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Dimensional regulation in gigantic molybdenum blue wheels featuring{(W)Mo_(5)}motifs for enhanced proton conductivity

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Nano Research 2024年第9期17卷 8261-8268页

作者： Yu-Lun Wu Jing Du Hai-Ying Zhang Ming-Jun Hou Qiao-Yue Li Wei-Chao Chen Kui-Zhan Shao Bo Zhu Chao Qin Xin-Long Wang Zhong-Min Su Key Laboratory of Polyoxometalate and Reticular Material chemistry of Ministry of Education Department of ChemistryNortheast Normal UniversityChangchun 130024China hebei Key Laboratory of Organic Functional Molecules National Demonstration Center for Experimental Chemistry EducationTesting and Analysis CenterCollege of Chemistry and Materials ScienceHebei Normal UniversityShijiazhuang 050024China State Key Laboratory of Supramolecular Structure and Materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China

Dimensional regulation in polyoxometalates is an effective strategy during the design and synthesis of polyoxometalates-based high proton conductors,but it is not available to ***,the precise regulation of dimensionality has been realized in an unprecedented gigantic molybdenum blue wheel family featuring pentagonal{(W)Mo5}motifs through optimizing the molar ratio of Mo/W,including[Gd_(2)Mo_(124)W_(14)O_(422)(H_(2)O)62]38-(0D-{Mo_(124)W_(14)},1),[Mo_(126)W_(14)O441(H_(2)O)51]^(70-)(1D-{Mo_(126)W_(14)}n,2),and[Mo_(124)W_(14)O_(430)(H_(2)O)50]60-(2D-{Mo_(124)W_(14)}n,3).Such important{(W)Mo5}structural motif brings new reactivity into gigantic Mo blue *** are different numbers and sites of{Mo2}defects in each wheel-shaped monomer in 1-3,which leads to the monomers of 2 and 3 to form 1D and 2D architectures via Mo-O-Mo covalent bonds driven by{Mo2}-mediated H_(2)O ligands substitution process,respectively,thus achieving the controllable dimensional *** expected,the proton conductivity of 3 is 10 times higher than that of 1 and 1.7 times higher than that of *** continuous proton hopping sites in 2D network are responsible for the enhanced proton conductivity with lower activation *** study highlights that this dimensional regulation approach remains great potential in preparing polyoxometalates-based high proton conductive materials.

关键词： polyoxometalate molybdenum blue wheels Mo/W mixed-addenda polyoxometalates dimensional regulation proton conduction

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Reviewing electrochemical stability of ionic liquids-/deep eutectic solvents-based electrolytes in lithium-ion,lithium-metal and post-lithium-ion batteries for green and safe energy

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Green Energy & Environment 2024年第6期9卷 966-991页

作者： Yu Chen Shuzi Liu Zixin Bi Zheng Li Fengyi Zhou Ruifen shi Tiancheng Mu department of chemistry and Material Science Langfang Normal UniversityNO.100 Aimin West RoadLangfangHebei065000China department of chemistry Renmin University of ChinNO.59 Zhongguancun StreetHaidian DistrictBeijing100872China

Sustainable energy is the key issue for the environment protection,human activity and economic *** liquids(ILs)and deep eutectic solvents(DESs)are dogmatically regarded as green and sustainable electrolytes in lithium-ion,lithium-metal(e.g.,lithium-sulphur,lithium-oxygen)and post-lithium-ion(e.g.,sodium-ion,magnesium-ion,and aluminum-ion)*** electrochemical stability of ILs/DESs is one of the prerequisites for green,sustainable and safe energy;while easy electrochemical decomposition of ILs/DESs would be contradictory to the concept of green chemistry by adding the cost,releasing volatile/hazardous by-products and hindering the ***,(1)are ILs/DESs-based electrolytes really electrochemically stable when they are not used in batteries?(2)are ILs/DESs-based electrolytes really electrochemically stable in real batteries?(3)how to design ILs/DESs-based electrolytes with high electrochemical stability for batteries to achieve sustainability and green development?Up to now,there is no summary on this topic,to the best of our ***,we review the effect of chemical structure and non-structural factors on the electrochemical stability of ILs/DESs in simulated *** importantly,electrochemical stability of ILs/DESs in real lithium-ion,lithium-metal and post-lithium-ion batteries is concluded and ***,the strategies to improve the electrochemical stability of ILs/DESs in lithium-ion,lithium-metal and post-lithium-ion batteries are *** review would provide a guide to design ILs/DESs with high electrochemical stability for lithium-ion,lithium-metal and postlithium-ion batteries to achieve sustainable and green energy.

关键词： Green solvents Decomposition Sustainable chemistry Lithium-oxygen batteries Lithium-sulphur batteries Sodium-ion batteries

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Weak interaction-steered evolution of polyoxovanadate-based metal-organic polyhedra from transformation via interlock to packing

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Chinese Chemical Letters 2024年第2期35卷 527-533页

作者： Yan-Hu Wang Ke-Wei Tong Chao-Qin Chen Jing Du Peng Yang College of chemistry and Chemical Engineering Advanced Catalytic Engineering Research Center of the Ministry of EducationHunan UniversityChangsha 410082China College of chemistry and Materials Science Testing and Analysis CenterHebei Normal UniversityShijiazhuang 050024China

A bottleneck in biomimetic synthesis consists in the full copy of,for example,the hierarchical structure of proteins directed by weak *** contrast with covalent bonds bearing definite orientation and high stability,weak intermolecular forces within a continuous dynamic equilibrium can be hardly tamed for molecular *** this endeavor,a ligand-dominated strategy that embodies tunable electrostatic repulsion andπ···πstacking was first employed to shape polyoxovanadate-based metal-organic polyhedra(VMOPs).Structural evolution involving transformation,interlock,and discovery of an unprecedented prototype of the Star of David was hence *** only as a handy tool for the primary structural control over VMOPs,these weak forces allow for an advanced management on the spatial distribution of such manmade macromolecules as well as the associated physicochemical behaviors,representing an ideal model for simulating and interpreting the conformation-function relationship of proteins.

关键词： Polyoxometalates Polyoxovanadates Metal-organic polyhedron Interlock Weak intermolecular forces

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Small-sized Ni-Co/Mo_(2)C/Co_(6)Mo_(6)C_(2)@C for efficient alkaline and acidic hydrogen evolution reaction by an anchoring calcination strategy

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Frontiers of Chemical Science and Engineering 2024年第5期18卷 95-103页

作者： Jianxia Gu Ying Zhu Haiyan Zheng Chunyi Sun Zhongmin Su department of chemistry Xinzhou Normal UniversityXinzhou 034000China School of chemistry Northeast Normal UniversityChangchun 130024China

A novel,cheap and highly efficient Ni-Co/Mo_(2)C/Co_(6)Mo_(6)C_(2)@C nanocomposite has been successfully constructed through simple one-step carbonization method in a nitrogen *** in the precursor can effectively anchor molybdenum-based Keggin-type polyoxometallate and NiCo-layered double hydroxide through electrostatic and coordination interactions,which avoids the aggregation of catalyst particles during the pyrolysis *** optimization,the obtained Ni-Co/Mo_(2)C/Co_(6)Mo_(6)C_(2)@C possesses small size(3-8 nm),large specific surface area and hierarchical pore *** importantly,Ni-Co/Mo_(2)C/Co_(6)Mo_(6)C_(2)@C presents remarkable hydrogen evolution reaction activity with low overpotentials in 0.5 mol·L^(-1)H_(2)SO_(4)(102.3 mV)and 1 mol·L^(-1)KOH(95 mV)to afford the current density of 10 mA·cm^(-2),as well as small Tafel slopes of 82.49 and 99.92 mV·dec^(-1),***,this catalyst also shows outstanding stability for 12 h without a significant change in current *** excellent catalytic performance of Ni-Co/Mo_(2)C/Co_(6)Mo_(6)C_(2)@C can put down to the synergistic effect between multiple components and the small size of the *** work provides unique insights into the preparation of efficient transition metal-based catalysts for HER.

关键词： polyoxometallates layered double hydroxide transition metal-based electrocatalysts hydrogen evolution reaction

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Rare earth fluorescent nanoprobes with minimal side effects enable tumor microenvironment activation for chemotherapy

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Journal of Rare Earths 2024年第2期42卷 256-262,I0001页

作者： Tianqi Cao Yuxin Liu Qi Jia Xiaolu Wang Shouqiang Zhang Jing Zhou department of chemistry Capital Normal UniversityBeijing100048China

Chemotherapy,the use of antitumor drugs to kill cancer cells,is currently one of the most effective treatments for ***,serious toxic side effects caused by long-term drug accumulation can cause significant damage to the body,which limits the clinical application of antitumor *** this study,a novel RENPs@DOX-Fe nanoprobe(NP) was constructed by coating the surface of rare earth nanomaterials(NaLuF_(4):Yb,Er) with a complex formed by doxorubicin(DOX) and iron ion(Ⅲ).Due to the low toxicity of anthracycline-metal complexes,the damage to normal cells is *** unique acidic microenvironment in tumor cells facilitates the decomposition and gradual release of DOX from the DOX-Fe *** addition,the DOX-Fe complex can convert near-infrared(NIR) light into heat energy,which promotes the decomposition of the complex,further enhancing the release of DOX in the tumor *** change of ratio fluorescence of rare earth nanomaterials at 660 and 1550 nm after DOX release enables visual monitoring of drug release,which can potentially improve the chemotherapeutic *** vitro experiments established that RENPs@DOX-Fe NPs with NIR illumination had good therapeutic efficacy in *** work provides new insights into designing tumor microenvironment-responsive nanoprobes for chemotherapy with minimal side effects.

关键词： Rare earth nanoprobes Fluorescence Ratiometric imaging DOX Chemotherapy

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Multicolor circularly polarized phosphorescence of axially chiral binuclear platinum(Ⅱ) complexes

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Science China chemistry 2024年第11期67卷 3757-3766页

作者： Jintong Song Rui Zeng Hui Xiao Hailiang Ni Zong-Xiang Xu Haifeng Xiang College of chemistry and Materials Science Sichuan Normal University department of chemistry Southern University of Science and Technology College of chemistry Sichuan University

D-A charge transfer, including through-bond charge transfer and through-space charge transfer between two different electron donors（D） and electron acceptors（A）, is a fundamental and powerful tool to tune the optical properties of organic dyes. Herein,we demonstrate a unique strategy to tune phosphorescence and circularly polarized luminescence properties of axially chiral binuclear Pt（Ⅱ） complexes through long-range charge transfer, even though these molecules have two totally identical segments on either side of the chiral core. The presence of axial chirality would break not only the symmetry of molecular structure and π-conjugation system but also the symmetry of charge distribution for long-range charge transfer. These binaphthyl-based Pt（Ⅱ）complexes bearing coordinated atoms far away from chiral axis exhibit no Pt-Pt interactions but colorful concentrationdependent phosphorescence with quantum yield up to 86.4% and could be applied as emitters in highly efficient solutionprocessed organic light-emitting diodes to achieve luminance, luminance efficiency, power efficiency, external quantum efficiency, and asymmetry factor up to 8.94 × 10～3cd m-2, 41.9 cd A-1, 18.8 lm W-1, 12.6% and 2.98 × 10-3, respectively. Therefore,the present work affords a new and simple way to utilize the inherently asymmetric advantage of chirality for the design of D-Abased organic dyes.

关键词： Pt(II) complexes organic light-emitting diodes circularly polarized phosphorescence axial chirality

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Constructing S-scheme charge separation in cobalt phthalocyanine/oxygen-doped g-C_(3)N_(4) heterojunction with enhanced photothermal-assisted photocatalytic H_(2) evolution

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Rare Metals 2024年第1期43卷 198-211页

作者： Wei-Long shi Zheng Xu Yu-Xing shi Ling-Ling Li Jia-Lin Lu Xin-Hai Sun Xin Du Feng Guo Chang-Yu Lu School of Material Science and Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China School of Energy and Power Jiangsu University of Science and TechnologyZhenjiang 212003JiangsuChina College of chemistry Zhengzhou UniversityZhengzhou 450001China School of Water Resource and Environment Hebei Province Key Laboratory of Sustained Utilization and Development of Water RecourseHebei Center for Ecological and Environmental Geology ResearchHebei Geo UniversityShijiazhuang 050031China

Hydrogen acquisition from solar energy is an effective way to address energy crisis,which makes the development of efficient photocatalysts become the main direction of scientific ***,cobalt phthalocyanine/oxygen-doped g-C_(3)N_(4)(CoPc/OCN) S-scheme heterojunction photocatalyst was designed by coupling multi-step calcination with solvothermal method for enhanced photothermal-assisted photocatalytic H_(2) *** multistep calcined g-C_(3)N_(4) is easier for O-doping formation,and the ethanol solvothermal strategy is utilized to enhance the dispersion of CoPc on OCN nano sheet surface and forms sufficient S-scheme heterojunction through *** addition,the active sites and excellent photothermal properties of CoPc itself further improve the integrated photocatalytic activity of CoPc/OCN S-scheme *** optimal photocatalytic hydrogen evolution rate of CoPc/OCN S-scheme heterojunction photocatalyst reached 9.56 mmol·g^(-1)·h^(-1),which is 2.69 and 1.23 times higher than that of CN and OCN,*** work provides a valuable design idea and scheme for enhancing the multi-factor co-assisted photocatalytic H_(2) evolution performance.

关键词： Photothermal Photocatalytic H_(2)evolution Cobalt phthalocyanine Oxygen-doped g-C_(3)N_(4) Sscheme heterojunction

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Low-Strain and High-Energy KVPO4F Cathode with Multifunctional Stabilizer for Advanced Potassium-Ion Batteries

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Energy & Environmental Materials 2024年第5期7卷 144-153页

作者： Yongli Heng Zhenyi Gu Jinzhi Guo Haojie Liang Yan Liu Wei Guo Xinxin Zhao Xiaotong Wang Xinglong Wu MOE Key Laboratory for UV Light-Emitting Materials and Technology Northeast Normal University Key Laboratory of Organo-Pharmaceutical chemistry of Jiangxi Province Gannan Normal University department of chemistry Northeast Normal University

KVPO4F with excellent structural stability and high operating voltage has been identified as a promising cathode for potassium-ion batteries （PIBs）,but limits in sluggish ion transport and severe volume change cause insufficient potassium storage ***,a high-energy and low-strain KVPO4F composite cathode assisted by multifunctional K2C4O4electrode stabilizer is exquisitely *** electrochemical investigations demonstrate that this composite cathode can deliver a remarkable energy density up to 530 Wh kg-1with 142.7 mAh g-1of reversible capacity at25 mA g-1,outstanding rate capability of 70.6 mAh g-1at 1000 mA g-1,and decent cycling ***,slight volume change （-5%） and increased interfacial stability with thin and even cathode-electrolyte interphase can be observed through in situ and ex situ characterizations,which are attributed to the synergistic effect from in situ potassium compensation and carbon deposition through self-sacrificing K2C4O4additive.

关键词： high energy density K2C4O4 KVPO4F composite cathode low strain potassium-ion batteries

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Photochromic radical states in 3D covalent organic frameworks with zyg topology for enhanced photocatalysis

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National Science Review 2024年第7期11卷 177-188页

作者： Tian-Tian Ma Guo-Zhang Huang Xiao-Han Wang Yan Liang Run-Han Li Bin Wang Su-Juan Yao Jia-Peng Liao Shun-Li Li Yong Yan Ya-Qian Lan School of chemistry South China Normal University department of chemistry Guangdong Provincial Key Laboratory of Catalytic Chemistry Southern University of Science and Technology

Covalent-organic frameworks（COFs） with photoinduced donor-acceptor（D-A） radical pairs show enhanced photocatalytic activity in principle. However, achieving long-lived charge separation in COFs proves challenging due to the rapid charge recombination. Here, we develop a novel strategy by combining[6 + 4] nodes to construct zyg-type 3D COFs, first reported in COF chemistry. This structure type exhibits a fused Olympic-rings-like shape, which provides a platform for stabilizing the photoinduced D-A radical pairs. The zyg-type COFs containing catalytically active moieties such as triphenylamine and phenothiazine（PTZ） show superior photocatalytic production rates of hydrogen peroxide（H2O2）. Significantly, the photochromic radical states of these COFs show up to 400% enhancement in photocatalytic activity compared to the parent states, achieving a remarkable H2O2synthesis rate of 3324 μmol g-1h-1, which makes the PTZ-COF one of the best crystalline porous photocatalysts in H2O2production. This work will shed light on the synthesis of efficient 3D COF photocatalysts built on topologies that can facilitate photogenerating D-A radical pairs for enhanced photocatalysis.

关键词： 3D covalent-organic frameworks photochromic radical states donor and acceptor hydrogen peroxide photocatalysis

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Facile synthesis of a tumor microenvironment-responsive nanomaterial with metallic polyphenol-encapsulated for enhanced synergistic therapy

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Journal of Rare Earths 2024年第10期42卷 1895-1902页

作者： Kaige Yu Nuo Kou Shouqiang Zhang Tianqi Cao Hanqing Wu Jing Zhou department of chemistry Capital Normal UniversityBejing100048China College of Teacher Education Capital Normal University Beijing100048China

The tumor microenvironment(TME)differs from normal tissue cells in its physiological and biochemical *** construction of TME-responsive nanoplatforms requires a tedious preparation process and complex multicomponent *** this work,Er@EGCG-Cu,a TME-responsive nanoplatform,was simply and rapidly synthesized by combining rare earth-doped nanomaterials(NaLuF_(4):Yb,Er)with EGCG-Cu which is based on the ability of metal ions to coordinate with polyphenols to form a metal-phenolic network(MPN)*** MPN structure is then destroyed under an acidic TME,releasing the chemotherapy(CT)drug EGCG,which can cause apoptosis,Cu_(x)S_(y)is generated by combining Cu^(2+)with H_2S overexpressed in human colorectal cancer cells and can be used for photothermal therapy(PTT).Cell experiments show that laser irradiation improves the CT/PTT synergistic effect of Er@*** study has significance for the construction of TME-responsive nanomedicines with simple and rapid preparation for synergistic therapy.

关键词： Tumor microenvironment Metal-polyphenol networks Synergistic therapy Rare earths Nanomaterials

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