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Tuning the local coordination environment of silver(Ⅰ) coordination networks with counterions for enhanced electrocatalytic CO_(2) reduction

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Science China Chemistry 2024年第5期67卷 1524-1530页

作者： Xiaofeng Cui Xueting Wang Cong fu Bing Liu Mei-Yan Gao Tingting kong Yujie Xiong Anhui Engineering Research Center of Carbon Neutrality The Key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Laboratory of Molecular-Based MaterialsCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China Department of Chemical Sciences Bernal InstituteUniversity of LimerickLimerick V94 T9PXRepublic of Ireland School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China School of Chemical and Material Engineering Jiangnan UniversityWuxi 214122China

Very recently, the local coordination environment of active sites has been found to strongly influence their performance in electrocatalytic CO_(2) reduction by tuning the intrinsic kinetics of CO_(2) activation and intermediate stabilization. It is imperative to elucidate the mechanism for such an influence towards the rational design of efficient catalysts;however, the complex interactions between the multiple factors involved in the system make it challenging to establish a clear structure–performance relationship. In this work, we chose ion-intercalated silver(I)-based coordination networks(AgCNs) with a well-defined structure as a model platform, which enables us to understand the regulation mechanism of counterions as the counterions are the only tuning factor involved in such a system. We prepared two isostructural Ag CNs with different intercalation ions or counterions of BF_(4)^(-) and ClO_(4)^(-)(named as AgCNs-BF_(4) and AgCNs-ClO_(4)) and found that the former has a more competitive CO_(2) electroreduction performance than the latter. AgCNs-BF_(4) achieves the highest Faradaic efficiency for CO_(2) to CO of 87.1% at-1.0 V(vs. RHE) with a higher partial current density, while AgCNs-ClO_(4) exhibits only 77.2% at the same applied *** characterizations and theoretical calculation reveal that the presence of BF_(4)^(-)is more favorable for stabilizing the COOH^(*) intermediate by weakening hydrogen bonds, which accounts for the superior activity of Ag CNs-BF_(4).

关键词： electrocatalytic CO_(2) reduction coordination networks local environment counterions intercalation ions

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Transformation of long-period stacking ordered structures in Mg-Gd-Y-Zn alloys upon synergistic characterization of first-principles calculation and experiment and its effects on mechanical properties

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Journal of Magnesium and Alloys 2024年第5期12卷 1867-1879页

作者： Mingyu Li guangzong Zhang Siqi Yin Changfeng Wang Ying fu Chenyang gu Renguo guan School of Materials Science and Engineering Northeastern UniversityShenyang 110819China Key Laboratory of Near-Net Forming of Light Metals of Liaoning Province Dalian Jiaotong UniversityDalian 116028China Engineering Research Center of Continuous Extrusion Ministry of EducationDalian Jiaotong UniversityDalian 116028China Songshan Lake Materials Laboratory Dongguan 523808China

Based on experiments and first-principles calculations,the microstructures and mechanical properties of as-cast and solution treated Mg-10Gd-4Y-xZn-0.6Zr(x=0,1,2,wt.%)alloys are *** transformation process of long-period stacking ordered(LPSO)structure during solidification and heat treatment and its effect on the mechanical properties of experimental alloys are *** reveal that the stacking faults and 18R LPSO phases appear in the as-cast Mg-10Gd-4Y-1Zn-0.6Zr and Mg-10Gd-4Y-2Zn-0.6Zr alloys,*** solution treatment,the stacking faults and 18R LPSO phase transform into 14H LPSO *** Enthalpies of formation and reaction energy of 14H and 18R LPSO are calculated based on *** show that the alloying ability of 18R is stronger than that of *** reaction energies show that the 14H LPSO phase is more stable than the 18R *** elastic properties of the 14H and 18R LPSO phases are also evaluated by first-principles calculations,and the results are in good agreement with the experimental *** precipitation of LPSO phase improves the tensile strength,yield strength and elongation of the *** solution treatment,the Mg-10Gd-4Y-2Zn-0.6Zr alloy has the best mechanical properties,and its ultimate tensile strength and yield strength are 278.7 MPa and 196.4 MPa,*** elongation of Mg-10Gd-4Y-2Zn-0.6Zr reaches 15.1,which is higher than that of Mg-10Gd-4Y0.6Zr *** improving mechanism of elastic modulus by the LPSO phases and the influence on the alloy mechanical properties are also analyzed.

关键词： Mg-Gd-Y-Zn alloys Long-period stacking ordered First-principles calculations Enthalpies Mechanical properties

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Fate of organophosphate esters from the Northwestern Pacific to the Southern Ocean:Occurrence,distribution,and fugacity model simulation

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Journal of Environmental Sciences 2024年第3期137卷 347-357页

作者： Tengda Shi Ruijing Li Jie fu Chao Hou Hui Gao guanjie Cheng Haibo Zhang Shuaichen Jin Liang kong guangshui Na College of Marine Technology and Environment Dalian Ocean UniversityDalian 116023China Laboratory for coastal marine eco-environment process and carbon sink of Hainan province/Yazhou Bay Innovation Institute Hainan Tropical Ocean UniversitySanya 572022China National Marine Environmental Monitoring Center Dalian 116023China College of Marine Ecology and Environment Shanghai Ocean UniversityShanghai 201306China NCS Testing Technology Co. Ltd.Beijing 10081China

Eleven organophosphate esters(OPEs)in the air and seawater were investigated from the northwestern Pacific Ocean to the Southern Ocean during the 2018 Chinese 34th Antarctic Scientific *** concentration of total OPEs ranged from 164.82 to 3501.79 pg/m~3in air and from 4.54 to 70.09 ng/L in *** halogenated OPEs,tri(chloropropyl)phosphate(TCPP)and tri(2-chloroethyl)phosphate(TCEP),were generally more abundant than the non-halogenated OPEs.A levelⅢfugacity model was developed to simulate the transfer and fate of seven OPEs in the air and seawater regions of the central Ross *** model results indicate that OPEs are transferred from the air to the seawater in the central Ross Sea in summer,during which the Ross Sea acts as a final OPE *** and wet deposition dominated the processes involving OPE transfer to *** OPE degradation process was also found to be more pervasive in the atmosphere than in the seawater *** findings highlights the importance of long-range transport of OPEs and their air–seawater interface behavior in the Antarctic.

关键词： Organophosphate esters(OPEs) Long-range transport fugacity model Antarctic Fate

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Lithium polysulfide solvation and speciation in the aprotic lithium-sulfur batteries

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Particuology 2024年第6期89卷 238-245页

作者： Jinhao Zhang Qingshan fu Peng Li Ruibo Linghu Xiaozhong Fan Haibin Lin Juncao Bian Songbai Han Gengzhi Sun Long kong Frontiers Science Center for Flexible Electronics and Xi’an Institute of Flexible Electronics Northwestern Polytechnical UniversityXi’an710129China China Automotive Innovation Corporation Nanjing211100China Academy for Advanced Interdisciplinary Studies Southern University of Science and TechnologyShenzhen518055China Institute of Advanced Materials Nanjing Tech UniversityNanjing211816China

Fingerprinting sulfur speciation in aprotic electrolytes is a key to understand fundamental chemistry and design well-performing lithium–sulfur(Li–S)*** polysulfide(LiPS)dissolution and deposition in ether-based electrolytes during redox reactions have been probed and established by spectroscopy and ***,detailed LiPS structure and solvation properties influenced by conventional and newly developed electrolytes remain elusive,which exert fundamental challenges and practical difficulties in decoupling battery performance from electrolyte *** perspective aims to provide timely information to uncover underlying mechanisms that rein in sulfur speciation by considering the charge density of LiPSs and the coordination strength of solvents/*** discussion starts with unlocking the baseline electrolyte formulation to investigate its role in LiPS formation and *** that,the term coordination strength is used instead of donor number and dielectric constant to describe interactions between solvents and LiPSs and to reveal LiPS structure *** work is expected to encourage the discovery of new electrolyte working mechanisms to develop energy-dense and power-intensive Li–S batteries.

关键词： Sulfur speciation Redox kinetics Coordination strength Solvation chemistry Lithium-sulfur batteries

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Probing phase transition of band topology via radiation topology

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Photonics Research 2024年第6期12卷 1150-1157页

作者： CHANG-YIN JI WENZE LAN PENG fu GANG WANG CHANGZHI gu YELIANG WANG JIAFANG LI YUguI YAO BAOLI LIU Key Laboratory of Advanced Optoelectronic Quantum Architecture and Measurement(MOE) Beijing Key Laboratory of Nanophotonics&Ultrafine Optoelectronic Systemsand School of PhysicsBeijing Institute of TechnologyBeijing 100081China School of Integrated Circuits and Electronics MIIT Key Laboratory for Low-Dimensional Quantum Structure and DevicesBeijing Institute of TechnologyBeijing 100081China Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China School of Physical Sciences CAS Key Laboratory of Vacuum PhysicsUniversity of Chinese Academy of SciencesBeijing 100190China CAS Center for Excellence in Topological Quantum Computation CAS Key Laboratory of Vacuum PhysicsUniversity of Chinese Academy of SciencesBeijing 100190China

Topological photonics has received extensive attention from researchers because it provides brand new physical principles to manipulate *** topology is characterized using the Berry phase defined by Bloch *** now,the scheme for experimentally probing the topological phase transition of band topology has always been relatively lacking in topological ***,radiation topology can be aroused by the far-field polarization singularities of Bloch states,which is described by the Stokes *** such two types of topologies are both related to Bloch states on the band structures,it is rather surprising that their development is almost ***,in optical analogs of the quantum spin Hall effects(QSHEs)and Su-Schrieffer-Heeger model,we reveal the correlation between the phase transition of band topology and radiation topology and then demonstrate that the radiation topology can be employed to study the band topological *** experimentally demonstrate such an intriguing phenomenon in optical analogs of *** findings not only provide an insightful understanding of band topology and radiation topology,but also can serve as a route to manipulate light.

关键词： transition. topology topological

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The Traf2 and NcK interacting kinase inhibitor NCB-0846 suppresses seizure activity involving the decrease of GRIA1

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Genes & Diseases 2024年第3期11卷 452-467页

作者： Min Wang Yixue gu Qiubo Li Bangzhe Feng Xinke Lv Hao Zhang Qingxia kong Zhifang Dong Xin Tian Yanke Zhang Department of Neurology Affiliated Hospital of Jining Medical UniversityJiningShandong 272000China Department of Neurology The First Affiliated Hospital of Chongqing Medical UniversityChongqing Key Laboratory of NeurologyChongqing 400016China Department of Pediatrics Affiliated Hospital of Jining Medical UniversityJiningShandong 272000China Department of Neurosurgery Affliated Hospital of Jining Medical UniversityJiningShandong 272000China Pediatric Research Institute Ministry of Education Key Laboratory of Child Development and DisordersNational Clinical Research Center for Child Health and DisordersChongqing Key Laboratory of Translational Medical Research in Cognitive Development and Learning and Memory DisordersChildren's Hospital of Chongqing Medical UniversityChongqing 400014China Center for Excellence in Brain Science and Intelligence Technology Chinese Academy of SciencesShanghai 200031China

Epilepsy,one of the most common neurological disorders,is characterized by spon-taneous recurrent *** lobe epilepsy(TLE)is one of the most common medically intractable seizure ***2-and NcK-interacting kinase(TNIK)has recently attracted attention as a critical modulation target of many neurological and psychiatric disorders,but its role in epilepsy remains *** this study,we hypothesized the involvement of TNIK in epilepsy and investigated TNIK expression in patients with intractable TLE and in a pilocarpineinduced rat model of epilepsy by western blotting,immunofluorescence,and immunohistochemistry.A pentylenetetrazole(PTZ)-induced epilepsy rat model was used to determine the effect of the TNIK inhibitor NCB-0846 on behavioral manifestations of ***(Co-IP)/mass spectrometry(MS)was used to identify the potential *** Co-IP,we detected and confirmed the main potential TNIK *** fractionation was used to establish the effect of NCB-0846 on the expression of the main interactors in postsynaptic density(PSD)*** found that TNIK was primarily located in neurons and decreased significantly in epilepsy model rats and TLE patients compared with ***-0846 delayed kindling progression and decreased seizure ***-IP/MS identified 63 candidate TNIK interactors in rat hippocampi,notably ***-IP showed that TNIK might correlate with endogenous GRIA1,SYN2,PSD-95,CaMKIV,GABRG1,and *** addition,the significant decrease in GRIA1 in hippocampal total lysate and PSDs after NCB-0846 treatment might help modify the progression of PTZ *** results suggest that TNIK contributes to epileptic pathology and is a potential antiepileptic drug target.

关键词： Epilepsy NCB-0846 Rat TLE TNIK Traf2-and NcK-interacting kinase

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The dynamic characteristics of saturated remolded loess under cyclic load

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Earthquake Research Advances 2024年第2期4卷 27-35页

作者： Yuting fu Yanbo Cao Jiaxu kong Jia Zheng Jiaqi Mu Jie Wang Jianqi Zhuang College of Geological Engineering and Geomatics Key Laboratory of Western China Mineral Resources and Geological EngineeringChang’an UniversityXi’an710054China

Due to the joint development characteristic and macropore structure of loess,it is easy to cause structure collapse under earthquake or artificial *** study on the loess disaster effect and its mechanism under earthquake action is insufficient due to its ***,to study the deformation and mechanical properties more accurately,the dynamic characteristics of saturated remolded loess under cyclic dynamic load were tested using a GDS dynamic triaxial instrument in this *** test results show that strain and pore water pressure increase gradually at different rates with the development of vibration,and there is an obvious inflection point in the time-history curve of *** the number of vibrations(N)exceeds this point,the strain increases rapidly,and pore water pressure tends to be *** the action of large amplitude and low-frequency dynamic load,the strain and pore water pressure increase rapidly with fewer vibrations and the deviator stress(q)decreases rapidly,while the sample achieves damage faster with the increase of *** the application of a dynamic load,the effective stress(p)gradually decreases and its rate of change slows ***,when the saturated remolded loess is subjected to a constant-amplitude dynamic load,the combination of large amplitude and low frequency leads to the failure of the sample in the shortest time.

关键词： Loess Pore water pressure Strain Frequency Amplitude Quake(vibration)

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Ribosome-inspired electrocatalysts inducing preferential nucleation and growth of three-dimensional lithium sulfide for high-performance lithium-sulfur batteries

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Journal of Energy Chemistry 2024年第7期94卷 517-526页

作者： Zhen Wu Wenfeng He Jiahui Yang Yunuo gu Ruiqi Yang Yiran Sun Jiajia Yuan Xin Wang Junwu Zhu Yongsheng fu Key Laboratory for Soft Chemistry and functional Materials of Ministry of Education Nanjing University of Science and TechnologyNanjing 210094JiangsuChina School of Energy and Power Engineering Jiangsu UniversityZhenjiang 212013JiangsuChina FEB Res Inst Far East BatteryWuxi 214200JiangsuChina

Nucleation of lithium sulfide(Li_(2)S)induced by electrocatalysts plays a crucial role in mitigating the shut-tle ***,short-chain polysulfides on electrocatalysts surfaces tend to re-dissolve into elec-trolytes,delaying Li_(2)S supersaturation and its *** this study,we draw inspiration from the ribosome-driven protein synthesis process in cells to prepare ultrasmall nitrogen-doped MoS_(2) nanocrys-tals anchored on porous nitrogen-doped carbon networks(N-MoS_(2)-NC)***,the ex-situ SEM demonstrates that ribosome-inspired N-MoS_(2)-NC electrocatalysts induce early nucleation and rapid growth of three-dimensional Li_(2)s during *** calculations reveal that the Li-s bond length in N-MoS_(2)-Li_(2)S(100)is shorter,and the corresponding interfacial formation energy is lower than in MoS_(2)-Li_(2)S(100).This accelerated conversion of lithium polysulfides to Li_(2)S can enhance the utilization of active substances and inhibit the shuttle *** study highlights the potential of ribosome-inspired N-MoS_(2)-NC in improving the electrochemical stability of Li-S batteries,providing valuable insights for future electrocatalyst design.

关键词： Lithium-sulfur batteries Electrocatalysts Nanocrystals Ribosome-inspired Nucleation and growth

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Revealing the Structure-Property Difference of Natural Rubber Prepared by Different Methods: Protein and Gel Content are Key Factors

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Chinese Journal of Polymer Science 2024年第4期42卷 457-467页

作者： Shao-Qi Huang Jun-Qi Zhang Yong Zhu Ling-Min kong Lu-Sheng Liao fu-Quan Zhang Zheng-Tian Xie Jin-Rong Wu State Key Laboratory of Polymer Materials Engineering College of Polymer Science and EngineeringSichuan UniversityChengdu610065China Hainan Provincial Key Laboratory of Natural Rubber Processing Agricultural Products Processing Research Institute of Chinese Academy of Tropical Agricultural SciencesZhanjiang524001China

Natural rubber (NR) is widely used in various fields including aerospace, military industry and transportation due to its superior elasticity and comprehensive mechanical properties. Nonetheless, the commercial NR prepared by different methods usually exhibits different mechanical properties, primarily due to variations in processing conditions during the conversion from latex to bulk rubber material. Consequently, this poses challenges in scientific research and industrial production of NR. In order to assess the properties of various commercially available NR and identify key structural and compositional components, this study systematically compares and analyzes four representative NR raw materials: air dried sheet (ADS), ribbed smoked sheets (RSS), constant viscidity NR (CV), and whole field latex rubber (WF). The investigation focuses on evaluating their static mechanical behavior, SIC behavior, wear resistance, and fatigue resistance. The findings indicate that protein and gel content exhibit a crucial influence on the NR properties. These constituents contribute to the formation of a high-crosslinking density region, generating a heterogeneous network structure within the rubber. This structure amplifies strains during deformation, leading to earlier and stronger strain-induced crystallization (SIC). Among the four commercial NR brands, RSS demonstrates superior overall mechanical and dynamic properties owing to its high protein and gel content. This study serves as a valuable reference for comprehending the differences in properties among various commercial NR, thereby offering guidance for the actual processing and selection of NR.

关键词： Natural rubber Processingmethod Protein Gel content Property

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Ceria nanoparticles: biomedical applications and toxicity

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Journal of Zhejiang University-Science B(Biomedicine & Biotechnology) 2024年第5期25卷 361-388页

作者： Xiaoxuan fu Peng LI Xi CHEN Yuanyuan MA Rong WANG Wenxuan JI Jiakuo gu Bowen SHENG Yizhou WANG Zhuhong ZHANG School of Pharmacy Key Laboratory of Molecular Pharmacology and Drug Evaluation(Yantai University)Ministry of EducationCollaborative Innovation Center of Advanced Drug Delivery System and Biotech Drugs in Universities of ShandongYantai UniversityYantai 264005China Department of Nephrology Yantai Yuhuangding HospitalQingdao UniversityYantai 264005China Institute of Crop Science College of Agriculture and BiotechnologyZhejiang UniversityHangzhou 310058China

Ceria nanoparticles(CeO_(2) NPs)have become popular materials in biomedical and industrial fields due to their potential applications in anti-oxidation,cancer therapy,photocatalytic degradation of pollutants,sensors,*** methods,including gas phase,solid phase,liquid phase,and the newly proposed green synthesis method,have been reported for the synthesis of CeO_(2) *** to the wide application of CeO_(2) NPs,concerns about their adverse impacts on human health have been *** review covers recent studies on the biomedical applications of CeO_(2) NPs,including their use in the treatment of various diseases(e.g.,Alzheimer's disease,ischemic stroke,retinal damage,chronic inflammation,and cancer).CeO_(2) NP toxicity is discussed in terms of the different systems of the human body(e.g.,cytotoxicity,genotoxicity,respiratory toxicity,neurotoxicity,and hepatotoxicity).This comprehensive review covers both fundamental discoveries and exploratory progress in CeO_(2) NP research that may lead to practical developments in the future.

关键词： Ceria nanoparticle Synthetic method Biomedical application Oxidative stress Toxicity

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