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Anti-corrosive and highly reversible zinc metal anode enabled by the phenolic resin coating

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Rare Metals 2024年第5期43卷 2115-2124页

作者： Ya-Ping Wang Ya-Di Yang Shu-Qi Duan Li Wang Jia-Shuo Guo An-Qiang Pan School of materials Science and Engineering Hebei University of TechnologyTianjin 300130China key laboratory of Special functional materials for Ecological environment and Information(Hebei University of Technology).Ministry of Education Tianjin 300130China key laboratory for New Type of functional materials in Hebei Province Hebei University of TechnologyTianjin 300130China School of materials Science and Engineering Central South UniversityChangsha 410083China

Aqueous zinc-ion batteries have attracted much attention due to their high theoretical capacity,low cost high safety,and ***,challenges such as dendrite growth and side reactions severely hinder the electrochemical performance of the Zn anode,leading to low Coulombic efficiency(CE)or even short circuits Herein,phenolic resin(PF)is used as a protective coating on the surface of the zinc metal *** PF layer can greatly improve the corrosion resistance of the Zn electrode in the ***,this artificial electrode/electrolyte interphase also elevates the nucleation barrier and restrains Zn^(2+)2D diffusion,regulating the zinc deposition/dissolution *** a result,PF@Zn symmetric cells exhibit superior performance than that of bare Zn symmetric cells,achieving a stable and dendrite-free cycle of 1400 ***,the carbon nanotube MnO_(2)||PF@Zn(CNT/MnO_(2)||PF@Zn)full cell also delivers a long cycle life with a high-capacity retention of about 180.0 m Ah·g^(-1)after 1400 cycles,far exceeding that of bare Zn *** work provides a facile strategy for achieving a dendrite-free and rechargeable zinc anode.

关键词： Rechargeable aqueous batteries Zn metal anode Phenolic resin Anti-corrosion

Tailoring electron vortex beams with customizable intensity patterns by electron diffraction holography

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Opto-Electronic Advances 2024年第2期7卷 14-21页

作者： Pengcheng Huo Ruixuan Yu Mingze Liu Hui Zhang Yan-qing Lu Ting Xu National laboratory of Solid-State Microstructures and Collaborative Innovation Center of Advanced Microstructures Nanjing UniversityNanjing 210093China College of Engineering and Applied Sciences Key Laboratory of Intelligent Optical Sensing and Manipulation and Jiangsu Key Laboratory of Artificial Functional MaterialsNanjing UniversityNanjing 210093China

An electron vortex beam(EVB) carrying orbital angular momentum(OAM) plays a key role in a series of fundamental scientific researches, such as chiral energy-loss spectroscopy and magnetic dichroism spectroscopy. So far, almost all the experimentally created EVBs manifest isotropic doughnut intensity patterns. Here, based on the correlation between local divergence angle of electron beam and phase gradient along azimuthal direction, we show that free electrons can be tailored to EVBs with customizable intensity patterns independent of the carried OAM. As proof-of-concept, by using computer generated hologram and designing phase masks to shape the incident free electrons in the transmission electron microscope, three structured EVBs carrying identical OAM are tailored to exhibit completely different intensity patterns. Furthermore, through the modal decomposition, we quantitatively investigate their OAM spectral distributions and reveal that structured EVBs present a superposition of a series of different eigenstates induced by the locally varied geometries. These results not only generalize the concept of EVB, but also demonstrate an extra highly controllable degree of freedom for electron beam manipulation in addition to OAM.

关键词： electron vortex beam orbital angular momentum diffraction holography

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

Constructing oxygen deficiency-rich V_(2)O_(3)@PEDOT cathode for high-performance aqueous zinc-ion batteries

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Rare Metals 2024年第2期43卷 635-646页

作者： Dong-Fei Sun Zi-Juan Wang Tian Tian Xin Yu Dan-Dan Yu Xiao-Zhong Zhou Guo-Fu Ma Zi-Qiang Lei key laboratory of Eco-functional Polymer materials of the Ministry of Education Key Laboratory of Eco-environmental Polymer Materials of Gansu ProvinceSchool of College of Chemistry and Chemical EngineeringNorthwest Normal UniversityLanzhou730070China

Aqueous zinc-ion batteries(AZIBs)have attracted widespread attention due to the advantages of high safety and environmental *** V_(2)O_(3) is a promising cathode,the strong electrostatic interaction between Zn^(2+) and V_(2)O_(3) crystal,and the sluggish reaction kinetics still limit their application in ***,the oxygen defects rich V_(2)O_(3) with conducive poly(3,4-ethylenedioxythiophene)(PEDOT)shell(V_(2)O_(3)-Od@PEDOT)was fabricated for AZIBs by combining the sulfur-assisted thermal reduction and in-situ polymerization *** introduced oxygen vacancies of V_(2)O_(3)–Od@PEDOT weaken the electrostatic interaction between Zn^(2+) and the host material,improving the interfacial electron transport,while the PEDOT coating enhances the structural stability and conductivity of V_(2)O_(3),thus accelerating the reaction *** on the advantages,V_(2)O_(3)–Od@PEDOT electrode delivers a reversible capacity of 495 mAh·g^(−1) at 0.1 A·g^(−1),good rate capability(189 mAh·g^(−1)at 8.0 A·g^(−1)),and an impressive cycling stability with 90.1%capacity retention over 1000 cycles at 8.0 A·g^(−1).The strategy may provide a path for exploiting the other materials for high performance AZIBs.

关键词： Oxygen defects V_(2)O_(3) PEDOT Electrochemical self-optimization Aqueous zinc-ion batteries

Semicrystalline Unfused Polymer Donors with Backbone Halogenation toward Cost-Effective Organic Solar Cells

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Chinese Journal of Chemistry 2024年第7期42卷 752-759页

作者： Yuxin Kong Shijie Ju Hongmei Qin Min Hun Jee Simeng Xia Jiaqi Ren Chao Gao Jianyu Yuan Wenyan Su Han Young Woo Yuxiang Li School of materials Science and Engineering Xi'an University of Science and TechnologyXianShaanxi 710054China Department of Chemistry Korea UniversitySeoul 02841Republic of Korea Xi'an key laboratory of Liquid Crystal and Organic Photovoltaic materials State Key Laboratory of Fluorine&Nitrogen ChemicalsXi'an Modern Chemistry Research InstituteXi'anShaanxi 710065China jiangsu key laboratory for Carbon-Based functional materials&Devices Institute of Functional Nano&Soft Materials(FUNSOM)Soochow University199 Ren'ai RoadSuzhouJiangsu 215123China

Developing novel unfused building blocks with simple synthesis and low cost is essential to advance and enrich cost-effective poly-mer donors;however,it remains a challenge due to the lack of efficient molecular ***,a class of low-cost and fully unfused polymer donors with precisely regulated backbone planarity via halogenation was designed and synthesized,namely PDTBTBz-2H,PDTBTBz-2F,and *** polymer donors possess a four-step synthesis route with over 80%yield from cheap raw chemicals comparable to existing low-cost polymer donors,such as *** from the planar backbone via in-corporating the F…S non-covalent interactions,PDTBTBz-2F exhibits more robust J-type aggregation in solution and a long-ranged molecular stacking in film relative to PDTBTBz-2H and ***,the systematical study of PDTBTBz-based organic so-lar cells(OSCs)reveals the close relationship between optimized molecular self-assembly and charge separation/transport regarding backbone halogenation when paired with the non-fullerene acceptor(Y6-BO-4F).As a result,the photovoltaic devices based on semicrystalline PDTBTBz-2F achieved a promising power conversion efficiency(PCE)of 12.37%.Our work highlighted the influence of backbone halogenation on the molecular self-assembly properties and a potential unfused backbone motif for further developing cost-effective OSCs.

关键词： Low-cost Polymer donors Backbone halogenation Molecular self-assembly Organic solar cells

Isocyanide-Based One-Pot Cascade Synthesis of 3-Acyl Isoindolinones

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Chinese Journal of Chemistry 2024年第3期42卷 259-263页

作者： Jia Liu Yi-Ming Zhu Xiao-Ping Xu Shun-Jun Ji key laboratory of Organic Synthesis of jiangsu Province College of ChemistryChemical Engineering and Materials Science & Collaborative Innovation Center of Suzhou Nano Science and TechnologySoochow UniversitySuzhouJiangsu215123 China Suzhou Baolidi functional materials Research Institute SuzhouJiangsu215144 China

A series of 3-acyl-substituted isoindolinone derivatives were synthesized in a one-pot manner via the reaction of o-bromobenzaldehydes,isocyanides,and carboxylic acids in the presence of palladium catalyst and base. The reaction employing easily available starting materials features simple operation and high efficiency. The mechanistic study showed that the reaction might undergo 1) Pd-catalyzed [3+2] cyclization of o-bromobenzaldehyde with isocyanide and the re-insertion of another molecule of isocyanide,2) addition of carboxylic acid to in situ formed ketenimine followed by a rearrangement relay to give 3,3-diacyl-substituted isoindolinone derivative. Further transformations of the obtained products through decarbonylation could also be realized.

关键词： One-pot reaction Isocyanide Pd catalysis Rearrangement reaction Isoindolinone

Metal complex catalysts broaden bioorthogonal reactions

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Science China Chemistry 2024年第2期67卷 428-449页

作者： Hanjie Zhang Xiaoyu Qin Junping Wang Li Ma Tianfeng Chen Department of Chemistry Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou510632China

Bioorthogonal reactions involving transition metals have diversified applications in imaging,drug development,chemical catalysis and other *** metals used to catalyze the bioorthogonal reaction mainly include ruthenium,palladium,copper,and ***,the great potential for translational applications of bioorthogonal reaction needs to be further expanded and their reaction efficiency should be ***,it is an urgent need for the development of this field to find more suitable catalysts to efficiently catalyze existing biological orthogonal reactions and expand the types of biological orthogonal ***,this review not only summarizes those transition metal complexes-based catalysts participating in bioorthogonal reaction and some bioorthogonal reactions involving transition metals inside the cells,but also sheds light into the discovery of new transition metal complexes and their future development in applications.

关键词： transition metal complexes bioorthogonal reactions biological applications

Excellent energy storage performance in Bi_(0.5)Na_(0.5)TiO_(3)-based lead-free high-entropy relaxor ferroelectrics via B-site modification

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Journal of Advanced Ceramics 2024年第3期13卷 345-353页

作者： Kaihua Yang Gengguang Luo Li Ma Ruoxuan Che Zhiyi Che Qin Feng Zhenyong Cen Xiyong Chen Jiajun Zhou Nengneng Luo State key laboratory of Featured Metal materials and Life-cycle Safety for Composite Structures School of ResourcesEnvironment and MaterialsGuangxi UniversityNanning 530004China School of Optical and Electronic Information Key Lab of Functional Materials for Electronic Information(B)of Ministry of EducationHuazhong University of Science and TechnologyWuhan 430074China

Next-generation advanced high/pulsed power capacitors urgently require dielectric materials with outstanding energy storage ***_(0.5)Na_(0.5)TiO_(3)-based lead-free materials exhibit high polarization,but the high remanent polarization and large polarization hysteresis limit their applications in dielectric ***,high-entropy perovskite relaxor ferroelectrics(Na_(0.2)Bi_(0.2)Ba_(0.2)Sr_(0.2)Ca_(0.2))(Ti1-x%Zrx%)O_(3)are designed by adding multiple ions in the A-site and replacing the B-site Ti^(4+)with a certain amount of Zr^(4+).The newly designed system showed high relaxor feature and slim polarization-electric(P-E)***,improved relaxor feature and obviously delayed polarization saturation were found with the increasing of Zr^(4+).Of particular importance is that both high recoverable energy storage density of 6.6 J/cm^(3) and energy efficiency of 93.5%were achieved under 550 kV/cm for the ceramics of x=6,accompanying with excellent frequency stability,appreciable thermal stability,and prosperous discharge *** work not only provides potential dielectric materials for energy storage applications,but also offers an effective strategy to obtain dielectric ceramics with ultrahigh comprehensive energy storage performance to meet the demanding requirements of advanced energy storage applications.

关键词： energy storage density (Bi_(0.5)Na_(0.5))TiO_(3) high-entropy perovskite ceramics polarization saturation relaxor ferroelectrics(RFEs)

Hierarchical porous(Ta_(0.2)Nb_(0.2)Ti_(0.2)Zr_(0.2)Hf_(0.2))C high-entropy ceramics prepared by a self-foaming method for thermal insulation

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Journal of Advanced Ceramics 2024年第7期13卷 956-966页

作者： Cuiyan Li Ruinan Gao Haibo Ouyang Tianzhan Shen Zihao Chen Yanlei Li key laboratory for Green Manufacturing&functional Application of Inorganic materials School of Materials Science and EngineeringShaanxi University of Science and TechnologyXi’an 710021China

To meet the emerging demands for thermal protection materials for hypersonic aircraft,developing porous ultrahigh-temperature ceramics with both robust mechanical properties and superior thermal insulation performance is a critical ***,we report novel porous(Ta_(0.2)Nb_(0.2)Ti_(0.2)Zr_(0.2)Hf_(0.2))C high-entropy carbide(PHEC)ceramics fabricated by a self-foaming method using commercially available metal chloride and furfuryl alcohol(FA)as *** PHEC ceramics are constructed of microspheres with a size of 2µm,leading to a high porosity of 91.3%and an interconnected *** microspheres consist of high-entropy carbide grains(20 nm),resulting in abundant interfaces and nanosized pores in the PHEC *** to its unique hierarchical structure,the prepared PHEC ceramics have outstanding compressive strength(28.1±2 MPa)and exceptionally low thermal conductivity(κT,0.046 W·m^(-1)·K^(-1))at room *** makes it a promising thermal insulation materials for ultrahigh temperature *** work provides a cost-effective and facile strategy for producing porous ultrahigh-temperature ceramics.

关键词： porous ceramics high-entropy carbides hierarchical structure thermal insulation self-foaming