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Structural Properties of Ions and Polyelectrolytes in Aqueous Solutions under External Electric Fields:The Sign Effect

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Chinese Journal of Polymer Science 2024年第9期42卷 1341-1352,I0007页

作者： Cheng-Jiang Lin Jun-Jun Wang Yuan Jiang Shu-Li Chen Hong-Fei Li Wen-Han Zhao Qing-Rong Huang Chang-Ru Rong Xiao-Zheng Duan State Key laboratory of Polymer Physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China School of applied chemistry and Engineering University of Science and Technology of ChinaHefei230026China National Key laboratory of Advanced Vehicle Integration and Control China FAW Group Co.Ltd.Changchun130013China State Key laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai200438China Department of Food Science Rutgers University65 Dudley RoadNew BrunswickNew Jersey08901USA

We utilize molecular dynamics simulations to investigate the microstructures of ions and polyelectrolytes in aqueous solutions under external electric *** focusing on the multi-body interactions between ionic components and H_(2)O molecules,as well as their responses to the external electric fields,we clarify several nontrivial molecular features of the ionic and polyelectrolyte solutions,such as the solvations of cations and anions,clustering of the ions,and dispersions/aggregations of polyelectrolyte chains,as well as the corresponding responses of H_(2)O molecules in these *** simulations illustrate the variations in structures of ionic solutions caused by reversing the charge sign of the ions,and elucidate the disparity in structures between anionic and cationic polyelectrolyte solutions in the presence of the external electric *** work clarifies the mechanism for the alternations in complex multi-body interactions in aqueous solutions caused by the application electric field,which can contribute to the fundamental understanding of the physical and chemical natures of ion-containing and charged polymeric systems.

关键词： Polyelectrolyte Ions Aqueous solutions External electric fields Asymmetric dipole

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A bifunctional nitrile additive for high-performance lithiumoxygen batteries

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Nano Research 2024年第7期17卷 6119-6126页

作者： Ziwei Li Yue Yu Dongyue Yang Jin Wang Junmin Yan Gang Huang Tong Liu Xinbo Zhang Key laboratory of Automobile Materials Ministry of EducationDepartment of Materials Science and EngineeringJilin UniversityChangchun 130022China State Key laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Department of chemistry and Waterloo Institute for Nanotechnology University of Waterloo200 University Ave.W.WaterlooOntario N2L 3G1Canada School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

Li-O_(2)batteries with high energy density hold significant promise as next-generation energy storage ***,Li-O_(2)batteries have poor cycling performance at high current densities and large capacities,primarily due to the high impedance caused by the instability of the lithium anode and the sluggish kinetics in the discharge products decomposition on the ***,we investigated a bifunctional nitrile additive(2-methoxy benzonitrile(2-MBN))with good chemical/electrochemical stability to improve the performances of Li-O_(2)*** 2-MBN could actively modify the anode by ensuring uniform Li+deposition and optimizing the composition of solid electrolyte interphase(SEI).Meanwhile,it could also facilitate the decomposition of discharge products by inducing the formation of sheet-like Li_(2)O_(2),significantly reducing the battery charge *** bifunctional effects of 2-MBN for the anode and cathode enable Li-O_(2)batteries to achieve a stable lifetime of 97 cycles at a current density of 600 mA·g^(−1)with a fixed capacity of 2000 mAh·g^(−1),much better than that of Li-O_(2)batteries without 2-MBN(28 cycles).The inclusion of 2-MBN provides an effective approach for attaining high-performance Li-O_(2)batteries.

关键词： nitrile additives Li-O_(2)batteries lithium metal anode charge overpotential

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DPY19L3 promotes vasculogenicmimicry by its C-mannosyltransferase activity

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Oncology Research 2024年第4期32卷 607-614页

作者： HASSAN BAYDOUN YUJI KATO HIROKI KAMO ANNA HÜSCH HAYATO MIZUTA RYOTA KAWAHARA SIRO SIMIZU Department of applied chemistry Faculty of Science and TechnologyKeio UniversityYokohama223-8522Japan Department of Pharmacy and biochemistry Faculty of ScienceUniversity of TübingenTübingen72074Germany

C-mannosylation is a post-translational modification that occurs intracellularly in the endoplasmic *** humans,biosynthesis of C-mannosylation in proteins containing thrombospondin type 1 repeat is catalyzed by the DPY19 family;nonetheless,biological functions of protein C-mannosylation are not yet fully understood,especially in tumor *** mimicry(VM)is the formation of fluid-conducting channels by highly invasive and genetically deregulated tumor cells,enabling the tumors to form matrix-embedded vasculogenic structures,containing plasma and blood cells to meet the metabolic demands of rapidly growing *** this study,we focused on DPY19L3,a C-mannosyltransferase,and aimed to unravel its role in *** of DPY19L3 inhibited the formation of VM in HT1080 human fibrosarcoma ***-expression of wild-type DPY19L3 recovered VM formation;however,DPY19L3 isoform2,an enzymatic activity-defect mutant,did not restore it,suggesting that the C-mannosyltransferase activity of DPY19L3 is crucial to its ***,the knockdown of DPY19L3 in MDA-MB-231 breast cancer cells hindered its network formation ***,our findings suggest that DPY19L3 is required for VM formation and stipulate the relevance of C-mannosylation in oncogenesis.

关键词： C-mannosylation Vasculogenic mimicry DPY19L3

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Yolk-shell FeSe_(2)@CoSe_(2)/FeSe_(2) heterojunction as anode materials for sodium-ion batteries with high rate capability and stability

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Journal of Materials Science & Technology 2024年第5期172卷 185-195页

作者： Liuyang Zhang Bicheng Zhu Difa Xu Zibao Qian Ping Xie Tao Liu Jiaguo Yu laboratory of Solar Fuel Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430078China Hunan Key laboratory of applied Environmental Photocatalysis Changsha UniversityChangsha 410022China State Key laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Sodium-ion batteries are promising candidates for large-scale grid storage systems and other *** foremost advantage derives from superior environmental credentials,enhanced safety as well as lower raw material costs than lithium-ion *** is still challenging to explore desirable anode *** this study,FeSe_(2)@CoSe_(2)/FeSe_(2),with a yolk-shell structure was prepared by ion exchange and *** FeSe_(2)@CoSe_(2)/FeSe_(2)prepared as anode material for sodiumion batteries exhibits excellent rate capability due to the synergistic effect of bimetallic selenides and the interfacial effect of the ***,it delivers high performance(510 mAh g^(-1)at 0.2 A g^(-1)),superior rate capa-bility(90%retention at 5 A g^(-1)),and good long-time cycling stability(78%capacity retention after 1800 cycles at a high current density of 2 A g^(-1)).The optimized sodiumion full cell with FeSe_(2)@CoSe_(2)/FeSe_(2)as the anode and Na 3 V 2(PO 4)3 as the cathode still demonstrates excellent ***,a ca-pacity of 272 mAh g^(-1)(at 1 A g^(-1))within the operating voltage from 1 to 3.8 V can be *** work illustrates the potential of bimetallic selenides with heterostructures for performance enhancement of sodium-ion batteries.

关键词： Cobalt-iron selenide Heterojunctions Sodium storage Anode material Full battery

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Engineering oxygen vacancies on Tb-doped ceria supported Pt catalyst for hydrogen production through steam reforming of long-chain hydrocarbon fuels

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Chinese Journal of Chemical Engineering 2024年第4期68卷 181-192页

作者： Zhourong Xiao Changxuan Zhang Peng Li Desong Wang Xiangwen Zhang Li Wang Jijun Zou Guozhu Li State Key laboratory of Metastable Materials Science and Technology(MMST) Hebei Key Laboratory of Applied ChemistryCollege of Environmental and Chemical EngineeringYanshan UniversityQinhuangdao 066004China Key laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell *** this work,Pt catalysts supported on CeO_(2)and Tb-doped CeO_(2)were prepared by a precipitation *** physical structure and chemical properties of the as-prepared catalysts were characterized by powder X-ray diffraction,scanning electron microscopy,transmission electron microscopy,Raman spectroscopy,H_(2)temperature programmed reduction,and X-ray photoelectron *** results show that Tb-doped CeO_(2)supported Pt possesses abundant surface oxygen vacancies,good inhibition of ceria sintering,and strong metal-support interaction compared with CeO_(2)supported *** catalytic performance of hydrogen production via steam reforming of long-chain hydrocarbon fuels(n-dodecane)was *** with 2Pt/CeO_(2),2Pt/Ce_(0.9)Tb_(0.1)O_(2),and 2Pt/Ce_(0.5)Tb_(0.5)O_(2),the 2Pt/Ce_(0.7)Tb_(0.3)O_(2)has higher activity and stability for hydrogen production,on which the conversion of n-dodecane was maintained at about 53.2%after 600 min reaction under 700℃at liquid space velocity of 9 ml·g^(-1)·h^(-1).2Pt/CeO_(2)rapidly deactivated,the conversion of n-dodecane was reduced to only 41.6%after 600 min.

关键词： Steam reforming n-Dodecane Hydrogen production Pt-based catalyst Oxygen vacancy CeO_(2)

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Polyoxometalate-based flexible conductive materials with superionic conductivity

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Science China chemistry 2024年

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 Chemistry Northeast Normal University State Key laboratory of Polymer Physics and chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

Flexible ion-conductive materials exhibit intriguing advantages for applications in flexible electronic devices. Currently, 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 challenge. Herein, 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 °C(3.33×10-2S cm-1) to room temperature(2.78×10-1S cm-1) under ambient humidity. Moreover, 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 devices. Both 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% hydrogel. This work provides new insights into the design of POM-based flexible materials with superionic conductivity.

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MicroED as a powerful technique for the structure determination of complex porous materials

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Chinese Journal of Structural chemistry 2024年第3期43卷 41-54页

作者： Chao Ma Cong Lin Jian Li State Key laboratory of Coordination chemistry School of Chemistry and Chemical EngineeringNanjing UniversityNanjing210023China Department of applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityKowloonHong Kong China

Porous materials have garnered significant attention in recent *** the intrinsic relationship between their structures and properties requires precise knowledge of their atomic ***-crystal X-ray diffraction(SCXRD)has traditionally been the primary method for elucidating such structures,but it demands large,high-quality crystals,often exceeding 5μm in *** growth of these crystals can be a time-consuming process,especially for one-and two-dimensional *** explore structures at the nanoscale,MicroED(microcrystal electron diffraction(ED))offers unprecedented insights into the realm of *** revolutionary technique enables researchers to uncover intricate details within nanoscale structures,promising to reshape our fundamental understanding of *** this review,we delve into the applications of MicroED in the study of various porous materials,including zeolites,metal-organic frameworks(MOFs),and covalent organic frameworks(COFs).We emphasize the pivotal role of MicroED in nanomaterial characterization,enabling precise crystallographic analysis and phase identification.

关键词： Atomic structure MicroED Porous materials Three-dimensional electron diffraction

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Exploring battery material failure mechanisms through synchrotron X-ray characterization techniques

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Journal of Energy chemistry 2024年第7期94卷 128-135页

作者： Lingzhe Fang Xiaozhao Liu Tao Li Department of chemistry and biochemistry Northern Illinois UniversityDeKalbIL 60115USA X-ray Science Division and Joint Center forEnergy Storage Research Argonne National LaboratoryLemontIL6439UA

Rechargeable battery cycling performance and related safety have been persistent *** is crucial to decipher the capacity fading induced by electrode material failure via a range of *** these,synchrotron-based X-ray techniques with high flux and brightness play a key role in understanding degradation *** this comprehensive review,we summarize recent advancements in degra-dation modes and mechanisms that were revealed by synchrotron X-ray ***,an overview of X-ray absorption spectroscopy and X-ray scattering techniques is introduced for charac-terizing failure phenomena at local coordination atomic environment and long-range order crystal struc-ture scale,*** last,we envision the future of exploring material failure mechanism.

关键词： Battery failure Synchrotron-based techniques X-ray scattering X-ray absorption spectroscopy

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Imidazole-Linked Fully Conjugated Covalent Organic Framework for High-Performance Sodium-Ion Battery

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CCS chemistry 2024年第5期6卷 1255-1263页

作者： Lu Liu Yu Gong Yifan Tong Hao Tian Xubo Wang Yiming Hu Shaofeng Huang Weiwei Huang Sandeep Sharma Jingnan Cui Yinghua Jin Weitao Gong Wei Zhang State Key laboratory of Fine Chemicals School of Chemical EngineeringDalian University of TechnologyDalian 116024 Department of chemistry University of Colorado BoulderBoulderColorado 80309 Hebei Key laboratory of applied chemistry Yanshan UniversityQinhuangdao 066004

Covalent organic frameworks(COFs)have garnered increasing attention as promising electrode materials for sodium-ion batteries(SIBs)due to their ordered backbones,uniform pore sizes,and high surface ***,they also face challenges,including low capacity,unsatisfactory rate performance,and limited cycling stability,which pose the primary obstacles to their practical ***,a pyrenoimidazole-based COF,denoted as PyIm-COF,has been synthesized as a novel electrode material for highperformance SIBs using an efficient synthetic *** extended fully conjugated backbones and readily accessible redox-active sites,PyIm-COF demonstrates remarkable high-rate performance,delivering around 250 m Ah g^(−1)and excellent cycling stability,retaining 97.2%of its capacity even after 2500 cycles at 5 A g^(−1),which is higher than that of most previously reported COF-based *** work provides valuable insights into the development of nitrogen-rich conjugated COF electrode materials for rechargeable SIBs.

关键词： pyrenoimidazole fully conjugated backbones covalent organic framework electrode material sodium-ion battery

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Supported Cu/Ni Bimetallic Cluster Electrocatalysts Boost CO_(2) Reduction

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Precision chemistry 2024年第3期2卷 96-102页

作者： Depeng Wang Jiazhi Wang Zhi Wang Ning Zhang Jianrong Zeng Haixia Zhong Xinbo Zhang State Key laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

Supported metal clusters with the integrated advantages of single-atom catalysts and conventional nanoparticles held great promise in the electrocatalytic carbon dioxide reduction(ECO_(2)R)operated at low overpotential and high current ***,its precise synthesis and the understanding of synergisti-cally catalytic effects remain ***,we report a facile method to synthesize the bimetallic Cu and Ni clusters anchored on porous carbon(Cu/Ni-NC)and achieve an enhanced ECO_(2)*** aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and synchrotron X-ray absorption spectroscopy were employed to verify the metal dispersion and the coordination of Cu/Ni clusters on *** a result of this route,the target Cu/Ni-NC exhibits excellent electrocatalytic performance including a stable 30 h electrolysis at 200 mA cm^(-2) with carbon monoxide Faradaic efficiency of∼95.1%using a membrane electrode assembly electrolysis *** with the in situ analysis of the surface-enhanced Fourier transform infrared spectroelectrochemistry,we propose that the synergistic effects between Ni and Cu can effectively promote the H_(2)O dissociation,thereby accelerate the hydrogenation of CO_(2)to*COOH and the overall reaction process.

关键词： electrocatalytic CO_(2)reduction bimetallic cluster synergistic catalysis membrane electrode assembly electrolysis cell in situ surface-enhanced infrared absorption spectroscopy

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