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Silvery fullerene in Ag102 nanosaucer

National Science Review 2024年第7期11卷 158-167页

作者： Zhi Wang Yuchen Wang Chengkai Zhang Yan-Jie Zhu Ke-Peng Song Christine M.Aikens Chen-ho tung Di Sun School of Chemistry and Chemical Engineering Shandong University Department of Chemistry Kansas State University

Despite the discovery of a series of fullerenes and a handful of noncarbon clusters with the typical topology of Ih-C60, the smallest fullerene with a large degree of curvature, C20, and its other-element counterparts are difficult to isolate experimentally. In coinage metal nanoclusters（NCs）, the first all-gold fullerene, Au3., was discovered after a long-lasting pursuit, but the isolation of similar silvery fullerene structures is still challenging. Herein, we report a flying saucer-shaped 102-nuclei silver NC（Ag102） with a silvery fullerene kernel of Ag3., which is embraced by a robust cyclic anionic passivation layer of（KPO4）10. This Ag3.kernel can be viewed as a non-centered icosahedron Ag12encaged into a dodecahedron Ag20, forming the silvery fullerene of Ag12@Ag20. The anionic layer（KPO4）10is located at the interlayer between the Ag3.kernel and Ag70shell, passivating the Ag3.silvery fullerene and templating the Ag70shell. The ~tBuPhS-and CF3.OO-ligands on the silver shell show a regioselective arrangement with the 60 ~tBuPhS-ligands as expanders covering the upper and lower of the flying saucer and 10 CF3.OO-as terminators neatly encircling the edges of the structure. In addition, Ag102 shows excellent photothermal conversion efficiency（η） from the visible to near-infrared region（η = 67.1% ± 0.9% at 450 nm, 60.9% ± 0.9% at 660 nm and 50.2% ± 0.5% at 808 nm）, rendering it a promising material for photothermal converters and potential application in remote laser ignition. This work not only captures silver kernels with the topology of the smallest fullerene C20, but also provides a pathway for incorporating alkali metal（M） into coinage metal NCs via M-oxoanions.

关键词： silvery fullerene >Ag102 nanosaucer cyclic anionic passivation layer photothermal conversion DFT calculation

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Copper(Ⅰ)-catalyzed interrupted click/radical relay:A four-component modular synthesis of triazole sulfones

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Chinese Chemical Letters 2024年第3期35卷 247-251页

作者： Pengfei Sun Fang Wei Chen-ho tung Zhenghu Xu Key Lab for Colloid and Interface Chemistry of Education Ministry Shandong UniversityJi'nan 250100China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China Functional Molecules of Zhejiang Province School of ScienceWestlake UniversityHangzhou 310024China Key Laboratory of Organic Chemistry in Jiangxi Province Institute of Organic ChemistryJiangxi Science&Technology Normal UniversityNanchang 330013China

A new,four component copper(Ⅰ)-catalyzed interrupted click/radical relay cascade has been *** unprecedented interrupted click reaction provides a rapid modular synthesis of triazole sulfones,important privileged heterocyclic pharmacophores which cannot be accessed by a traditional click *** interception of cuprate-triazole,the key reaction intermediate formed in situ,is an important feature of this process.

关键词： Click reaction Triazole Sulfone Radical relay

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Cathode nanoarchitectonics with Na_(3.VFe_(0.5)Ti_(0.5)(PO_(4))_(3.: Overcoming the energy barriers of multielectron reactions for sodium-ion batteries

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Carbon Energy 2024年第9期6卷 1-14页

作者： Vaiyapuri Soundharrajan Sungjin Kim Subramanian Nithiananth Muhammad H.Alfaruqi JunJi Piao Duong tung Pham Vinod Mathew Sang A.Han Jung ho Kim Jaekook Kim Department of Materials Science and Engineering Chonnam National UniversityBukguGwangjuRepublic of Korea Graduate School of Science and Technology Shizuoka UniversityHamamatsuShizuokaJapan Departemen Teknik Metalurgi Universitas Teknologi SumbawaSumbawaIndonesia School of Engineering Physics Hanoi University of Science and TechnologyHanoiVietnam Institute for Superconducting and Electronic Materials(ISEM) Australian Institute of Innovative Materials(AIIM)University of WollongongNorth WollongongNew South WalesAustralia Research Center for Artificial Intelligence Assisted Ionics Based Materials Development Platform Chonnam National UniversityGwangjuRepublic of Korea

High electrochemical stability and safety make Na+superionic conductor(NASICON)-class cathodes highly desirable for Na-ion batteries(SIBs).however,their practical capacity is limited,leading to low specific ***,the low electrical conductivity combined with a decline in capacity upon prolonged cycling(>1000 cycles)related to the loss of active material-carbon conducting contact regions contributes to moderate rate performance and cycling *** need for high specific energy cathodes that meet practical electrochemical requirements has prompted a search for new ***,we introduce a new carbon-coated Na_(3.VFe_(0.5)Ti_(0.5)(PO_(4))_(3.(NVFTP/C)material as a promising candidate in the NASICON family of cathodes for *** a high specific energy of∼457 Wh kg^(-1) and a high Na+insertion voltage of 3.0 V versus Na^(+)/Na,this cathode can undergo a reversible single-phase solid-solution and two-phase(de)sodiation evolution at 28 C(1 C=174.7 mAh g^(-1))for up to 10,000 *** study highlights the potential of utilizing low-cost and highly efficient cathodes made from Earth-abundant and harmless materials(Fe and Ti)with enriched Na^(+)-storage properties in practical SIBs.

关键词： Fe and Ti swapping Na_(3.VFe_(0.5)Ti_(0.5)(PO_(4))_(3. prolonged cycle life structural stabilit

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Dangling Ligand Enables an Iron Hexa-Coordinated Molecular Catalyst for Water Oxidation by Photocatalysis

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CCS Chemistry 2024年第3期6卷 623-630页

作者： Bing Yang Qi Liu Xiang-Zhu Wei Tao Lei Qing-Qing Yang Xu-Zhe Wang Jing-Xin Jian Xin Jiang Chen-ho tung Li-Zhu Wu Key Laboratory of Photochemical Conversion and Optoelectronic Materials New Cornerstone Science LaboratoryTechnical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190 School of Future Technology University of Chinese Academy of SciencesBeijing 100049

Photocatalytic water oxidation reaction by transition metal complexes remains a challenge because of their poor stability under irradiation,especially for earth-abundant metal *** this regard,ironbased water oxidation catalysts are prone to hydrolysis and/or dissociate the ligands to form nanoparticles under a real catalytic ***,we describe a unique hexa-coordinated catalyst 1[Fe^(II)(Py_(3.tacn)Cl_(2)]and its reference 2[Fe^(II)(PhPy_(2)tacn)Cl_(2)]with a dangling pyridyl ligand and a phenyl group,*** anticipated that the dynamically open and close coordination behaviors of the pyridyl ligand enabled balance of the reactivity and stability of catalyst *** our delight,the“open form”of catalyst 1 provided a free coordination site,and the“close form”guaranteed its molecular integrity,resulting in a water oxidation reaction with high efficiency and *** turnover number and turnover frequency values of 23.2 and 60 s^(−1)are the highest known to date among iron-based homogeneous water oxidation systems under visible light irradiation.

关键词： water oxidation photocatalysis homogeneous catalysis iron complexes dangling ligand intermediates characterization

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Hierarchical homochiral Assembly of Polyhedral Cage-Type Nanoclusters

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CCS Chemistry 2024年第10期6卷 2537-2548页

作者： Cheng-Long Deng Bao-Liang Han Ze-Yu Liu Zhong-Hua Pan Jiao He Yu-Long Li Zhi-Lin Yang Geng-Geng Luo Chen-ho tung Di Sun Lan-Sun Zheng Key Laboratory of Environmentally Friendly Function Materials Ministry of EducationCollege of Materials Science and EngineeringHuaqiao UniversityXiamen 361021 School of Chemistry and Chemical Engineering State Key Laboratory of Crystal MaterialsShandong UniversityJi’nan 250100 College of Physical Science and Technology Xiamen UniversityXiamen 361005 College of Chemistry and Environmental Engineering Sichuan University of Science and EngineeringZigong 643000 State Key Laboratory for Physical Chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005

Hierarchical chiral self-assembly is of profound significance for biomolecules for their biological ***-precise metal nanoclusters(NCs)offer better opportunities to construct hierarchical ***,achieving hierarchical homochiral assembly of nanocrystals protected by achiral ligands has proven to be a formidable task,with existing examples primarily limited to heterochiral *** we put forward a hierarchical assembly strategy towards precisely fabricating highly ordered homochiral ***,clusterin-nanocage type copper-hydride NCs act as synthons,of which entity is featured with a hexagonal close-packed Cu_(9)kernel embedded in a C_(3.-symmetric trigonal-prismatic metallacage,leading to a chiral core-shell primary structure with either P or M *** four homochiral NCs combined with guests through synergistic noncovalent interactions spontaneously organize into a supramolecular tetrahedral secondary structure within a unit ***,these nanoscopic supramolecular motifs pack into tertiary hierarchical superlattice of chiral cubic crystalline ***,the crystalline material shows excellent robustness,and fascinating blueexcitable near-infrared thermally activated delayed fluorescence *** work not only exhibits that nanocage-type NCs can be smart as proteins to translate chiral primary structure into tertiary chiral hierarchical complexity,but also provides new insights into structure-to-superstructure,enabling bottom-up creation of higher-level hierarchical homochiral superlattice structures.

关键词： polyhydrido copper nanoclusters chiral polyhedral metallacage hierarchical homochiral assembly thermally activated delayed fluorescence

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Photo-induced Intramolecular Charge Transfer in Strained Organic Cage Containing Orthogonally Arranged Donors and Acceptors

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CCS Chemistry 2024年第8期6卷 1920-1928页

作者： Jingxuan Yang Run Shi Liang-Liang Mao hongyan Xiao Yi Zeng Guohong Liao Yuxiang Weng Xu-Bing Li Jiaqi Zhao Yunxuan Zhao Tierui Zhang Chen-ho tung Li-Zhu Wu Huan Cong Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190 Key Laboratory of Bio-Inspired Materials and Interfacial Science Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190 Beijing National Laboratory for Condensed Matter Physics Laboratory of Soft Matter PhysicsInstitute of PhysicsChinese Academy of SciencesBeijing 100190 University of Chinese Academy of Sciences Beijing 100049 Binzhou Institute of Technology Weiqiao-UCAS Science and Technology ParkBinzhou CityShandong 256606 Songshan Lake Materials Laboratory DongguanGuangdong 523808

Designing and creating molecular structures with precisely organized organic chromophores as donors and acceptors are critical for exploring photo-induced charge transfer *** and acceptor moieties can be incorporated to the confined skeletons of organic cages,thereby offering opportunities tomanipulate excited state characters for the development of novel photofunctional ***,we present the convergent synthesis and photophysical characterizations of an organic cage with anisotropic *** strained and rigid cage can be concisely prepared by connecting two distinct macrocycles through axial stacking strategy,featuring triarylamine and amide moieties as separate donors and acceptors,***-state and time-resolved spectra reveal photo-induced through-space intramolecular charge transfer and long-lived charge separation,thereby verifying the cage’s photocatalytic utility for efficient hydrogen production.

关键词： organic cage macrocycles photoinduced charge transfer through-space photocatalytic hydrogen evolution

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Comparative impact behaviours of ultra high performance concrete columns reinforced with polypropylene vs steel fibres

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Defence Technology（防务技术） 2024年第10期40卷 138-153页

作者： Thong M.Pham Harrison Hyde Maw K.Kaung Yan Zhuge Duong T.Tran Des Vlietstra tung M.Tran UniSA STEMUniversity of South AustraliaMawson LakesSA 5095Australia BG&E Pty Ltd Wellington StreetPerthWA6000Australia Austral Construction Pty Ltd St Georges TerracePerthWA6000Australia Centre for Infrastructural Monitoring and Protection(CIMP) Curtin UniversityKent StBentleyWA 6102Australia Barchip Australia Pty Ltd U 26 Qualtroughq StreetWoolloongabbaQueensland4102Australia Sustainable Developments in Civil Engineering Research Group Faculty of Civil EngineeringTon Duc Thang UniversityHo Chi Minh City72915Viet Nam

Polypropylene(PP) fibres have primarily used to control shrinkage cracks or mitigate explosive spalling in concrete structures exposed to fire or subjected to impact/blast loads, with limited investigations on capacity improvement. This study unveils the possibility of using PP micro-fibres to improve the impact behaviour of fibre-reinforced ultra-high-performance concrete(FRUHPC) columns. Results show that the addition of fibres significantly improves the impact behaviour of FRUHPC columns by shifting the failure mechanism from brittle shear to favourable flexural failure. The addition of steel or PP fibres affected the impact responses differently. Steel fibres considerably increased the peak impact force(up to 18%) while PP micro-fibres slightly increased the peak(3.-4%). FRUHPC significantly reduced the maximum midheight displacement by up to 3.%(under 20°impact) and substantially improved the displacement recovery by up to 100%(under 20° impact). FRUHPC with steel fibres significantly improved the energy absorption while those with PP micro-fibres reduced the energy absorption, which is different from the effect of PP-macro fibre reported in the literature. The optimal fibre content for micro-PP fibres is 1% due to its minimal fibre usage and low peak and residual displacement. This study highlights the potential of FRUHPC as a promising material for impact-resistant structures by creating a more favourable flexural failure mechanism, enhancing ductility and toughness under impact loading, and advancing the understanding of the role of fibres in structural performance.

关键词： Ultra high-performance concrete Steel fibre Polypropylene micro-fibre Fibre volume fraction Impact loading Pendulum tests Columns

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Asymmetric synthesis of tricyclic 6,5,5-fusedpolycycles by the desymmetric Pauson–Khandreaction

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Organic Chemistry Frontiers 2022年第6期9卷 1680-1685页

作者： Qi Teng Dong Chen Chen-ho tung Zhenghu Xu Key Lab of Colloid and Interface Chemistry of Ministry of Education School of Chemistry and Chemical EngineeringShandong UniversityNo.27 South Shanda RoadJinanShandong 250100China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic Chemistry Chinese Academy of SciencesShanghai 200032PR China Key Laboratory of Precise Synthesis of Functional Molecules of Zhejiang Province School of ScienceWestlake University18 Shilongshan RoadHangzhou 310024Zhejiang ProvinceChina

A new rhodium(I)–BINAP-catalyzed enantioselective desymmetric Pauson–Khand (PK) reaction of prochiral 1,6-enynes with CO has been developed. Diverse tricyclic 6,5,5-fused bowl type polycycles withthree continuous ch... 详细信息

关键词： fused symmetric chiral

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羧基功能化金纳米团簇的仿生结晶及其近红外磷光性质

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Science Bulletin 2024年第1期69卷 40-48页

作者：田伟东司为丹 Shana Havenridge 张成凯王芝 Christine M.Aikens 佟振合孙頔 School of Chemistry and Chemical Engineering State Key Laboratory of Crystal MaterialsShandong UniversityJinan 250100China Department of Chemistry Kansas State UniversityManhattan KS 66506USA

As an interdisciplinary product,water-soluble gold nanoclusters(AuNCs)stabilized by ligands containing carboxyl(-COOH)group have garnered significant attention from synthetic chemists and biologists due to their immense potential for biomedical ***,revealing the crystallographic structures of-COOH-functionalized AuNCs remains a ***,we successfully applied the salting-out method to obtain a series of high-quality single crystals of-COOH-functionalized Au_(25)nanoclusters and revealed their crystallographic ***,K_(3.Au_(25)(2-Hmna)_9(mna)_6]^(-)(Au25a)protected by 2-mercaptonicotinic acid features an unprecedented tetrameric Au_(4)(SR^(S))_(3.(SR^(S,N))_(2)staple motifs surrounding the icosahedral Au_(13.kernel,breaking the traditional perception on the structure of Au_(25)(SR)_(18).Au25a exhibits a distinct near-infrared emission at 970 nm with long lifetime of 8690 ns,which have been studied by transient absorption spectroscopy and time-dependent density functional *** work compensates for the research gap in the experimental structure of-COOHfunctionalized AuNCs and opens up a new avenue to explore their structure-property correlations.

关键词： Water-soluble gold nanoclusters Near-infrared phosphorescence Salting-out method

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Template-free large-scale synthesis of g-C3.4 microtubes for enhanced visible light-driven photocatalytic H2 production

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Nano Research 2018年第6期11卷 3462-3468页

作者： Chao Zhou Run Shi Lu Shang Li-Zhu Wu Chen-ho tung Tierui Zhang Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing 100190 China University of Chinese Academy of Sciences Beijing 100049 China

A template-free hydrothermal-assisted thermal polymerization method has been developed for the large-scale synthesis of one-dimensional （1D） graphitic carbon nitride （g-C3.4） microtubes. The g-C3.4 microtubes were obtained by simple thermal polymerization of melamine-cyanuric acid complex microrods under N2 atmosphere, which were synthesized by hydrothermal treatment of melamine solution at 180℃ for 24 h. The as-obtained g-C3.4 microtubes exhibited a large surface area and a unique one-dimensional tubular structure, which provided abundant active sites for proton reduction and also facilitated the electron transfer processes. As such, the g-C3.4 microtubes showed enhanced photocatalytic H2 production activity in lactic acid aqueous solutions under visible light irradiation （A 〉 420 nm）, which was - 3.1 times higher than that of bulk g-C3.4 prepared by direct thermal polymerization of the melamine precursor under the same calcination conditions.

关键词： graphitic carbon nitride(g-C3.4)microtubes photocatalytic water splitting visible light response

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