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A highly reduced Mo_(74) polyoxometalate featuring high proton conductivity accessed by building block strategy

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Science China chemistry 2024年第3期67卷 862-868页

作者： Shi-Yi Liu Xue-Xin Li Wei-Chao Chen Kui-Zhan Shao Xin-Long Wang Chao Qin Zhong-Min Su Key Laboratory of Polyoxometalate and Reticular Material chemistry of Ministry of Education Department of ChemistryNortheast Normal UniversityChangchun 130024China State Key Laboratory of Supramolecular Structure and Materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China

Highly reduced polyoxometalates(POMs) are predicted to be used as rather high energy density materials;however,it still suffers from the limited cluster species and reduction *** we demonstrate that it is possible to employ the building block strategy to generate a highly reduced polyoxomolybdate(C_(2)H_(8)N)_(14)(NH_(4))_(4)H_(14)[Mo_(48)-ⅤMo_(26)ⅥO_(202)(OH)_(12)(SO_(4))_(6)]·46H_(2)O(Mo_(74)).The fundamental Mo-based{Mo_x}(x=4,5,and 6) building blocks,which are templated by tetra-coordinated anions{MoO_(4)}or{SO_(4)},not only lay foundation for the formation of Mo_(74) featuring an unprecedented reduction ratio of 65%,but also give rise to SBBs-mediated(secondary building blocks) supramolecular dense packing interactions among the isolated Mo_(74) clusters that are favorable for proton ***,high proton conductivity(2.04×10^(-2)S cm^(-1)) had been realized at 50℃ and 90% relative humidity,revealing one of the well-known POMs-based crystalline proton conducting *** result highlights that this building block approach possesses great potential in producing highly reduced POM systems that can achieve controllable reduced ratio and desirable properties.

关键词： polyoxometalate building block molybdenum highly reduced state proton conduction

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

Interface matters: how to print single atoms?

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Science China Materials 2024年第3期67卷 1002-1003页

作者： Dingsheng Wang department of chemistry Tsinghua UniversityBeijing 100084China

Recently, single-atom catalysts (SACs) have emerged as highly efficient catalysts for multiple reactions, making them as the new stars in the catalytic field [1–7]. Single metal atoms can be anchored onto various supports (such as defective carbon, oxides, sulfides and carbides [8]), endowing single atoms with diverse electronic and coordination structures.

关键词： sulfide coordination oxides

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Record-high efficiency perovskite LEDs achieved by accelerating radiative recombination

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Science China Materials 2024年第9期67卷 3039-3040页

作者： Feng Gao department of Physics Chemistry and BiologyLink?ping University

Light-emitting diodes(LEDs) have revolutionized the lighting and displays due to their superior energy efficiency. The increasing demand for more efficient and brighter thin-film LEDs in flat-panel displays and solid-state lighting applications has driven extensive research into perovskite materials, which show great promise for high brightness and efficiency.

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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

Facile synthesis of transition metal complexes with five coplanar metal-carbon σ-bonds

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National Science Review 2024年第4期11卷 11-12页

作者： Guocheng Jia department of chemistry Hong Kong University of Science and Technology

Carbon is one of the most important elements in chemistry, forming a vast number of organic compounds. It can also form a variety of organometallic compounds with a metal–carbon bond. Metal alkyl, carbene and carbyne complexes are classical examples of organometallic compounds. A particularly interesting class of organometallic compounds are all-carbon metallacycles formed by combination of a metal and a hydrocarbon chain serving as a chelating agent with only carbon atoms as the donor atoms. Many interesting monocyclic metallacycles made of a chelating bidentate hydrocarbon chain are known, for example, metallacyclobutadienes, metallacyclopentadienes and metallabenzenes[1].

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Heavier Group 14 Congeners of Metalla-isobenzenes:Access to Metalla-isosilabenzene and Metalla-isogermabenzene by One-Pot Reactions

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Chinese Journal of chemistry 2024年第10期42卷 1121-1127页

作者： Jinyu Zhao Yapeng Cai Xin Yang Hong Zhang department of chemistry Xiamen UniversityXiamenFujian 361005China

Metalla-isosilabenzenes and metalla-isogermabenzenes have been successfully synthesized by the formal[5+1]-cycloaddition of diethynylsilane or diethynylgermane with simple metal *** is the first example of a heavier Group 14 metalla-isobenzene isomer bearing a cumulative double bond motif within a *** novel complexes were fully characterized by NMR spectroscopy and single-crystal X-ray diffraction *** stabilization of the cyclic metal-vinylidene complexes has been analyzed using density functional theory(DFT)*** the metalla-isosilabenzenes bearing Si—H bond were treated with the trityl salt as a hydride scavenger,the formation of silylium cation was observed *** of metalla-isosilabenzenes and metalla-isogermabenzenes can readily undergo migratory insertion reactions to furnish siloles or germoles.

关键词： Metalla-isosilabenzene Metalla-isogermabenzene Density functional calculations Cycloaddition Metallacycles

Durable poly(binaphthyl-co-p-terphenyl piperidinium)-based anion exchange membranes with dual side chains

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Journal of Energy chemistry 2024年第2期89卷 324-335,I0008页

作者： Weiting Gao Xuelang Gao Qiugen Zhang Aimei Zhu Qinglin Liu department of Chemical&Biochemical Engineering Fujian Provincial Key Laboratory of Theoretical and Computational ChemistryThe College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina department of chemistry Pohang University of Science and Technology(POSTECH)Pohang 790-784South Korea

Building well-developed ion-conductive highways is highly desirable for anion exchange membranes(AEMs).Grafting side chain is a highly effective approach for constructing a well-defined phaseseparated morphological structure and forming unblocked ion pathways in AEMs for fast ion *** of side chains can further enhance phase separation due to the superhydrophobic nature of fluorine ***,their electronic effect on the alkaline stability of side chains and membranes is rarely ***,fluorine-containing and fluorine-free side chains are introduced into the polyaromatic backbone in proper configuration to investigate the impact of the fluorine terminal group on the stability of the side chains and membrane *** poly(binaphthyl-co-p-terphenyl piperidinium)AEM(QBNp TP)has the highest molecular weight and most dimensional stability due to its favorable backbone arrangement among ortho-and meta-terphenyl based ***,by introducing both a fluorinated piperidinium side chain and a hexane chain into the p-terphenyl-based backbone,the prepared AEM(QBNp TP-QFC)presents an enhanced conductivity(150.6 m S cm^(-1))and a constrained swelling at 80℃.The electronic effect of fluorinated side chains is contemplated by experiments and *** results demonstrate that the presence of strong electro-withdrawing fluorine groups weakens the electronic cloud of adjacent C atoms,increasing OH^(-)attack on the C atom and improving the stability of piperidinium *** QBNp TP-QFC possesses a robust alkaline stability at 80℃(95.3%conductivity retention after testing in 2 M Na OH for 2160 h).An excellent peak power density of 1.44 W cm^(-2)and a remarkable durability at 80℃(4.5%voltage loss after 100 h)can be observed.

关键词： Anion exchange membranes Backbone structure Fluorinated side chain Alkaline stability

Electric-field-controlled highly regioselective thiocyanation of N-containing heterocycles

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Science China chemistry 2024年第4期67卷 1263-1269页

作者： Ming Gong Qian Wu Jung Keun Kim Mengmeng Huang Yabo Li Yangjie Wu Jong Seung Kim Henan Key Laboratory of Chemical Biology and Organic chemistry Key Laboratory of Applied Chemistry of Henan UniversitiesCollege of ChemistryZhengzhou UniversityZhengzhou 450052China department of chemistry Korea UniversitySeoul 02841Korea

Achieving highly regioselective synthesis in organic chemistry is challenging due to the uncontrollable orientation between reacting *** electric fields(EEFs)can influence the reactivity and selectivity of the substrate by causing directional ***,scalable and efficient techniques for using EEFs as“smart catalysts”have been lacking,hindering their *** this study,we present a novel method for modifying the regioselectivity of quinoxaline-2(1H)-ones by functionalizing their C7-position using the electric double layer(EDL)*** approach led to moderate to good yields of the corresponding C7-thiocyanation *** calculations and control experiments demonstrated that EEFs could reverse the regioselectivity of quinoxaline-2(1H)-ones,allowing the C7-thiocyanation to proceed via a radical reaction ***,the resulting 7-thiocyano-1-methylquinoxaline-2(1H)-ones exhibited promising AIE *** work showcases a promising strategy for achieving highly regioselective functionalization by aligning the electric field with the desired reaction/bond axis.

关键词： electric fields reaction-axis rule electric double layer C7-thiocyanation C-S bond formation

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