1)),***,their capacitances were well preserved after 1000 times of 600%stretch-release *** study showcased new possibilities of incorporating biobased lignin nanospheres in energy storage devices to fabricate stretchable devices leveraging synergies among various two-dimensional nanomaterials.

关键词： Hollow lignin nanospheres MXene Gradient-layered architecture Wrinkled electrodes Stretchable supercapacitors

Synergistic promotion strategy of “dual-site” and “dual-path” to enhance the c–c coupling between cO2 and HcHO driven by photoelectrocatalysis

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Journal of Energy chemistry 2025年第1期100卷 39-49页

作者： Hongqiang yang Jianfeng Zheng Guoyu Wang Yifei Gao Yatao yang Jia Li Xiaojin Han yan cui Zhanggen Huang National key Laboratory of High Efficiency and Low carbon Utilization of coal Institute of Coal Chemistry Chinese Academy of Science University of chinese Academy of Science Shenyang University of chemical Technology

Photoelectrocatalytic coupling cO2and volatile organic compounds （VOcs） is a promising green strategy for the synergistic conversion of the two carbon-containing resources to *** catalytic efficiency is always at the mercy of chemical inertness of cO2and the competitive hydrogen evolution of ***,a modified g-c3N4/ZnAl-LDH Z-scheme heterojunction catalyst with dual reaction site was rationally designed and precisely *** Faraday efficiency of ethanol reached 68.67%with a corresponding formation rate of 227.3μmol *** revealed by in-situ characterizations and density functional theory calculations,cO2and HcHO were absorbed at Zn site and N site,***,*cO generated from cO2and HcHO was converted to*cH3O and*cHO on the dual-active-site *** detailed reaction mechanism experiments indicated that c–c coupling only occurred between*cO and*cH3O in electrocatalysis *** from the“*cO+*cH3O”path,another“*cO+*cHO”coupling path was also detected in photoelectrocatalytic *** selectivity of ethanol was significantly enhanced due to the synthesis of dual-site catalyst and the dual-path coupling path between cO2and HcHO simultaneously driven by light and electricity.

关键词： Ethanol

Boosting cationic and anionic redox activity of Li-rich layered oxide cathodes via Li/Ni disordered regulation

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Journal of Energy chemistry 2025年第1期100卷 533-543页

作者： Zewen Liu Zhen Wu Hao Wang Xudong Zhang Yuanzhen chen Yongning Liu Shengwu Guo Shenghua chen yanli Nan yan Liu State key Laboratory for Mechanical Behavior of Materials Xi'an Jiaotong University School of Materials Science and Engineering Xi'an University of Architecture and Technology Hefei Advanced computing center Operation Management corp Ltd Network Information center Xi'an Jiaotong University

Lithium-rich layered oxides （LLOs） are increasingly recognized as promising cathode materials for nextgeneration high-energy-density lithium-ion batteries （LIBs）.However,they suffer from voltage decay and low initial coulombic efficiency （IcE） due to severe structural degradation caused by irreversible O ***,we introduce a three-in-one strategy of increasing Ni and Mn content,along with Li/Ni disordering and TM–O covalency regulation to boost cationic and anionic redox activity simultaneously and thus enhance the electrochemical activity of *** target material,Li1.2Ni0.168Mn0.558co0.074O2（L1）,exhibits an improved IcE of 87.2%and specific capacity of 293.2 mA h g-1and minimal voltage decay of less than 0.53 m V cycle-1over 300 cycles at 1c,compared to Li1.2Ni0.13Mn0.54co0.13O2（Ls）(274.4 mA h g-1for initial capacity,73.8%for IcE and voltage decay of 0.84 mV/cycle over 300 cycles at 1c).Theoretical calculations reveal that the density of states （DOS） area near the Fermi energy level for L1 is larger than that of Ls,indicating higher anionic and cationic redox reactivity than ***,L1 exhibits increased O-vacancy formation energy due to higher Li/Ni disordering of 4.76%（quantified by X-ray diffraction Rietveld refinement） and enhanced TM–O covalency,making lattice O release more difficult and thus improving electrochemical *** increased Li/Ni disordering also leads to more Ni2+presence in the Li layer,which acts as a pillar during Li+de-embedding,improving structural *** research not only presents a viable approach to designing low-co LLOs with enhanced capacity and IcE but also contributes significantly to the fundamental understanding of structural regulation in high-performance LIB cathodes.

关键词： Ice

Discovery of a new family member of arsenic–vanadium polyoxometalates with high catalytic performance for one-pot coupling of cO2, epoxides and amines

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Tungsten 2025年第1期7卷 80-87页

作者： Fang-Qian Wang Yin Zhang Wei-Wei Wang Mei-Qian Fu Hong-Bing Mo Wei-Dong Yu chao Liu Jun yan college of chemistry and chemical Engineering Central South University Junior Education Department Changsha Normal University School of Science Hunan University of Technology and Business

Arsenic-vanadium polyoxometalates（POMs） represent a family of tremendous potential catalysts owing to their peculiar physical and chemical *** in cO2conversion,using POMs to catalyze the conversion of cO2and epoxide into chemical intermediates is the research ***,A new family number of arsenic-vanadium POMs,[N（cH3）4]4[As8V12O38（H2O）]·2H2O({As8V12O38}),was reported and characterized by single-crystal X-ray diffraction,fourier transform infrared spectroscopy,X-ray photoelectron spectroscopy,*** from other allotropicity,{As8V12O38}shows a different structure pattern with an I-43d *** obtained {As8V12O38} was employed as a catalyst for the *** initial catalytic reaction confirmed that {As8V12O38} can catalyze the formation of epoxy carbonate by using 1.01 kPa cO2and epoxide at 70℃.Furtherly,when added amine in the catalytic system,oxazolidinone could be obtained by high yields,which provides an efficient way to convert cO2into profitable ***,a possible catalytic reaction mechanism was proposed by using different characterization analyses.{As8V12O38} first catalyzes the epoxide and cO2to form an epoxy carbonate and then catalyzes epoxy carbonate and benzylamine into oxazolidinone.

关键词： Arsenic cO2 conversion Oxazolidinone Polyoxometalates Vanadium

小世界、结构洞与城市创新的网络机制:来自长三角城市群的证据

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管理工程学报 2025年第2期39卷 14-26页

作者：袁燕吴妍杨大鹏浙江科技大学经济与管理学院浙江杭州310023 浙江金融职业学院电子商务与新消费研究院浙江杭州310018 中共浙江省委党校工商管理教研部浙江杭州311121

近年来,创新网络作为区域和城市创新驱动力的重要性得到了广泛关注。一些研究将网络关系视为知识在城市内和城市间传播的渠道,并通过网络分析视角洞察城市创新的结构和动态。然而,城市创新的网络机制,特别是数字经济发展背景下的数字赋... 详细信息

近年来,创新网络作为区域和城市创新驱动力的重要性得到了广泛关注。一些研究将网络关系视为知识在城市内和城市间传播的渠道,并通过网络分析视角洞察城市创新的结构和动态。然而,城市创新的网络机制,特别是数字经济发展背景下的数字赋能城市创新能力提升机制还有待进一步研究。本文利用长三角城市群26个城市2009年—2018年联合申请专利数据构建了城市创新网络,探讨了网络结构属性——小世界和结构洞对城市创新能力的影响。结果表明,小世界与城市创新能力呈“倒U型”关系,数字经济发展水平正向调节了二者之间的“倒U型”关系,结构洞对城市创新能力具有正向影响。本文厘清了创新网络结构对城市创新能力的影响,回应了以往研究关于小世界和结构洞对创新影响的理论争议,为区域创新的理论研究提供了新颖性观点,深化了对城市群创新发展规律的认识,对推进中国城市群协同创新具有重要意义。

关键词：创新网络城市创新能力专利合作数字经济

Deciphering Water Oxidation catalysts:The Dominant Role of Surface chemistry over Reconstruction Degree in Activity Promotion

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Nano-Micro Letters 2025年第3期17卷 340-354页

作者： Li An Jianyi Li Yuanmiao Sun Jiamin Zhu Justin Zhu Yeow Seow Hong Zhang Nan Zhang Pinxian Xi * Zhichuan JXu chun‑Hua yan State key Laboratory of Applied Organic chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu ProvinceFrontiers Science Center for Rare IsotopesCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000People’s Republic of China School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Singapore Faculty of Materials Science and Energy Engineering Institute of Technology for Carbon NeutralityShenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055People’s Republic of China key Laboratory of Electromagnetic Materials and Devices National Center for International Research On Photoelectric and Energy MaterialsSchool of Materials and EnergyElectron Microscopy CenterYunnan UniversityKunming 650091People’s Republic of China State key Laboratory of Baiyunobo Rare Earth Resource Researches and comprehensive Utilization Baotou Research Institute of Rare EarthsBaotou 014030People’s Republic of China Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU‑HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryPeking UniversityBeijing 100871People’s Republic of China

Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution *** surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has been often correlated with the activity ***,a systematic study on the roles of Fe substitution in activation of perovskite LaNiO_(3)is *** substituting Fe content influences both current change tendency and surface reconstruction ***_(0.9)Fe_(0.1)O_(3)is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi_(1-x)Fe_(x)O_(3)(x=0.00,0.10,0.25,0.50,0.75,1.00)*** reconstructed LaNi_(0.9)Fe_(0.1)O_(3)shows a higher intrinsic activity than most reported NiFe-based ***,density functional theory calculations reveal that Fe substitution can lower the O 2p level,which thus stabilize lattice oxygen in LaNi0.9Fe0.1O3 and ensure its long-term ***,it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction *** effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface *** finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.

关键词： Oxygen evolution reaction Perovskite oxides Doping Activation and reconstruction