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Syntheses of new di-nuclear and tetra-nuclear lanthanide 9-anthracenecarboxylates:Magnetocaloric effect,slow magnetic relaxation and luminescent properties

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Journal of Rare Earths 2024年第6期42卷 1101-1109,I0004页

作者： Xing Liu Ruonan Yang Lu Zhang Jian Zhou Chunmei Huang Huahong Zou Zunhong Xiao Chongqing Key laboratory of Inorganic Functional Materials College of ChemistryChongqing Normal UniversityChongqing401331China Key laboratory for the {1. and Molecular Engineering of Medicinal Resources(Ministry of Education of China) School of Chemistry and Chemical Engineering of Guangxi Normal UniversityGuilin541004China School of chemistry and Materials Guizhou Normal UniversityGuiyang550025China

Lanthanide complex-based materials with magnetic and luminescent properties have received a great deal of attention,owing to their importantly potential applications in diverse *** this work,the 9-anthracenecarboxylic acid(9-Haca)as bridging ligand was applied in combination with optically activeπ-conjugated 2,4,6-tri(2-pyridyl)-1.3,5-triazine(tptz)to construct a series of new di-nuclear and tetranuclear lanthanide 9-anthracenecarboxylates[La_(2)(9-aca)_(6)(tptz)_(2)(μ-H_(2)O)]·0.25H_(2)O(1.,[Ln_(2)(9-aca)_(6)(tptz)_(2)(H_(2)O)_(2)]·0.5AQ·CH_(3)COOH_(2)H_(2)O[Ln=Sm(2a),Eu(2b),Gd(2c),Tb(2d),Dy(2e),Tm(2f);AQ=9,1.-anthracenedione]and[Ln_(4)(9-aca)_(1.)(tptz)_(2)(CH3COO)2]·H_(2)O[Ln=Eu(3a),Gd(3b),Dy(3c)].1.displays a di-nuclear centrosymmetric moiety[La_(2)(9-aca)_(6)(tptz)_(2)(μ-H_(2)O)]built up from two complex[La(9-aca)_(2)(tptz)]groups bridged by one H_(2)O molecule and two syn-syn-μ2-η1.η1.9-aca-bridging ligands,while 2a-2f are isostructural and co mprise another di-nuclear centrosymmetric moieties[Ln_(2)(9-aca)_(6)(tptz)_(2)(H_(2)O)_(2)]based on two complex[Ln(9-aca)_(2)(tptz)(H_(2)O)]groups connected by two syn-syn-μ2-η1.η1.9-aca-bridging ligands,3a-3c are isostructural and show tetra-nuclear centro symmetric moieties[Ln4(9-aca)1.(tptz)2(CH3COO)2]containing three types of coordination modes of *** present compounds offer the only examples of lanthanide 9-anthracenecarboxylates decorated by optically active *** investigations of 2a,2c-2f,and 3b-3c indicate that 3c is typical of slow relaxation of the magnetization,while 2c and 3b show significant magnetocaloric effect(MCE)with the value of-ΔSm of 5.26 J/(kg·K)at 4 K and 1..65 J/(kg·K)at 2 K(ΔH=7 T),*** luminescent properties were also studied and reveal that the characteristic luminescent properties of the 7r-conjugated aromatic ligands are introduced into magnetic lanthanide 9-anthracenecarboxylates,simultaneously exhibiting slow magnetic relaxation(or MCE)and luminescen

关键词： Lanthanide complexes Luminescence Magnetic properties Magnetocaloric effect Slow magnetic relaxation Rare earths

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Indole-3-acetic acid,a potential therapeutic target in Alzheimer's disease

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Science Bulletin 2024年第2期69卷 146-147页

作者： Jinghong Li Department of chemistry Center for Bioanalytical ChemistryKey Laboratory of Bioorganic Phosphorus Chemistry and Chemical Biology(Ministry of Education)Tsinghua UniversityBeijing 100084China

Alzheimer's disease(AD)is a chronic and progressive neurodegenerative disease that is characterized by the presence of amyloid-β(Ap)plaques,hyperphosphorylated microtubule-associated tau protein(p-tau)neurofibrillary tangles and neuronal *** to recent data,AD is the most common global cause of dementia in the *** billions of dollars have been invested in research,there is still no effective drug for the treatment of AD;consequently,this disease imposes a huge burden on individuals,families,and healthcare systems[1.2].

关键词： Alzheimer tau degeneration

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Precision design of Ti sites for unprecedented catalytic performance

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National Science Review 2024年第7期11卷 67-68页

作者： Haoquan Zheng Shunai Che Key laboratory of Applied Surface and Colloid {1. Ministry of Education School of Chemistry and Chemical Engineering Shaanxi Normal University School of chemistry and Chemical Engineering Shanghai Jiao Tong University

In 1.83, Taramasso et al. incorporated titanium(Ti) into porous silica frameworks to endow Ti sites with catalytic oxidation ability [1.. Nowadays, catalytic oxidation reactions using titanium silicate materials have ...

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Single-atom Zn confined in hierarchical hollow microstructure as an acid/base-resistant microwave absorption materials

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Nano Research 2024年第8期17卷 6785-6794页

作者： Yue Lou Jiao Li Xiaokun Li Zhenyu Zhu Zhan Shi Biao Xu School of chemistry and Chemical Engineering Nanjing University of Science and TechnologyNanjing 210094China State Key laboratory of Inorganic Synthesis and Preparative {1. College of ChemistryJilin UniversityChangchun 130012China

Developing acid/base-resistant and low-price microwave-absorbing materials with lighter weight is highly desired for practical applications in extreme ***,we demonstrate the successful synthesis of the N-doped porous carbon(NC)material with hierarchical pore structure by the spray pyrolysis *** large specific surface area(SBET=707.53 m^(2)·g^(−1.)of materials enables multiple scattering of incident electromagnetic waves,and N doping greatly enhances the electrical conductivity of the ***,single-atom Zn can adjust the local electronic structure of adjacent sites such as carbon and nitrogen atoms,induce the center of polarization,and thus change the dielectric and electronic properties of the host *** porous carbon coating of single-atom Zn avoids the deterioration of electromagnetic parameters caused by the accumulation of magnetic particles under high-temperature *** the same time,they can also be used in various complex environments,such as acidic and basic ***,NC-1.00,with high surface area,low density,and good chemical stability,obtained a minimum reflection loss(RLmin)of−50.5 dB and an effective absorption bandwidth(EAB)exceeding 5.1.GHz at the thickness of 1.9 *** soaking in the strong acid and base solution,the electromagnetic wave absorption performance of the material decreased by1.%.Widely available raw materials and a simple preparation scheme are expected to expedite industrial mass production for this novel type of materials.

关键词： hierarchical hollow microstructure microwave absorption metal-organic framework(MOF) impedance matching singleatom Zn acid/base-resistant

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High-Performanceα-Diimine Nickel Complexes for Facile Access of PE Elastomers with Exceptional Material Properties

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Chinese Journal of Polymer Science 2024年第5期42卷 620-635,I0008页

作者： Li-Dong Qin Xin-Yu Wang Qaiser Mahmood Zhi-Xin Yu Yi-Zhou Wang Song Zou Tong-Ling Liang Wen-Hua Sun School of Pharmaceutical Sciences Changchun University of Chinese MedicineChangchun130117China chemistry and Chemical Engineering Guangdong {1. Shantou515031China Key laboratory of Engineering Plastics and Beijing National laboratory for Molecular Science Institute of ChemistryChinese Academy of SciencesBeijing100190China

For practicable elastomeric polyethylene,achieving high catalyst thermal stability and activity,along with precise control of polymer properties such as branching density,molecular weights,and distribution,is crucial but *** this study,two sets of symmetricalα-diimine nickel complexes,each comprising four nickel bromide or chloride complexes,were synthesized and investigated their performance for ethylene polymerization under various reaction *** activation with either Et2AlCl or MMAO cocatalysts,these complexes displayed not only high activity but also generated high molecular weight polyethylenes with controlled polydispersity and a substantial number of *** catalyst with the least steric hindrance displayed the remarkable high activity(up to 1.2×1.^(7) g·mol^(-1.·h^(-1.).Notably,nickel bromides demonstrated higher activity compared to their chloride *** investigation into the effect of reaction temperature on catalytic performance revealed that NiBrMe-MMAO system displayed high thermal stability(activity up to 2.51.1.^(6) g·mol^(-1.·h^(-1. at 1.0℃)and consistently yielded high polymer molecular weights with narrow polydispersity over a broad temperature range of 30-1.0℃.Of significant note,mechanical analysis of the resulting polyethylene demonstrated excellent ultimate tensile strength and high strain at ***,the polyethylene sample prepared at 1.0℃exhibited ultimate tensile strength up to 1. MPa with 1.63%maximum strain at break and a strain recovery of up to 54.9%after ten cycles at a fixed strain of 300%,indicating excellent material properties of prepared thermoplastic polyethylene elastomers(TPE).

关键词： Thermoplastic polyethylene elastomers α-Diimine nickel pre-catalysts Ethylene polymerization Mechanical properties Highly branched polyethylene

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Highly selective photocatalytic reduction of CO_(2) to CH_(4) on electron-rich Fe species cocatalyst under visible light irradiation

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Carbon Energy 2024年第1期6卷 255-266页

作者： Qianying Lin Jiwu Zhao Pu Zhang Shuo Wang Ying Wang Zizhong Zhang Na Wen Zhengxin Ding Rusheng Yuan Xuxu Wang Jinlin Long State Key laboratory of Photocatalysis on Energy and Environment College of ChemistryFuzhou UniversityFuzhouChina

Efficient photocatalytic reduction of CO_(2) to high-calorific-value CH4,an ideal target product,is a blueprint for C_(1.industry relevance and carbon neutrality,but it also faces great ***,we demonstrate unprecedented hybrid SiC photocatalysts modified by Fe-based cocatalyst,which are prepared via a facile impregnation-reduction method,featuring an optimized local electronic *** exhibits a superior photocatalytic carbon-based products yield of 30.0μmol g^(−1. h^(−1. and achieves a record CH_(4) selectivity of up to 94.3%,which highlights the effectiveness of electron-rich Fe cocatalyst for boosting photocatalytic performance and ***,the synergistic effects of directional migration of photogenerated electrons and strongπ-back bonding on low-valence Fe effectively strengthen the adsorption and activation of reactants and intermediates in the CO_(2)→CH_(4) *** study inspires an effective strategy for enhancing the multielectron reduction capacity of semiconductor photocatalysts with low-cost Fe instead of noble metals as cocatalysts.

关键词： artificial synthesis of CH_(4) electronic structure optimization Fe species cocatalyst photocatalytic CO_(2) reduction SiC

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Synthesis and characterization of iron clusters with an icosahedral [Fe@Fe1.]1.+ 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 {1. 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 {1. 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*）4W4S1.(Fe@Fe1.) cluster(Tp*=tris（3,5-dimethyl-1.pyrazolyl）borate（1.）),which features a rare trideca-nuclear,icosahedral[Fe@Fe1.] 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 1.-electron shell-closing of the [Fe@Fe1.]1.+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： Fe1. cluster iron-sulfur cluster low-valence iron iron−iron bond high spin complex

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Polyethylene to gasoline via a self-supplied hydrogen strategy

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Science China chemistry 2024年第10期67卷 3187-3188页

作者： Yong Tang State Key laboratory of Organometallic {1. Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Polyethylenes(PEs)are one of the most widely used plastics in almost every aspect of modern life and are produced on a huge scale(a market volume of 1.0.1. million metric tons worldwide in 2022)[1..A large portion of the PEs are used once and discarded as waste,which caused severe problems such as plastic pollution as well as a waste of the fossoil resource.

关键词： pollution plastics strategy

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Furfural residues derived nitrogen-sulfur co-doped sheet-like carbon: An excellent electrode for dual carbon lithium-ion capacitors

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Green Energy & Environment 2024年第9期9卷 1427-1439页

作者： Xiaoying Guo Yan Qiao Zonglin Yi Christian Marcus Pedersen Yingxiong Wang Xiaodong Tian Peide Han College of Materials Science and Engineering Taiyuan University of Technology State Key laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences University of Chinese Academy of Sciences CAS Key laboratory of Carbon Materials Institute of Coal Chemistry Chinese Academy of Sciences Department of chemistry University of Copenhagen Universitetsparken 5 College of chemistry Taiyuan University of Technology

The state-of-the-art lithium-ion capacitors （LICs）,consisting of high-capacity battery-type anode and high-rate capacitor-type cathode,can deliver high energy density and large power density when comparing with traditional supercapacitors and lithium-ion batteries,***,the ion kinetics mismatch between cathode and anode leads to unsatisfied cycling lifetime and anode *** efforts have been devoted to solving the abovementioned *** promising strategy is altering high conductive hard carbon anode with excellent structural stability to match with activated carbon cathode,assembling dual-carbon *** this contribution,one-pot in-situ expansion and heteroatom doping strategy was adopted to prepare sheet-like hard carbon,while activated carbon was obtained involving *** persulfate was used as expanding and doping agent *** furfural residues （FR） were served as carbon *** resulting hard carbon （FRNS-HC） and activated carbon （FRNS-AC）show excellent electrochemical performance as negative and positive electrodes in a lithium-ion battery （LIB）.To be specific,374.2 m Ah g-1.nd 1.3.1.m Ah g-1.an be achieved at 0.1.A g-1.nd 5 A g-1.hen FRNS-HC was tested as *** combined with a highly porous carbon cathode (SBET=2961.m2g-1. synthesized from the same precursor,the LIC showed high specific energy of1.7.67 Wh kg-1.t approximately 1.9.93 W kg-1.and outstanding cycling life with negligible capacitance fading over 1.00 *** study could lead the way for the development of heteroatom-doped porous carbon nanomaterials applied to Li-based energy storage applications.

关键词： Furfural residue Ammonium persulfate Sheet-like carbon Lithium-ion capacitors Hard carbon

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Anchoring heterometallic cluster on P-doped carbon nitride for efficient photocatalytic nitrogen fixation in water and air ambient

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Chinese Chemical Letters 2024年第4期35卷 176-180页

作者： Chao-Long Chen Rong Chen La-Sheng Long Lan-Sun Zheng Xiang-Jian Kong Collaborative Innovation Center of chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Light-driven nitrogen fixation to produce ammonia is a green and economical technology of nitrogen reduction but is still quite challenging, especially in an air atmosphere without any sacrificial ***, we demonstrate efficient photocatalytic nitrogen fixation using water and air directly by loading lanthanide–transition metal(4f–3d) cluster NdCo_(3) on two-dimensional P-doped graphitic carbon nitrides(PCN) material surface. Benefiting from the increase in the number of nitrogen vacancies(NVs) and highly matched band gap structure and excellent hole trapping ability of clusters, the NdCo_(3)/PCN photocatalyst exhibits efficient nitrogen reduction activity with 371.in air) and 825 μmol h^(-1.g^(-1.(in pure nitrogen)without any sacrificial reagents. The introduction of potassium sulfate inhibits hydrogen production and promotes nitrogen reduction activation. This work suggests that anchoring precisely structured clusters on 2D materials may enhance photocatalytic nitrogen reduction under normal temperature and pressure.

关键词： Photocatalytic Nitrogen fixation 4f-3d Cluster Air atmosphere

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