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Energy & Environmental materials 2024年第3期7卷 223-231页

作者： Sihang Cheng Cuimei Liu Yingqi Li Huaqiao Tan Yonghui Wang Yangguang Li key laboratory of polyoxometalate and reticular material chemistry of ministry of education Faculty of ChemistryNortheast Normal University

Solar vapor generation （SVC） represents a promising technique for seawater desalination to alleviate the global water crisis and energy *** of its main bottleneck problems is that the evaporation efficiency and stability are limited by salt crystallization under high-salinity ***,we demonstrate that the 3D porous melamine-foam （MF） wrapped by a type of self-assembling composite materials based on reduced polyoxometalates （*** blue,HPB）,oleic acid （OA）,and polypyrrole （PPy）(labeled with MF@HPB-PPy_n-OA) can serve as efficient and stable SVC material at high *** characterizations of MF@HPB-PPy_n-OA indicate that both hydrophilic region of HPBs and hydrophobic region of OA co-exist on the surface of composite materials,optimizing the hydrophilic and hydrophobic interfaces of the SVC materials,and fully exerting its functionality for ultrahigh water-evaporation and anti-salt *** optimal MF@HPBPPy10-OA operates continuously and stably for over 100 h in 10wt%***,MF@HPB-PPy10-OA accomplishes complete salt-water separation of 10wt%brine with 3.3kgm-2h-1under 1-sun irradiation,yielding salt harvesting efficiency of 96.5%,which belongs to the record high of high-salinity systems reported so far and is close to achieving zero liquid ***,the low cost of MF@HPB-PPy10-OA (2.56$m-2)suggests its potential application in the practical SVC technique.

关键词： heteropoly blue (HPB) hydrophilic-hydrophobic interface polyoxometalates (POM) salt-water separation solar vapor generation (SVG)

Rare earth inorganic-organic hybrid compounds based on Keggin-type polyoxometalate {SiW_(12)} with fast-responsive photochromism and switchable luminescence properties

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Journal of Rare Earths 2024年第2期42卷 286-292,I0003页

作者： Hong Cui Yanli Yang Xue Bai Xu Han Wensha Zhang Ying Lu Shuxia Liu key laboratory of polyoxometalate and reticular material chemistry of the ministry of education College of ChemistryNortheast Normal UniversityChangchun 130024China

Four rare earth inorganic-organic hybrid compounds based on Keggin-type polyoxometalate {SiW_(12)}with general formula [{RE(DMF)_(4)(H_(2)O)_4RE(DMF)_(6)}_(2){SiW_(12)O_(40)}_(3)](RE = La(1),Pr(2),Sm(3),Eu(4),DMF=N,N-dimethylformamide) were synthesized by the conventional solution *** analyses indicate that four compounds are isostructural and are all built from three [SiW_(12)O_(40)]^(4-) polyoxoanions and DMF ligands linked by RE^(3+).Compounds 1-4 are extremely sensitive to UV light and present excellent photochromic properties,in which the coloring and fading time of samples are both no more than 2 min,and the reversible coloring-fading process can be repeated for at least 10 cycles with little fatigue,suggesting that compounds 1-4 can be a series of fast-responsive and durable photochromic ***,the solid-state photoluminescence spectra of compounds 3(Sm) and 4(Eu)display strong characteristic emissions of rare earth ions based on f-f ***,compound4(Eu) has a longer fluorescence lifetime up to 566.74 μ***,co mpounds 3(Sm) and 4(Eu) exhibit the switchable luminescence behavior induced by photochromism,which allows them to be used as potential molecular switches.

关键词： Inorganic-organic hybrid Keggin-type polyoxometalates Rare earths Photochromism Photoluminescence

polyoxometalate-based flexible conductive materials with superionic conductivity

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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 University State key laboratory of Polymer Physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of Sciences

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,H3PW12O40（HPW） and NH2SO3H（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℃(3.33×10-2S cm-1) to room temperature(2.78×10-1S 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

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

Nanocomposite: Keggin-type Co_(4)-polyoxometalate@cobaltporphyrin linked graphdiyne for hydrogen evolution in seawater

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Nano Research 2024年第3期17卷 1281-1287页

作者： Jiejie Ping Danyang He Fei Wang Nan Wang Yi-cheng Fu Zihao Xing Zhiyu Jia Guo-Yu Yang key laboratory of Cluster Science Ministry of EducationSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China key laboratory of polyoxometalate and reticular material chemistry of ministry of education Facluty of Chmeistry Northeast Normal UniversityChangchun 130024China Peking University Third Hospital Beijing 100190China

polyoxometalate-based nanocomposites with electrocatalytic activity have been applied in hydrogen evolution reactions(HER).Seawater as the main water resource on the earth should be developed as the water electrolysis to prepare high-purity *** this paper,we used two synthesis strategies to prepare the nanocomposite Co_(4)-POM@Co-PGDY(Co_(4)-POM:the Kegging-type microcrystals of K_(10)[Co_(4)(PW_(9)O_(3)4)2]and Co-PGDY:cobalt-porphyrin linked graphdiyne)with excellent activity for ***-PGDY as the porous material is applied not only as the protection of microcrystals towards the metal ion in seawater but also as the co-electrocatalyst of Co_(4)-***_(4)-POM@Co-PGDY exhibits excellent HER performance in seawater electrolytes with low overpotential and high stability at high ***,we have observed a key H_(3)O+intermediate emergence on the surface of nanocomposite during hydrogen evolution process in seawater by Raman synchrotron radiation-based Fourier transform infrared(SR-FTIR).The results in this paper provide an effective strategy for preparing polyoxometalate-based electrocatalysts with high-performance toward hydrogen evolution reaction.

关键词： polyoxometalate graphdiyne seawater hydrogen evolution reaction

Synthesis and oxidative desulfurization activity of vanadium-substituted Keggin-type polyoxometalate hybrid compounds

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Tungsten 2024年第3期6卷 529-535页

作者： Min Xing Xiao-Ying Ji Shu-Xia Liu key laboratory of polyoxometalate and reticular material chemistry of ministry of education Department of chemistry Northeast Normal University

SOxfrom fuel oil has caused much air pollution. Therefore, the desulfurization of fuel oil is necessary. Oxidative desulfurization（ODS）, as one of the most efficient nonhydrodesulfurization technologies, has become a major solution of desulfurization for fuel oil owing to its high reactivity for the removal of refractory organic sulfur compounds including dibenzothiophene（DBT） and its derivatives under mild reaction conditions [1]. Among them,

关键词： FRAMEWORK CHAIN

polyoxometalate as the assembly material to self-assembled Ni(OH)_(2) nanosheets with electrocatalytic performance

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Nano Research 2024年第8期17卷 7061-7067页

作者： Danyang He Tianyang Li Luozhen Jiang Fei Wang Zihao Xing Nan Wang Zhiyu Jia Guo-Yu Yang key laboratory of Cluster Science Ministry of EducationSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China Shanghai Advanced Research Institute Chinese Academy of ScienceShanghai 201210China key laboratory of polyoxometalate and reticular material chemistry of ministry of education Facluty of ChemistryNortheast Normal UniversityChangchun 130024China

Developing non-noble metal-based electrocatalyst with high catalytic activity is essential for advancing hydrogen energy *** study introduces a hydrothermal method for synthesizing order Ni(OH)_(2) nanosheets,with H_(3)O_(40)PW_(12)(denoted as PW_(12))loaded onto reduced graphene oxide(rGO)coated on nickel foam(referred to as PW_(12)-Ni(OH)_(2)/rGO).This method contrasts with the electrodeposition of Ni(OH)_(2),where PW_(12) is added to the synthetic system to direct the assembly and morphology of the Ni(OH)_(2) through a hydrothermal *** this work,the nickel foam acts dual roles as both the substrate and the source of nickel for the formation of Ni(OH)_(2).The PW_(12)-Ni(OH)_(2)/rGO nanosheets,when successfully prepared and loaded onto the nickel foam(NF),exhibited superior electrocatalytic activity for the hydrogen evolution reaction(HER)in an alkaline electrolyte,achieving a current density of 10 mA·cm^(-2) at an overpotential of 69 ***,we endeavored to expand the application of this material towards the oxygen evolution reaction(OER)by preparing PW_(12)-(Fe/Co)Ni(OH)_(2)/rGO through the addition of metal *** nanocomposite displayed outstanding electrocatalytic activity in alkaline electrolytes,with a current density of 10 mA·cm^(-2)at an overpotential of 211 mV,and demonstrated excellent stability over a 50 h period in a 1 M KOH *** results presented in this paper offer an effective strategy for the preparation of polyoxometalate-based inorganic materials with diverse functionalities,applicable to both HER and OER.

关键词： polyoxometalate Ni(OH)_(2) assembly hydrogen evolution reaction oxygen evolution reaction

Two polyoxovanadoborates with over 100 nuclei assembled from a {V_(14)Co_(12)B_(72)} cluster

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Science China chemistry 2024年第8期67卷 2578-2585页

作者： Shuang-Xue Wu Yu-Jiao Dong Yang Yang Chao Qin Chun-Yi Sun Wei Guan Xin-Long Wang Zhong-Min Su key laboratory of polyoxometalate and reticular material chemistry of ministry of education Northeast Normal UniversityChangchun 130024China School of chemistry and Environmental Engineering Changchun University of Science and TechnologyChangchun 130013China key laboratory of Advanced materials of Tropical Island Resources Hainan UniversityHaikou 570228China

Combining theoretical prediction and experimental exploration, the first sandwich-type polyoxovanadoborate(POVB) with an odd number of nuclei, [V_(11)B_(26)O_(73)(OH)_(10)]^(8-)(1), was discovered under hydrothermal conditions. Density-functional theory(DFT)gives a rationalization for the existence of this structure and the structural feature is consistent with the {V_NB_(2N+X)}(X = 2, 4, 6, 8)general formula. Excitingly, when Co and 1,10-phenanthroline(phen) are introduced into the synthesis of vanadoborates system,a 100-nuclei [Co_6(phen)_(10)(H_(2)O)_8][V_(14)Co_(12)B_(72)O_(144)(OH)_(20)]·28H_(2)O(2) and a 102-nuclei [Co_6(phen)_(14)(H_(2)O)_(4)][V_(14)Co_(12)B_(72)O_(144)(OH)_(20)]·23H_(2)O(3) with the same core structure of [V_(14)Co_(12)B_(72)]^(12-)are obtained. The vase-shaped [V_(14)Co_(12)B_(72)] polyanion is a multilayered sandwich-type structure containing seven distinct structural layers and is the largest known POVB. Furthermore, 2demonstrates exceptional thermal and chemical stability and serves as an efficient and stable catalyst for the photoreduction of carbon dioxide.

关键词： boronate metallic materials polyoxovanadoborates density functional theory photocatalysis CO_(2)reduction

Covalent organic frameworks/carbon nanotubes composite with cobalt(II)pyrimidine sites for bifunctional oxygen electrocatalysis

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Nano materials Science 2024年第4期6卷 419-427页

作者： Zhuangzhuang Wu Lijuan Feng Zhe Lu Xinxin Yu Yuzhen Zhao Junming Luo Shaolei Wang Xinlong Tian Qi Chen State key laboratory of Marine Resource Utilization in South China Sea School of Marine Science and Engineering Hainan University key laboratory of polyoxometalate and reticular material chemistry of ministry of education School of Chemistry Northeast Normal University School of Bioengineering Zhuhai Campus of Zunyi Medical University

With characteristics and advantages of functional composite materials, they are commendably adopted in numerous fields especially in oxygen electrocatalysis, which is due to the significant synergies between various components. Herein, a novel bifunctional oxygen electrocatalyst（Co-CNT@COF-Pyr） has been synthesized through in-situ growth of covalent organic frameworks（COFs） layers on the outer surface of highly conductive carbon nanotubes（CNTs） followed by coordination with Co（II）. For electrocatalytic OER, Co-CNT@COF-Pyr reveals a low overpotential（438 mV） in alkaline electrolyte（1.0 M aqueous solution of KOH） with a current density of 10 mA cm-2, which is comparable to most discovered COF-based catalysts. For electrocatalytic ORR, CoCNT@COF-Pyr exhibits a low H2O2yield range（9.0 %–10.1 %） and a reaction pathway close to 4e-（n =3.82–3.80） in alkaline electrolyte（0.1 M aqueous solution of KOH） within the test potential range of 0.1–0.6 V ***, which is superior to most reported COF-based catalysts. Hence, this research could not only offer an innovative insight into the construction of composites, but also facilitate the practical application of renewable fuel cells, closed water cycle, and rechargeable metal-air batteries.

关键词： Oxygen electrocatalysis Covalent organic frameworks Carbon nanotubes Composite materials

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通过二维沸石调节铂的氢化选择性

Science China materials 2024年第7期67卷 2135-2141页

作者：翟玉慧马悦崔凤超田宇阳朱广山 key laboratory of polyoxometalate and reticular material chemistry of ministry of education Faculty of ChemistryNortheast Normal UniversityChangchun 130024China

不饱和醇是一类重要的医药中间体,然而C=C加氢比C=O加氢反应更具有热力学优势,因此由不饱和醛合成不饱和醇具有挑战性.为解决这一问题,需要寻求一种具有可调控选择性的氢化催化剂.二维沸石的高长径比和大量的末端基团作为锚定位点,使其... 详细信息

不饱和醇是一类重要的医药中间体,然而C=C加氢比C=O加氢反应更具有热力学优势,因此由不饱和醛合成不饱和醇具有挑战性.为解决这一问题,需要寻求一种具有可调控选择性的氢化催化剂.二维沸石的高长径比和大量的末端基团作为锚定位点,使其不仅能作为催化剂载体,还可以有效地调节催化剂性能.本研究利用二维沸石IPC-1P作为铂纳米颗粒的载体,成功制备出异相催化剂Pt@IPC-1P.铂纳米颗粒的尺寸小于2 nm且均匀地分布在IPC-1P上.令人惊喜的是,Pt@IPC-1P催化剂对不饱和醇的选择性超过了90%,并实现了接近100%的催化转化率,远超其他铂基催化剂.理论计算证实,二维沸石IPC-1P在肉桂醛向肉桂醇的转化过程中起到了积极作用,其放热效应能量高于苯丙醛.这项工作展现了二维沸石在催化有机物转化领域具有广阔的应用前景.

关键词： heterogeneous catalysis 2D zeolite hydrogenation selectivity cinnamaldehyde top-down approach