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Polyoxometalate-based flexible conductive materials with superionic conductivity

Science China chemistry 2024年第10期67卷 3299-3309页

作者： Yuxin Wang Shuping Xue Jun Geng Ying Lu Teng Li Xiaozheng Duan Xue Bai Yanli Yang Jingqi Yang Shuxia Liu Key Laboratory of Polyoxometalate and Reticular Material chemistry of Ministry of Education College of ChemistryNortheast Normal UniversityChangchun 130024China State Key Laboratory of Polymer Physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Flexible ion-conductive materials exhibit intriguing advantages for applications in flexible electronic ***,the further enhancement of their conductivity within environmental limitations is an urgent demand for the development of flexible electronic devices,yet remains as a great ***,we report a“dual-acid”strategy,via the encapsulation of two acids,H_(3)PW_(12)O_(40)(HPW) and NH_(2)SO_(3)H(SA),with synergistic interaction into poly(vinyl alcohol)-glycerol(PVA-Gly) hydrogel,to achieve polyoxometalate(POM)-based flexible materials with superionic conductivity under various environmental *** a representative example,the prepared PVA-Gly/HPW-SA-20% hydrogel presents an ultrahigh proton conductivity ranging from -30℃(3.33×10^(-2)S cm^(-1)) to room temperature(2.78×10^(-1)S cm^(-1)) under ambient ***,the PVA-Gly/HPW-SA-20% hydrogel exhibits remarkable advantages in anti-freezing,mechanical flexibility and self-adhesiveness,making it a promising multifunctional electrolyte for flexible electronic *** experimental results and molecular dynamics(MD) simulations jointly demonstrate that SA bridges HPW clusters to form a dense proton transport pathway induced by multiple electrostatic and hydrogen bonding interactions between SA and HPW counterparts,which contributes to the high-level proton conductivity of the PVA-Gly/HPW-SA-20% *** work provides new insights into the design of POM-based flexible materials with superionic conductivity.

关键词： polyoxometalates proton conduction dual-acid effect hydrogel molecular dynamics simulation

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Vacancy engineering induced reaction kinetics enhancement of cobalt metaphosphate for pH-universal hydrogen evolution

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Nano Research 2024年第5期17卷 3879-3887页

作者： Yuting Chen Tian Meng Zhicai Xing Yueying Yan Yang Yang Bohan Yao Dewen Wang Xiurong Yang State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

Developing efficient pH-universal hydrogen evolution reaction(HER)catalysts is critical in the field of water electrolysis,however,which is severely hampered by the sluggish kinetics in alkaline ***,a ruthenium(Ru)incorporation induced vacancy engineering strategy is firstly proposed to precisely construct oxygen vacancy(V_(O))-riched cobalt-ruthenium metaphosphate(CRPO)for high-efficiency pH-universal *** V_(O) modifies the electronic structure,improves the superficial hydrophilic and gas spillover capacity,it also reduces the coordination number of Ru atoms and regulates the coordination *** calculations indicate that Ru tends to adsorb H_(2)O and H^(*),whereas V_(O) tends to adsorb OH^(-),which greatly promotes the H_(2)O adsorption and the dissociation of HO-H ***,CRPO-2 exhibits remarkable HER performance,the mass activity is about 18.34,21.73,and 38.07 times higher than that of Pt/C in acidic,neutral,and alkaline media,respectively,at the same time maintain excellent *** findings may pave a new avenue for the rational design of electrocatalysts toward pH-universal water electrolysis.

关键词： cobalt metaphosphate pH-universal hydrogen evolution reaction(HER) vacancy engineering low-coordination atoms oxygen vacancy

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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

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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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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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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-1and 123.1 m Ah g-1can be achieved at 0.1 A g-1and 5 A g-1when 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 of147.67 Wh kg-1at approximately 199.93 W kg-1,and outstanding cycling life with negligible capacitance fading over 1000 *** 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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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 chemistry 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 110.13 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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Introducing hydroxyl groups to tailor the d-band center of Ir atom through side anchoring for boosted ORR and HER

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Journal of Energy chemistry 2024年第3期90卷 144-151,I0005页

作者： Qing Lv Meiping Li Xiaodong Li Xingru Yan Zhufeng Hou Changshui Huang Science Center for Material Creation and Energy Conversion School of Chemistry and Chemical EngineeringInstitute of Frontier and Interdisciplinary ScienceShandong UniversityJinan 250100ShandongChina institute of chemistry Chinese Academy of ScienceBeijing 100191China State Key Laboratory of Structural chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002FujianChina

Tuning the coordination atoms of central metal is an effective means to improve the electrocatalytic activity of atomic ***,iridium(Ir) is proposed to be asymmetrically anchored by sp-N and pyridinic N of hydrogen-substituted graphdiyne(HsGDY),and coordinated with OH as an Ir atomic catalyst(Ir_(1)-N-HsGDY).The electron structures,especially the d-band center of Ir atom,are optimized by these specific coordination ***,the as-synthesized Ir_(1)-N-HsGDY exhibits excellent electrocatalytic performances for oxygen reduction and hydrogen evolution reactions in both acidic and alkaline *** from the unique structure of HsGDY,IrN_(2)(OH)_(3) has been developed and demonstrated to act as the active site in these electrochemical *** those indicate the fresh role of the sp-N in graphdiyne in producing a new anchor way and contributing to promote the electrocatalytic activity,showing a new strategy to design novel electrochemical catalysts.

关键词： Oxygen reduction reaction D-band center Graphdiyne Hydroxyl group Electrocatalysis

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Thiol-mediated transportation pathway:an approach for improving tumor penetration of nanomedicines in vivo

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Science China chemistry 2024年第1期67卷 383-389页

作者： Junjie Zhang Weican Sun Xing Wang Senyan Chen Jingying Li Huanghao Yang New Cornerstone Science Laboratory Key Laboratory for Analytical Science of Food Safety and Biology(Ministry of Education)College of ChemistryFuzhou UniversityFuzhou 350116China Department of chemistry and College of Biological Science and Engineering Fuzhou UniversityFuzhou 350116China

Abnormal tumor microenvironment imposes barriers to tumor penetration of nanomedicine,which remains a major challenge for effective ***,we present disulfide-based nanoparticles that actively penetrate deep tumors in vivo through a thiol-mediated transportation *** achieve active tumor accumulation in vivo,disulfide-based nanoparticles are modified with folic acid units(FA-DBNPs).It is gratifying that FA-DBNPs still enter cells via the thiol-mediated pathway,which facilitates transcellular transportation and tumor penetration both in vitro and in ***,FA-DBNPs exhibit GSH concentration-dependent depolymerization characterization,indicating that the GSH level in tumor tissues regulates the penetration depth of *** from these advantages,FA-DBNPs showed potent anti-tumor activity in mouse models,leading to the significant regression of *** current study lays a foundation that thiol-mediated transportation is a promising approach in nanomedicine design for solid tumor therapy.

关键词： deep penetration thiol-mediated pathway transcellular transportation solid tumor

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One dimensional CeO_(2) nanorods/poly(ethylene oxide) solid composite electrolyte for all-solid-state lithium-ion batteries

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Journal of Rare Earths 2024年第3期42卷 570-577,I0005页

作者： Yudi Guo Erqing Zhao Xiaofang Zhao Shuailei Liu School of chemistry and Materials Engineering Xinxiang UniversityXinxiang453003China School of chemistry and Chemical Engineering Henan Institute of Science and TechnologyXinxiang453003China

The research of poly(ethylene oxide)(PEO)-based solid composite electrolyte with high ionic conductivity and excellent interfacial stability is the key to the development of all-solid-state lithium-ion batteries(ASSLIBs). Herein, uniform nanorod structured CeO_(2) fillers were controllably synthesized by electrospinning, which were subsequently filled into PEO polymer to prepare CeO_(2)/PEO solid composite electrolyte. The addition of CeO_(2) nanorods can reduce both the glass transition temperature and the melting point of PEO polymer, and also interact with PEO and lithium bis(trifluoromethanesulphonyl)imide(LITFSI) by Lewis acid—base reaction. Therefore, the solid composite electrolyte exhibits a high ionic conductivity of 4.52 × 10^(-4)S/cm, a wide electrochemical stability window of about 4.8 V, and a good interfacial stability with Li at 55℃. Moreover, the LiFePO_4/Li ASSLIB divulges the discharging specific capacity of 165, 162, 156 and 146 mA,h/g at 0.2, 0.5, 1 and 2 C, respectively, and achieves the capacity retention of 90.3% after 150 cycles at 0.5 C. Consequently, one dimensional CeO_(2) nanorods can be considered as an alternative filler for polymeric solid electrolyte.

关键词： Poly(ethylene oxide) Solid composite electrolyte CeO_(2)nanorods Ionic conductivity Rare earths

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