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A Stable Copper-based Metal-Azolate Framework for Efficient Electroreduction of CO_(2)to C_(2+)Products

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Chemical Research in Chinese Universities 2024年第4期40卷 664-669页

作者： LIU Yuan-Yuan zhu Hao-Lin LIAO Pei-Qin CHEN xiao-ming Key Laboratory of Bioinorganic and Synthetic Chemistry Ministry of EducationGBRCE for Functional Molecular EngineeringSchool of ChemistryIGCMESun Yat-sen UniversityGuangzhou510275P.R.China Chemistry and Chemical Engineering Guangdong Laboratory Shantou515031P.R.China

Driven by renewable or excess electrical energy,electrochemical CO_(2)reduction reaction(eCO_(2)RR)represents a promising carbon-neutral approach to generating valuable low-carbon fuels by consuming CO_(2)and H_(2)O.C_(2+)products are one of the most economically valuable products among the reduction species of eCO_(2)RR,but there are still some challenges,such as low selectivity or low current *** this work,we showed that a copper-based metal-azolate framework(MAF),denoted as MAF-203,exhibits the high performance of eCO_(2)RR to yield C_(2+)products with the Faradaic efficiency(C_(2+))of 52.5%and a current density of 660 mA/cm^(2)at-1.2 V *** in a flow cell device under alkaline *** experiment,in situ infrared spectroscopy and the density functional theory(DFT)calculations showed that the electron donating effect of methyl substituents on organic ligands of the copper-based MAF could enhance the ligand field and activation of key intermediates(*CO and*CHO species),thus promoting the coupling of*CO and*CHO for yielding C_(2+)products.

关键词： Metal-organic framework Carbon dioxide Electroreduction C_(2+)product Metal-azolate framework

Isocyanide-Based One-Pot Cascade Synthesis of 3-Acyl Isoindolinones

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Chinese Journal of Chemistry 2024年第3期42卷 259-263页

作者： Jia Liu Yi-ming zhu xiao-Ping Xu Shun-Jun Ji Key Laboratory of Organic Synthesis of Jiangsu Province College of ChemistryChemical Engineering and Materials Science & Collaborative Innovation Center of Suzhou Nano Science and TechnologySoochow UniversitySuzhouJiangsu215123 China Suzhou Baolidi Functional Materials Research Institute SuzhouJiangsu215144 China

A series of 3-acyl-substituted isoindolinone derivatives were synthesized in a one-pot manner via the reaction of o-bromobenzaldehydes,isocyanides,and carboxylic acids in the presence of palladium catalyst and base. The reaction employing easily available starting materials features simple operation and high efficiency. The mechanistic study showed that the reaction might undergo 1) Pd-catalyzed [3+2] cyclization of o-bromobenzaldehyde with isocyanide and the re-insertion of another molecule of isocyanide,2) addition of carboxylic acid to in situ formed ketenimine followed by a rearrangement relay to give 3,3-diacyl-substituted isoindolinone derivative. Further transformations of the obtained products through decarbonylation could also be realized.

关键词： One-pot reaction Isocyanide Pd catalysis Rearrangement reaction Isoindolinone

Unconventional Fluorescent and Multi-responsive Polyethyleneimine with LCST and UCST Behavior:Synthesis,Characterization and Biological Applications

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Chinese Journal of Polymer Science 2024年第6期42卷 826-837页

作者： Feng-ming Yin Li-Li Wu Shu-Sheng Li xiao-Na Pan xiao-Li zhu Xu-Bao Jiang Xiang Zheng Kong College of Chemistry and Chemical Engineering University of JinanJinan250022China Shandong Institute for Product Quality Inspection Jinan250102China College of Chemical Engineering Tianjin UniversityTianjin300072China

Non-aromatic fluorescent and multi-responsive materials,exhibiting inherent fluorescence emission and controlled phase change,have garnered significant attention in recent ***,the underlying interaction between their fluorescent properties and phase transition remains *** this study,we synthesized a series of catalyst-free aza-Michael addition-based polyethyleneimine(RFPEI)materials by reacting polyethyleneimine(PEI)with N-isopropyl acrylamide(NIPAM).The resulting RFPEI was comprehensively characterized,and demonstrated dual-phase transition behavior(LCST and UCST)in water,which could be finely tuned by adjusting its composition or external factors such as ***,upon UV irradiation(365 nm),RFPEI exhibited strong fluorescence *** further investigated the effects of NIPAM grafting percentage to PEI,polymer concentration,and pH on the LCST/UCST and fluorescent properties of RFPEI aqueous ***,we showcased the great potential of RFPEI as a versatile tool for physiological cell imaging,trace detection,and controlled release of *** study presents a novel class of stimuli-responsive fluorescent materials with promising applications in the field of biomedicine.

关键词： Polyethyleneimine Multi-responsiveness Intrinsic fluorescence emission Cell imaging Controlled drug release

A Self-Healing Elastomer with Extremely High Toughness Achieved by Acylsemicarbazide Hydrogen Bonding and Cu^(2+)-Neocuproine Coordination Interactions

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Chinese Journal of Polymer Science 2024年第10期42卷 1425-1434,I0007页

作者： xiao-ming An Yi-Ping Wang Tang-Song zhu Chong Xing Xu-Dong Jia Qiu-Hong Zhang Key Laboratory of High Performance Polymer Material and Technology of MOE Department of Polymer Science and EngineeringSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing210093China State Key Laboratory of Coordination Chemistry Nanjing UniversityNanjing210093China

Elastomers with high mechanical toughness can guarantee their durability during service ***-healing ability,as well as recyclability,can also extend the life of materials and save the consuming cost of the *** efforts have been dedicated to promoting the mechanical toughness as well as the self-healing capability of elastomers at the same time,while it remains a challenge to balance the trade-off between the above properties in one *** we proposed a molecular design driven by dual interactions of acylsemicarbazide hydrogen bonding and Cu^(2+)-neocuproine coordination *** introducing the reversible multiple hydrogen bonds and strong coordination bonds,we successfully fabricated an extremely tough and self-healing *** elastomer can achieve an impressive top-notch toughness of 491 MJ/m^(3).Furthermore,it boasted rapid elastic restorability within 10 min and outstanding crack tolerance with high fracture energy(152.6kJ/m^(2)).Benefiting from the combination of dynamic interactions,the material was able to self-repair under 80℃conveniently and could be reprocessed to restore the exceptional mechanical properties.

关键词： Metal-ligand coordination Hydrogen bond Ultra-tough elastomer Self-healing

Surface diffraction beamline at the SSRF

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Nuclear Science and Techniques 2024年第7期35卷 47-57页

作者： Yue-Liang Gu Xu Zheng Xing-Min Zhang Bin Zhao Guang-Zhi Yin Da-ming zhu Yuan-He Sun Xing-Yu Gao xiao-Long Li Shanghai Advanced Research Institute Chinese Academy of Sciences239 Zhangheng RoadPudong DistrictShanghai201204China

BL02U2 of the Shanghai Synchrotron Radiation Facility is a surface diffraction beamline with a photon flux of 5.5×10^(12) photons/s at 10 keV and a beam size of 160µm×80µm at the sample *** is dedicated to studying surfaces(solid-vacuum,solid-gas)and interfaces(solid-solid,solid-liquid,and liquid-liquid)in nanoscience,condensed matter,and soft matter systems using various surface scattering techniques over an energy range of 4.8-28 keV with transmission and reflection ***,BL02U2 has a high energy resolution,high angular resolution,and low beam divergence,which can provide excellent properties for X-ray diffraction experiments,such as grazing incident X-ray diffraction,X-ray reflectivity,crystal truncation rods,and liquid X-ray *** of in situ environments can also be provided for the samples *** paper describes the setup of the new beamline and its applications in various fields.

关键词： Surface and interface Beamline Surface diffraction Microstructure

Molecular Chain Flexibility and Dielectric Loss at High-Frequency:Impact of Ester Bond Arrangement in Poly(ester imide)s

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Chinese Journal of Polymer Science 2024年第8期42卷 1122-1133页

作者： Ya-Dong Li Hong Li Lu-Kun Feng Feng Bao ming-Liang Wang Cai-Zhen zhu Zhao-Hui Zheng xiao-Bin Ding Jian Xu Chengdu Institute of Organic Chemistry Chinese Academy of SciencesChengdu 610041China University of Chinese Academy of Sciences Beijing 100081China Institute of Low-Dimensional Materials Genome Initiative College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060China

The evolution of high-frequency communication has accentuated the significance of controlling dielectric properties in polymer ***,it has been theorized that rigid molecular chains lead to lower dielectric ***,the validity of this proposition at high frequencies remains *** scrutinize the correlation between chain flexibility and dielectric properties,we synthesized six poly(ester imide)s(PEIs)with systematically varied molecular chain flexibilities by modifying the ester's substitution on the aromatic *** introduction of ester bonds bestowed all PEI films with a low dielectric dissipation factor(D_(f)),ranging from 0.0021 to 0.0038 at 10 GHz in dry *** dry D_(f)displayed a pattern consistent with volume polarizability(P/V).Unexpectedly,PI-mmm-T,featu ring the most flexible molecular chain,exhibited the lowest dielectric loss under both dry(0.0021@10 GHz)and hygroscopic(0.0029@10 GHz)***,the observed increase in D_(f)after humidity absorption suggests that the high dielectric loss of PEI in applications may be attributed to its hygroscopic *** simulations and characterization of the aggregation structure revealed that the smaller cavities within flexible molecular chains,after close stacking,impede the entry of water *** sacrificing high-temperature resistance,the precursor exhibited enhanced solubility properties and could be processed into high-quality *** research unveils new insights into the relationship between flexibility and highfrequency dielectric loss,offering innovative perspectives on synthesizing aromatic polymers with exceptional dielectric properties.

关键词： 5G communications Poly(ester imide)s Molecular chain flexibility Dielectric properties Humidity absorption

Spatial-and spin-resolution ARPES and magnetism beamline at SSRF

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Nuclear Science and Techniques 2024年第8期35卷 23-37页

作者： Fang‑Yuan zhu Jie‑Feng Cao Xiang‑Yu Meng Jun‑Qin Li Rui Yu Ya‑Mei Wang Shan Qiao Bo Zhao ming‑zhu Zhang Zhong‑Kai Liu Mei‑xiao Wang Yong Wang Ren‑Zhong Tai Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China ShanghaiTech Laboratory for Topological Physics School of Physical Science and TechnologyShanghai Tech UniversityShanghai 201210China University of Chinese Academy of Sciences Beijing 100049China

The BL07U beamline is a new extreme ultraviolet and soft X-ray beamline housed in the Shanghai Synchrotron Radiation Facility. Beamlines are used in nano-resolved angle-resolved photoemission spectroscopy(nano-ARPES), spin-resolved angle-resolved photoemission spectroscopy(spin-ARPES), X-ray magnetic circular dichroism spectroscopy, and X-ray magnetic linear dichroism spectroscopy for certain scientific research. The BL07U beamline, which is based on a pair of elliptical polarized undulators and a variable-included-angle plane-grating monochromator, delivers circularly or linear polarized X-rays within the energy range of 50–2000 eV. The beamline features two branches: One dedicated to nano-ARPES,which has a minimum spot size of only ~ 200 nm, and another branch comprising spin-ARPES, a vector magnetic field, and superconductive magnetic end-station.

关键词： Soft X-ray beamline Nano-ARPES Spin-ARPES XMCD/XMLD

Estimating the optimal vegetation coverage for the dominant tree and shrub species over China's northwest drylands

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Science China Earth Sciences 2024年第5期67卷 1500-1517页

作者： Zhongdian ZHANG xiaoxu JIA Ping zhu mingbin HUANG Lidong REN ming’an SHAO School of Geographic Sciences Xinyang Normal UniversityXinyang 464000China Key Laboratory of Ecosystem Network Observation and Modeling Institute of Geographic Sciences and Natural Resources ResearchChinese Academy of SciencesBeijing 100101China College of Resources and Environment University of Chinese Academy of SciencesBeijing 100190China Yellow River Delta Modern Agricultural Engineering Laboratory Chinese Academy of SciencesBeijing 100101China State Key Laboratory of Soil Erosion and Dryland Farming on the Loess Plateau Institute of Soil and Water ConservationNorthwest A&F UniversityYangling 712100China

Anthropogenic revegetation is an effective way to control soil erosion and restore degraded ecosystems in China's northwest drylands(NWD).However,excessive vegetation cover expansion has long been known to increase evapotranspiration,leading to reduced local water availability,which can in turn threaten the health and services of restored *** the optimal vegetation coverage(OVC)is critical for balancing the trade-off between plant growth and water consumption in water-stressed areas,yet quantitative assessments over the entire NWD are still *** this study,a modified Biome BioGeochemical Cycles(Biome-BGC)model was used to simulate the long-term(1961–2020)dynamics of actual evapotranspiration(ET_(a)),net primary productivity(NPP),and leaf area index(LAI)for the dominant non-native tree(*** and ***)and shrub(*** and ***)species at 246 meteorological sites over *** modified model incorporated the Richards equation to simulate transient unsaturated water flow in a multilayer soil module,and both soil and eco-physiological parameters required by the model were validated using field-observed ETadata for each *** distributions of OVC(given by the mean maximum LAI,LAI_(max))for the dominant species were determined within three hydrogeomorphic sub-areas(i.e.,the loess hilly-gully sub-area,the windy and sandy sub-area,and the desert sub-area).The modified Biome-BGC model performed well in terms of simulating ET_(a) dynamics for the four plant *** distributions of mean ET_a,NPP,and LAI_(max)generally exhibited patterns similar to mean annual precipitation(MAP).In the loess hilly-gully sub-area(MAP:210 to 710 mm),the OVC respectively ranged from 1.7 to 2.9 and 0.8 to 2.9 for *** and *** the windy and sandy sub-area(MAP:135 to 500 mm),the OVC ranged from 0.3 to 3.3,0.5 to 2.6 and 0.6 to 2.1for ***,*** and ***,*** the desert sub-

关键词： Optimal vegetation coverage Water balance Leaf area index Biome-BGC model Dryland

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超表面透镜偏振可切换的多通道功能复用

红外与毫米波学报 2024年第3期43卷 369-374页

作者：刘小东朱亦鸣上海尼博电子科技有限公司上海201615 上海理工大学光电信息与计算机工程学院上海200093

超表面概念的提出为研究平面化和超薄的光学元器件提供了一种全新的设计思路。传统的几何相位型的超表面透镜受制于偏振锁定的限制,阻碍了其实现多功能的复用。文章提出了一种通过几何相位实现超表面透镜偏振解耦的方法。进一步,利用该... 详细信息

超表面概念的提出为研究平面化和超薄的光学元器件提供了一种全新的设计思路。传统的几何相位型的超表面透镜受制于偏振锁定的限制,阻碍了其实现多功能的复用。文章提出了一种通过几何相位实现超表面透镜偏振解耦的方法。进一步,利用该方法作者实现了超表面聚焦透镜在纵向以及纵向和横向实现多通道功能(如聚焦光斑和聚焦涡旋)的复用和偏振可切换特性。相关研究为实现多功能可集成的平面化器件提供了新的研究思路。

关键词：超表面超透镜聚焦涡旋