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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, Au32, 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 Ag32, which is embraced by a robust cyclic anionic passivation layer of（KPO4）10. This Ag32kernel 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 Ag32kernel and Ag70shell, passivating the Ag32silvery fullerene and templating the Ag70shell. The ~tBuPhS-and CF3COO-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 CF3COO-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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Terminal-selective C（sp3）–H borylation of unbranched alkanes enabled by intermolecular radical sampling and LMCT photocatalysis

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National Science Review 2024年第5期11卷 96-98页

作者： Zhexuan Lei jie Wu department of chemistry National University of Singapore

The selective functionalization of C（sp3）–H bonds with subtle differences in alkanes is highly sought after due to its atom-and step-efficiency. The activation of C（sp3）–H bonds through hydrogen atom transfer （HAT） has been extensively exploited to produce a valueadded product from unfunctionalized material [1,2].

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Strong and tough chitin hydrogel constructed by dehydration and rehydration strategy

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Nano Research 2024年第9期17卷 8192-8199页

作者： Rui-Rui Liu Li-Bo Mao shu-Hong Yu Division of Nanomaterials and chemistry Hefei National Research Center for Physical Sciences at the MicroscaleDepartment of ChemistryInstitute of Biomimetic Materials and ChemistryAnhui Engineering Laboratory of Biomimetic MaterialsUniversity of Science and Technology of ChinaHefei 230026China Institute of Innovative Materials Department of Materials Science and EngineeringDepartment of ChemistrySouthern University of Science and TechnologyShenzhen 518055China

As a renewable,biocompatible,biodegradable soft material,chitin hydrogels have better advantages in stability,antibacterial activity,antifouling,cost,immunogenicity,and so on than most polymer ***,compared with other widely used polymer hydrogels with high strength and toughness,the practical applications of chitin-based hydrogels have been limited by their weak mechanical properties,such as cartilage repair and meniscus ***,we present the design and fabrication of chitin hydrogels with excellent mechanical strength and toughness by a dehydration and rehydration *** sequential dehydration and rehydration processes,the crystalline domains in the chitin hydrogels can be properly *** optimized crystallinity,the elastic modulus of the chitin hydrogels exceeds all previously reported values,and the fracture toughness is even comparable to some synthetic polymer hydrogels,while maintaining a high-water-content of about 80 wt.%.At the same water content,the mechanical properties of the chitin hydrogels are positively correlated with the hydrogel crystallinity,which proves that the change of mechanical properties of hydrogels is not simply dependent on weight *** hydrogels can be further strengthened by incorporating other biopolymers that are intrinsically weak,which makes the hydrogels promising for applications in fields such as cartilage repair and meniscus ***,the hydrogels enable loading and release of water-soluble and poorly water-soluble *** highly extendable strengthening and toughening strategy of chitin and chitin-based biopolymer hydrogels paves the way for their widely applications.

关键词： chitin hydrogel crystallinity rehydration chemical transformation strong and tough

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Combining cisplatin and a STING agonist into one molecule for metalloimmunotherapy of cancer

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National Science Review 2024年第1期11卷 107-119页

作者： shuren Zhang Dongfan Song Wenhao Yu Ji Li Xiaoyu Wang Yachao Li Zihan Zhao Qi Xue Jing Zhao jie P.Li Zijian Guo State Key Laboratory of Coordination chemistry School of Chemistry and Chemical EngineeringChemistry and Biomedicine Innovation Center (ChemBIC) Nanjing University department of Urology Afflliated Drum Tower HospitalMedical SchoolNanjing University Nanchuang (Jiangsu)Institute of chemistry and Health

Mounting evidence suggests that strategies combining DNA-damaging agents and stimulator of interferon genes(STING) agonists are promising cancer therapeutic regimens because they can amplify STING activation and remodel the immunosuppressive tumor microenvironment. However, a single molecular entity comprising both agents has not yet been developed. Herein, we designed two PtIV-MSA-2 conjugates(Ⅰand Ⅱ) containing the DNA-damaging chemotherapeutic drug cisplatin and the innate immuneactivating STING agonist MSA-2; these conjugates showed great potential as multispecific small-molecule drugs against pancreatic cancer. Mechanistic studies revealed that conjugate Ⅰ upregulated the expression of transcripts associated with innate immunity and metabolism in cancer cells, significantly differing from cisplatin and MSA-2. An analysis of the tumor microenvironment demonstrated that conjugate I could enhance the infiltration of natural killer(NK) cells into tumors and promote the activation of T cells, NK cells and dendritic cells in tumor tissues. These findings indicated that conjugate I, which was created by incorporating a Pt chemotherapeutic drug and STING agonist into one molecule, is a promising and potent anticancer drug candidate, opening new avenues for small-molecule-based cancer metalloimmunotherapy.

关键词： platinum drug STING agonist single-molecule multitarget metalloimmunology

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High-rate lithium-ion battery performance of a ternary sea urchin-shaped CoNiO_(2)@NiP_(6)Mo_(18)/CNTs composites

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Journal of Energy chemistry 2024年第9期96卷 516-525页

作者： Li-ping Cui shuang Sun Kai Yu shu Zhang Mei-lin Wang Jia-jia Chen Bai-bin Zhou Key Laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Chemistry and Chemical EngineeringHarbin Normal UniversityHarbin 150025HeilongjiangChina State Key Laboratory of Physical chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringCollaborative Innovation Centre of Chemistry for Energy MaterialsXiamen UniversityXiamen 361005FujianChina

Bimetallic oxides are attractive anode materials for lithium-ion batteries(LIBs)due to their large theoretical ***,the low conductivity,short cycle life,and poor rate capability are the bottlenecks for their further *** overcome above issues,the basket-like polymolybdate(NiP_(6)Mo_(18))and carbon nanotubes(CNTs)were uniformly embedded on the urchin-shaped CoNiO_(2)nanospheres to yield a ternary composites CoNiO_(2)@NiP_(6)Mo_(18)/CNTs via electrostatic *** multi-level morphology of urchin spinules accelerates the diffusion rate of Li^(+);CNT improves the conductivity and enhances cycle stability of the material;and heteropoly acid contributes more redox activity ***,CoNiO_(2)@NiP_(6)Mo_(18)/CNTs as an anode of LIBs exhibits a high initial capacity(1396.7 mA h g^(−1)at 0.1 A g^(−1)),long-term cycling stability(750.2 mA h g^(−1)after 300 cycles),and rate performance(450.3 mA h g^(−1)at 2 A g^(−1)),which are superior to reported metallic oxides anode of *** density functional theory(DFT)and kinetic mechanism suggest that CoNiO_(2)@NiP_(6)Mo_(18)/CNTs delivers an outstanding pseudocapacitance and rapid Li^(+)diffusion behaviors,which is due to the rich surface area of the urchin-like CoNiO_(2)with the uniform embeddedness of NiP_(6)Mo_(18)and *** study provides a new idea for optimizing the performance of bimetallic oxides and developing high-rate lithium-ion battery composites.

关键词： Bi-metal oxides Transition metal oxides Polyoxometalates Nanocomposite LIBs

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How interfacial electron-donating defects influence the structure and charge of gold nanoparticles on TiO_(2)support

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Nano Research 2024年第7期17卷 5965-5974页

作者： Guang-jie Xia Yu Fu Wei Cao Jun Li yang-Gang Wang department of chemistry and Guangdong Provincial Key Laboratory of Catalysis Southern University of Science and TechnologyShenzhen 518055China School of Physical Sciences Great Bay UniversityDongguan 523000China department of chemistry Tsinghua UniversityBeijing 100084China

The reduction degree of TiO_(2)support is critical to the performances of metal *** many previous theoretical calculations,only the bridge oxygen vacancy(Ov)was considered as the electron-donating defect on reduced rutile TiO_(2)(r-TiO_(2−x))***,titanium adatoms(Tiad.),oxidized titanium islands(***),and acid hydroxyls(ObrH)also exist at the metal/support *** conducting density functional theory(DFT)calculations and ab initio molecular dynamics(AIMD)simulations,we compared r-TiO_(2−x)surfaces with Ov,Tiad.,***,and ObrH sites loaded with Au nanoparticles(NPs).The results showed the Au NPs were oxygen-phobic but titanium-philic,resulting in wetting of Ov and *** short contact with *** and *** Bader charges of Au NPs(QM)showed a good linear relationship with the ideal number of donating electrons(Ne)from the defective sites(QM=−KeNe+QM,S),demonstrating the intrinsic electron allocation at the *** Ov,Tiad.,and *** exhibited similar slopes(Ke),relatively steeper than that of *** means in the scope of Au NP charge state,the *** *** have a close electron-donating ability with Ov,but the ObrH donates relatively fewer *** linear relationship can be extended approximately to other *** higher the metal work function,the steeper the Ke for easier electron donation from defective *** stronger the metal oxygen affinity,the more positive the intercept(QM,S).That explains the easy generation of metallic or negative Pt and Au NPs on r-TiO_(2−x),but hard for Cu and Zn in *** provides theoretical guidance for regulating the charge of metal NPs over TiO_(2−x)supports.

关键词： metal-support interaction titanium oxide oxygen vacancy surface hydroxyl titanium adatom

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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

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Fluorescent carbon dots synthesized in solid phase and air for application in LEDs

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Nano Research 2024年第9期17卷 8495-8503页

作者： Wei-jie Zheng Zhao-Nan Sun Yi-Ming Wang Huan-Ming Xiong department of chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan UniversityShanghai 200438China

Carbon dots(CDs)have been widely adopted as optical materials because of their excellent luminescent ***,most of the reported synthetic methods are conducted in solvents,especially hydrothermal/solvothermal reactions,leading to intractable problems such as toxic and flammable solvents,complex and inseparable by-products,and dangerously high pressures and ***-phase synthesis of CDs in air is an effective solution to overcome the above issues,but solid reactions always result in uncontrolled growth and agglomeration of *** this study,some inorganic salts are selected as catalysts for synthesizing CDs in solid states and air,which also play as dispersants to hinder CDs *** the meantime,some aromatic derivatives containing hydroxyl and amino groups are chosen as carbon sources,ground with the optimized catalyst,and then heated together in *** production yields are affected by the reaction time and reactant ratio,while the graphitization degrees of the CDs are determined by the reaction *** IG/ID value of their Raman spectra increases from 0.59 to 0.85,and the particle size decreases from 2.5 to 1.4 nm when the synthesis temperature is increased from 200 to 280℃.The as-prepared CDs show emission peaks ranging from 366 to 606 nm,with the photoluminescence(PL)quantum yield up to 53%.Their emission color variation mainly results from different carbon sources,which can be ascribed to the differences in the element composition,functional groups,and graphitic nitrogen content of these *** dispersing CDs of different concentrations into polyvinyl alcohol(PVA)and combining them with blue LEDs,cold,standard,and warm white light emitting devices(WLEDs)are prepared,with a color rendering index(CRI)up to *** the as-prepared CDs have antioxidant ability at high temperature,the as-prepared WLEDs have long lifespans,remaining the effective white luminescence after 72 h continuous work.

关键词： carbon dot solid-phase synthesis white LED photoluminescence inorganic salt catalysis

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SO_(2)-Insertion induced enantioselective oxysulfonylation to access β-chiral sulfones with quaternary carbon stereocenters

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Science China chemistry 2024年第3期67卷 908-913页

作者： Jun Zhang Xuefeng Wang Peiqi Wang Jiayuan Fang Shaoyu Li jie Wu School of Pharmaceutical and Chemical Engineering&Institute for Advanced Studies Taizhou UniversityShanghai 200438China department of chemistry Fudan UniversityShanghai 200438China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of chemistry and Chemical Engineering Henan Normal UniversityXinxiang 453007China

β-Chiral sulfones are structural motifs widely found in natural products and bioactive molecules, while also serving as important intermediates for the synthesis of valuable chiral scaffolds. In contrast to the rapid growth of sulfur dioxide insertion chemistry over the last decade, enantioselective catalytic variants for accessing β-chiral sulfones, especially those bearing a quaternary carbon stereocenter, remain rare. Herein, we report an enantioselective copper/bisoxazoline catalyzed oxysulfonylation of alkenes to yield isoxazolinyl-containing β-chiral sulfones bearing quaternary carbon stereocenters with moderate to excellent yields and up to 96:4 er. The advantage and irreplaceability of this sulfur dioxide insertion catalytic system have been demonstrated by achieving transformations clearly unavailable with the previously reported sulfonyl chloride system. Additionally,the recoverability of the new-developed bisoxazoline ligand L9 and its reusability without any erosion of the catalytic activity and enantioselectivity further demonstrate the usefulness of the protocol.

关键词： β-chiral sulfones sulfur dioxide insertion oxysulfonylation copper catalysis enantioselectivity

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Phase modulation of nickel-tin alloys in regulating electrocatalytic nitrogen reduction properties

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Rare Metals 2024年第6期43卷 2851-2858页

作者： Lin Wang Hang-Ning Liu Xin Meng Chang-Hui Sun Hai-Dong Liu Liang-Yu Gong Zhen-Hua Yan jie Wang College of chemistry and Pharmaceutical Sciences Qingdao Agricultural UniversityQingdao 266109China department of chemistry-Angstrom Laboratory Uppsala University75121UppsalaSweden Key Laboratory of Advanced Energy Materials chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China

Electrocatalytic nitrogen reduction reaction(NRR)is one of the attractive methods for ammonia(NH_(3))production at ambient conditions,but the catalytic performance largely depends on the physical properties of the ***,Ni-Sn alloy nanoparticles with well-controlled physical properties have been synthesized via a simple two-step method,which are applied as efficient electrocatalysts for the NRR.

关键词： alloys alloy nickel

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