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Surface engineering of 1D nanocatalysts for value-added selective electrooxidation of organic chemicals

Nano Research 2024年第3期17卷 1327-1336页

作者： Yongping Yang Chuhao liu Tinglu Song Mufan Li Zipeng Zhao beijing key {2. of Construction Tailorable Advanced Functional Materials and Green Applications Experimental Center of Advanced MaterialsSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China beijing national {2. for molecular sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Electrolytic water splitting by renewable energy is a technology with great potential for producing hydrogen(H_(2.)without carbon emission,but this technical route is hindered by its huge energy(electricity)cost,which is mainly wasted by the anode oxygen evolution reaction(OER)while the value of the anode product(oxygen)is very *** the high-energy-cost OER with a selective organic compound electrooxidation carried out at a relatively lower potential can reduce the electricity cost while producing value-added ***,H_(2. generation coupled with synthesis of value-added organic compounds faces the challenge of low selectivity and slow generation rate of the anodic ***-dimensional(1D)nanocatalysts with a unique morphology,well-defined active sites,and good electron conductivity have shown excellent performance in many electrocatalytic *** rational design and regulation of 1D nanocatalysts through surface engineering can optimize the adsorption energy of intermediate molecules and improve the selectivity of organic electrooxidation ***,we summarized the recent research progress of 1D nanocatalysts applied in different organic electrooxidation reactions and introduced several different fabrication strategies for surface engineering of 1D ***,we focused on the relationship between surface engineering and the selectivity of organic electrooxidation reaction ***,future challenges and development prospects of 1D nanocatalysts in the coupled system consisting of organic electrooxidation and hydrogen evolution reactions are briefly outlined.

关键词： hydrogen generation organic compound electrooxidation one-dimensional(1D)nanocatalysts surface engineering selectivity

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Enhancing the deep-red/near-infrared fluorescence of higher rylene diimides via the chalcogen-annulation strategy

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Science china chemistry 2024年第4期67卷 1324-1333页

作者： Kai Chen Xiao Chen Ke Hu Yilun Zhao yujian liu Guogang liu Jinquan Chen Wei Jiang Zhigang Shuai Da-Hui Qu Zhaohui Wang key laboratory for Advanced Materials and Joint Inter{2. Research laboratory of Precision chemistry and molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China key laboratory of {2. Optoelectronics and molecular Engineering Department of ChemistryTsinghua UniversityBeijing 100084China State key laboratory of Precision Spectroscopy East China Normal University500 Dongchuan RoadShanghai 200241China

Deep-red/near-infrared fluorescence is highly suitable for bioimaging owing to its ability to deeply penetrate tissues,organs,and live ***,developing organic fluorophores with high deep-red/near-infrared fluorescence quantum yield(Φ_(FL))and fluorescent brightness remain a significant challenge owing to the energy gap ***,we developed a straightforward and effective chalcogen-annulation strategy by introducing O,S and Se into the bay region of TDI and QDI fluorophores,realizing the increase ofΦFLand fluorescent brightness up to 10 *** our best knowledge,this study potentially stands as the pioneering instance showcasing the anti-heavy-atom effect of chalcogens,and the absoluteΦFL(93%)and fluorescent brightness(12.,2.0 cm^(-1)mol^(-1)L)of Se-TDI is among top deep-red/near-infrared organic fluorophores currently *** femtosecond transient absorption(fs-TA)measurements show the absence of obvious changes of the excited state lifetime after the introduction of chalcogens in TDI and QDI fluorophores,indicating that intersystem crossing(ISC)can be neglected in TDI and QDI *** calculations further reveal the chalcogen-annulation strategy increase the radiative rates and reduce the reorganization energy of several accepting modes at the ground state in TDI fluorophores,leading to the suppression of internal conversion(IC)*** chalcogen-annulation strategy,which effectively increases the Φ_(FL)and restricts the IC processes,while remaining unaffected by the heavy-atom effect,offers novel insights and theoretical support for the design and synthesis of deep-red/near-infrared organic fluorophores with high Φ_(FL)and fluorescent brightness.

关键词： π-extended rylene diimides chalcogen-annulation strategy deep-red/near-infrared fluorescence

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New Strategy to Construct Fused/Bridged/Spiro Carbocyclic Scaffolds Based on the Design of Novel 6-C Synthon Precursor

New Strategy to Construct Fused/Bridged/Spiro Carbocyclic Sc...

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第十六届全国金属有机化学学术讨论会

作者： Jia liu,~(1,2) Xi Wang,~1 Chang-Liang Sun,~1 Bi-Jie Li,~1 Min Wang,~2 Zhang-Jie Shi~(*1,3) 1 beijing national laboratory of molecular sciences(BNLMS) and key laboratory of Bioorganic chemistry and molecular Engineering of Ministry of Education,College of chemistry and molecular Engineering and Green chemistry Center,Peking University,beijing 100871 and Department of chemistry,2 University of Agriculture of china,beijing 100094 and 3 State key laboratory of Organometallic chemistry,Shanghai institute of organic chemistry,chinese academy of sciences,Shanghai 200032,china

＜正＞Fused/bridged/spiro carbocyclic ring scaffolds are one of most important motifs in natural and synthetic organic *** design a new 6-C synthon,which could be applied to construct complex poly-,spiro-and bridged systems through the simple sequential chemical transformations from acyclic precursor by a one-pot strategy from

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Significant enhancement in local thermal conductivity of erythritol at interface with nanoparticles due to their interaction

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Nano Research 2024年第8期17卷 7726-7736页

作者： Ning Cao Yanhui Feng Kening Yan Zihan liu Jiawei Wan Lin Qiu School of Energy and Environmental Engineering University of Science and Technology BeijingBeijing 100083China State key laboratory of Biochemical Engineering Key Laboratory of Biopharmaceutical Preparation and DeliveryInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China

When nano-fillers are used to enhance the thermal conductivity of organic phase change materials(PCMs),the naturally formed interface is considered to hinder thermal transport of the composite ***,the effect of the interface on the thermal properties of surrounding PCM has not been fully *** this paper,three composite PCMs(Ery@SiC,Ery@SiO_(2. and Ery@Si_(3)N_(4))were prepared by melt-blending *** local thermal conductivity and reduced Young’s modulus(E^(*))of the erythritol at the interface and far away from the interface in the composite PCMs were simultaneously measured by scanning thermal microscopy(SThM).The results revealed significant enhancement in local thermal conductivity of erythritol at the interface and its obvious positive correlation with E^(*).For different composite PCMs,molecular dynamics(MD)simulations suggested that the increase in intrinsic thermal conductivity and E^(*)of erythritol is attributed to the increase in interaction energy between erythritol and nanoparticles,as more erythritol phonon vibrations transform from localized mode to delocalized mode and erythritol has a higher density at the *** findings will provide new ideas for the design of PCM for energy storage.

关键词： scanning thermal microscopy phase change materials thermal conductivity reduced Young’s modulus interaction energy phonon participation ratio

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Development of an automatic measurement system using atmospheric pressure photoionization ultrahigh-resolution mass spectrometry and application for on-line analysis of particulate matter

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Journal of Environmental sciences 2024年第4期138卷 516-530页

作者： Yayuan Dong Ranran liu Ling Xie Xiaole Pan Yele Sun Lin Wu ZifaWang State key laboratory of Atmospheric Boundary Layer Physics and Atmospheric {2. Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China College of Earth and Planetary sciences University of Chinese Academy of SciencesBeijing 100049China Center for Excellence in Regional Atmospheric Environment Chinese Academy of SciencesInstitute of Urban EnvironmentXiamen 361021China

On-line chemical characterization of atmospheric particulate matter(PM)with soft ionization technique and ultrahigh-resolution Mass Spectrometry(UHRMS)provides molecular information of organic constituents in real *** we describe the development and application of an automatic measurement system that incorporates PM_(2.5)sampling,thermal desorption,atmospheric pressure photoionization,and UHRMS *** formulas of detected organic compounds were deducted from the accurate(±10 ppm)molecular weights obtained at a mass resolution of 100,000,allowing the identification of small organic compounds in PM_(2.5).Detection efficiencies of 2. standard compounds were determined and we found a high sensitivity and selectivity towards organic amines with limits of detection below 10 *** a proof of principle,PM_(2.5)samples collected off-line in winter in the urban area of beijing were analyzed using the Ionization Module and HRMS of the *** automatic system was then applied to conduct on-line measurements during the summer time at a time resolution of 2.*** detected organic compounds comprised mainly CHON and CHN compounds below 350 m/*** seasonal variations in elemental composition were observed with shorter carbon backbones and higher O/C ratios in summer than that in *** result is consistent with stronger photochemical reactions and thus a higher oxidation state of organics in *** variation in signal intensity of each formula provides crucial information to reveal its source and formation *** summary,the automatic measurement system serves as an important tool for the on-line characterization and identification of organic species in PM_(2.5).

关键词： PM_(2.5) Chemical composition On-line measurement technique High resolution mass spectrometry

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Coexistence of solvatomagnetic effect and spin-glass behavior in a 1D coordination polymer constructed from EE-azido bridged Mnn3ⅢO Units

Coexistence of solvatomagnetic effect and spin-glass behavio...

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The 9th china-Japan Joint Symposium on Conduction and Photoconduction in organic {2. and Related Phenomena

作者： Cai-Ming liu De-Qing Zhang Dao-Ben Zhu beijing {2. laboratory for molecular sciences,Center for molecular Science,institute of chemistry,CAS,beijing 100080,P.R.china

The magnetic properties of molecular magnets can be modulated by a small change of circumstance,as illustrated by solvatomagnetic *** examples with such effect have been reported,most of them are high-dimensional porous coordination polymer molecular *** the other hand,azido-bridged coordination polymer molecular magnets or single molecular magnets have received increasing attention,however,the study on other magnetic phenomenon such as spin-glass behavior in this type of complex is still lacking. Herein we report the first 1D azido-bridged coordination polymer exhibiting not only solvatomagnetic effect but also spin-glass behavior,[MnO（Brppz）（MeOH）（N）] 2.eOH[1,Brppz=3-（5-bromine-2.phenolate）pyrazolate],which is constructed from EE-azido bridged MnO cluster ***,after losing its crystallized solvents,1 became another complex [MnO（Brppz）（MeOH）（N）]（2.,which no longer displays spin-glass behavior.

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Water-Excluding Underwater Glue Induced by Marangoni Effect

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CCS chemistry 2024年第5期6卷 1289-1299页

作者： Ke Zhang Xizi Wan Zi-yu liu Feilong Zhang Jingwei Lu Jingxin Meng Ye Tian Haeshin Lee Lei Jiang Shutao Wang CAS key laboratory of Bio-Inspired Materials and Interfacial Science Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190 Green Catalysis Center College of ChemistryZhengzhou UniversityZhengzhou 450001 University of chinese academy of sciences Beijing 100049 institute of Engineering Thermophysics Chinese Academy of SciencesBeijing 100190 beijing key {2. for Bioengineering and Sensing Technology School of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083 The Graduate School of Nanoscience and Technology Korea Advanced Institute of Science and Technology(KAIST)Daejeon 34141

Marangoni effect at the two-phase interface with different surface tension as a unique mass transfer phenomenon has been widely used in daily life and ***,their marvelous liquid-driving capability between miscible liquids has long been ignored,especially in water ***,we first reveal a distinct underwater Marangoni effect between the solvent of glues and the water layer on solid *** by the Marangoni effect,organic solvents with water solubility,high dielectric constant,and low diffusivity could effectively exclude the interfacial water layer,enabling direct and effective contact between glues and solid *** experimental results and theoretical simulation proved that a relatively large ratio of the Marangoni number in the horizontal direction and to the vertical direction ensured an effective underwater adhesion of the water-excluding *** surface engineering approach provides an alternative to the traditional methods of molecular engineering for realizing underwater adhesion.

关键词： Marangoni effect underwater adhesion dynamic water-excluding water layer solvent diffusion

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Strong metal-support interactions between highly dispersed Cu^(+) species and ceria via mix-MOF pyrolysis toward promoted water-gas shift reaction

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Journal of Energy chemistry 2024年第4期91卷 475-483页

作者： Xiao-Chen Sun Xing-Chi Li Ze-Wei Xie Chen-yue yuan De-Jiu Wang Qian Zhang Xiao-yu Guo Hao Dong Hai-Chao liu Ya-Wen Zhang beijing national {2. for molecular sciences(BNLMS) State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China beijing national {2. for molecular sciences(BNLMS) College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China beijing national {2. for molecular sciences(BNLMS) State Key Laboratory for Structural Chemistry of Stable and Unstable SpeciesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

The modulation of metal-support interfacial interaction is significant but challenging in the design of high-efficiency and high-stability supported ***,we report a synthetic strategy to upgrade Cu-CeO_(2.interfacial interaction by the pyrolysis of mixed metal-organic framework(MOF)*** obtained highly dispersed Cu/CeO_(2.-MOF catalyst via this strategy was used to catalyze water-gas shift reaction(WGSR),which exhibited high activity of 40.5μmolCOgcat^(-1).s^(-1)at 300℃and high stability of about 12. *** on comprehensive studies of electronic structure,pyrolysis strategy has significant effect on enhancing metal-support interaction and then stabilizing interfacial Cu^(+)species under reaction *** Cu^(+)species and generated oxygen vacancies over Cu/CeO_(2.-MOF catalyst played a key role in CO molecule activation and H2. molecule dissociation,*** collaborated closely and then promoted WGSR catalytic performance in comparison with traditio nal supported *** study shall offer a robust approach to harvest highly dispersed catalysts with finely-tuned metal-support interactions for stabilizing the most interfacial active metal species in diverse heterogeneous catalytic reactions.

关键词： Cu-based catalyst MOF derivative Water-gas shift reaction Metal-support interaction

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Ionic liquids inhibit the dynamic transition fromα-helices toβ-sheets in peptides

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Fundamental Research 2024年第4期4卷 777-784页

作者： Ju liu Yanlei Wang Feng Huo Hongyan He beijing key {2. of Ionic Liquids Clean Process State Key Laboratory of Mesoscience and EngineeringCAS Key Laboratory of Green Process and EngineeringInstituteof Process EngineeringChineseAcademyof SciencesBeijing100190China Longzihu New Energy laboratory Zhengzhou Institute of Emerging Industrial TechnologyHenan UniversityZhengzhou 450000China University of chinese academyof {2. Beijing100049China

Abnormalities in the transition betweenα-helices andβ-sheets(α-βtransition)may lead to devastating neurodegenerative diseases,such as Parkinson's syndrome and Alzheimer's *** liquids(ILs)are potential drugs for targeted therapies against these diseases because of their excellent bioactivity and designability of ***,the mechanism through which ILs regulate the aα-βtransition remains ***,a combination of GPU-accelerated microsecond molecular dynamics simulations,correlation analysis,and machine learning was used to probe the dynamicalα-βtransition process induced by ILs of 1-alkyl-3-methylimidazolium chloride([C_(n)mim]cl)and its molecular ***,the cation of [C_(n)mim]+in ILs can spontaneously insert into the peptides as free ions(n≤10)and clusters(n≥11).Such insertion can significantly inhibit theα-β,transition and the inhibiting ability for the clusters is more significant than that of free ions,where[Ciomim]+and[C_(12.mim]+can reduce the maximumβ-sheet content of the peptide by 18.5% and 44.9%,***,the correlation analysis and machine learning method were used to develop a predictive model accounting for the influencing factors on theα-βtransition,which could accurately predict the effect of ILs on theα-β***,these quantitative results may not only deepen the understanding of the role of ILs in theα-βtransition but also guide the development of the IL-based treatments for related diseases.

关键词： α-βtransition moleculardynamics simulation lonic liquids Machine learning Membrane channel protein

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本征柔性有机电子器件的研究进展

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科学通报 2024年第10期69卷 1279-1297页

作者：史文康赵志远郭云龙刘云圻中国科学院化学研究所有机固体重点实验室北京分子科学国家研究中心北京100190 中国科学院大学化学科学学院北京100049

本征柔性有机电子学是近年来涌现的一项变革性的前沿交叉学科,它赋予电子材料可印刷、可折叠和可拉伸等特性,使其应用于健康医疗、柔性显示、传感探测、人工智能和脑机接口等前沿领域.为了进一步拓展本征柔性有机电子器件的应用场景,设... 详细信息

本征柔性有机电子学是近年来涌现的一项变革性的前沿交叉学科,它赋予电子材料可印刷、可折叠和可拉伸等特性,使其应用于健康医疗、柔性显示、传感探测、人工智能和脑机接口等前沿领域.为了进一步拓展本征柔性有机电子器件的应用场景,设计开发高性能、高显示度、高稳定性的本征柔性材料和有机电子器件是当前的研究重点.本文主要介绍了近年来本征柔性有机电子学相关领域的前沿研究进展,重点讨论了本征柔性材料与有机电子器件的设计和制备策略、本征柔性材料图案化工艺和集成电路,分析了本征柔性有机电子学领域的技术瓶颈和前沿问题,总结和展望了本征柔性有机电子器件的应用前景与未来发展趋势.

关键词：柔性电子本征柔性材料本征柔性有机器件图案化工艺本征柔性有机电路

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