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Keto-form directed hierarchical chiral self-assembly of Schiff base derivatives with amplified circularly polarized luminescence

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Chinese Chemical Letters 2024年第1期35卷 366-370页

作者： Yimeng Sun Yuqian Jiang Jian Jiang Tiesheng Li minghua liu Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001China Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China National Laboratory for Molecular Science(BNLMS) CAS Laboratory of ColloidInterface and Chemical ThermodynamicsInstitute of ChemistryChinese Academy of ScienceBeijing 100190China University of Chinese Academy of Sciences Beijing 100190China

While enol-keto tautomerism has attracted great interest in Schiff bases and related compounds in solution and crystal states,the self-assembly of energy-unfavored keto form were scarcely investigated.Here,we report a keto-form directed self-assembly of a naphthalene-attached enantiomeric N-salicylideneanil analog L/DGG-Nap accompanied with a significantly amplified circularly polarized luminescence(CPL).It was found that LGG-Nap exists as a mixture of enol and keto form in monomer at a diluted toluene solution.The increment of the concentrations leads to the formation of predominated keto form,which subsequently triggers the self-assembly.Cryo-transmission electron microscopy(Cryo-TEM)revealed that a hierarchical assembly process happened upon increasing the concentration of LGG-Nap in toluene.Individual nanofibers formed at 1×10-4 mol/L and transferred into helical nanofiber bundles in 5×10-3 mol/L.Interestingly,while these is nearly no circular dichroism(CD)or CPL in the monomeric solution,the assembly showed strong CD and CPL.Remarkably,the dissymmetry factor(glum)was significantly amplified from zero in solution through the 0.005 in individual nanofiber to 0.1 in nanofiber bundles.This work demonstrates that the enol-keto tautomerism can be broken and trigger the self-assembly upon increasing the concentration,which can subsequently direct the chiral self-assembly and significantly amplify the dissymmetry factor of assembled CPL materials.

关键词： Enol-keto tautomerism Chiral self-assembly Schiff base Circularly polarized luminescence Nanofiber bundle

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Stress-corrosion coupled damage localization induced by secondary phases in bio-degradable Mg alloys:phase-field modeling

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Journal of Magnesium and Alloys 2024年第1期12卷 361-383页

作者： Chao Xie Shijie Bai Xiao liu minghua Zhang Jianke Du The Faculty of Mechanical Engineering and Mechanics Ningbo UniversityNingbo 315211P.R.China Key Laboratory of High Temperature Wear Resistant Materials Preparation Technology of Hunan Province Hunan University of Science and TechnologyXiangtan 411201P.R.China

In this study,a phase-field scheme that rigorously obeys conservation laws and irreversible thermodynamics is developed for modeling stress-corrosion coupled damage(SCCD).The coupling constitutive relationships of the deformation,phase-field damage,mass transfer,and electrostatic field are derived from the entropy inequality.The SCCD localization induced by secondary phases in Mg is numerically simulated using the implicit iterative algorithm of the self-defined finite elements.The quantitative evaluation of the SCCD of a C-ring is in good agreement with the experimental results.To capture the damage localization,a micro-galvanic corrosion domain is defined,and the buffering effect on charge migration is explored.Three cases are investigated to reveal the effect of localization on corrosion acceleration and provide guidance for the design for resistance to SCCD at the crystal scale.

关键词： Phase field Mg alloys Stress-corrosion coupled damage Damage localization Finite element method

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Robust Carbon-Carbon Cleavage in Lignin to Produce Phenol and Cyclohexanone

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Chemical Research in Chinese Universities 2024年第1期40卷 29-35页

作者： WANG Lulin CHENG Xiaomeng DONG minghua LUAN Sen WU Yuxuan HAN Buxing liu Huizhen Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesCenter for Carbon Neutral ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing 100190P.R.China University of Chinese Academy of Sciences Beijing 100049P.R.China

The challenge of breaking 5-5'bonds in lignin,attributed to their high bonding energy,has prompted the development of a new transformation pathway.Biphenyl,an important model compound for lignin,contains these 5-5'bonds,making it crucial to devise a strategy for their cleavage in lignin transformation.This study introduces a novel method for transforming biphenyl,involving selective hydrogenation to cyclohexylbenzene by Ni/SiO2 catalyst,followed by its oxidation to phenol and cyclohexanone through a radical mechanism.Results demonstrate that the catalysts with small particles have strong catalytic activity,while there is little difference in selectivity.The reason for the high selectivity of cyclohexylbenzene is due to the limited adsorption of cyclohexylbenzene on Ni/SiO2.This work presents a fresh approach to breaking resilient C-C bonds in lignin.

关键词： Lignin 5-5'Bond Ni/SiO_(2) Phenol

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Bifunctional TiO_(2-x)nanofibers enhanced gel polymer electrolyte for high performance lithium metal batteries

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Journal of Energy Chemistry 2024年第2期89卷 437-448,I0011页

作者： Yixin Wu Zhen Chen Yang Wang Yu Li Chunxing Zhang Yihui Zhu Ziyu Yue Xin liu minghua Chen Key Laboratory of Engineering Dielectric and Applications(Ministry of Education) School of Electrical and Electronic EngineeringHarbin University of Science and TechnologyHarbin 150080HeilongjiangChina

Exploration of advanced gel polymer electrolytes(GPEs)represents a viable strategy for mitigating dendritic lithium(Li)growth,which is crucial in ensuring the safe operation of high energy density Li metal batteries(LMBs).Despite this,the application of GPEs is still hindered by inadequate ionic conductivity,low Li^(+)transference number,and subpar physicochemical properties.Herein,Ti O_(2-x)nanofibers(NF)with oxygen vacancy defects were synthesized by a one-step process as inorganic fillers to enhance the thermal/mechanical/ionic-transportation performances of composite GPEs.Various characterizations and theoretical calculations reveal that the oxygen vacancies on the surface of Ti O_(2-x)NF accelerate the dissociation of Li PF_6,promote the rapid transfer of free Li^(+),and influence the formation of Li F-enriched solid electrolyte interphase.Consequently,the composite GPEs demonstrate enhanced ionic conductivity(1.90m S cm^(-1)at room temperature),higher lithium-ion transference number(0.70),wider electrochemical stability window(5.50 V),superior mechanical strength,excellent thermal stability(210℃),and improved compatibility with lithium,resulting in superior cycling stability and rate performance in both Li||Li,Li||Li Fe PO_(4),and Li||Li Ni_(0.8)Co_(0.1)Mn_(0.1)O_(2)cells.Overall,the synergistic influence of nanofiber morphology and enriched oxygen vacancy structure of fillers on electrochemical properties of composite GPEs is comprehensively investigated,thus,it is anticipated to shed new light on designing high-performance GPEs LMBs.

关键词： Nanofibers fillers Oxygen vacancies Gel polymer electrolytes Lithium metal batteries

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Propeller-shaped NI isomers of cathode interfacial material for efficient organic solar cells

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Nano Research 2024年第3期17卷 1564-1570页

作者： Hao liu Jilei Jiang Shuixing Dai Liangmin Yu Xu Zhang Xianbiao Hou Ke Gao Heqing Jiang minghua Huang School of Materials Science and Engineering Ocean University of ChinaQingdao 266100China Open Studio for Marine Corrosion and Protection Pilot National Laboratory for Marine Science and TechnologyQingdao 266100China Science Center for Material Creation and Energy Conversion Institute of Frontier and Interdisciplinary ScienceShandong UniversityQingdao 266237China Qingdao Key Laboratory of Functional Membrane Material and Membrane Technology Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101China

Cathode interfacial materials(CIMs)stand as critical elemental in organic solar cells(OSCs),which can align energy levels,and foster ohmic contacts between the cathode and active layer of the OSCs.Nevertheless,the lagging advancement in CIMs has concurrently engendered the oversight of theoretical inquiries pertaining to the impact of molecular structure on their performance.Delving into this realm,we present two propeller-shaped isomers,4,4',4''-(benzo[1,2-b:3,4-b':5,6-b'']trithiophene-2,5,8-triyl)tris(2-(3-(dimethylamino)propyl)-1H-benzo[de]isoquinoline-1,3(2H)-dione)(3ONIN)and 6,6',6''-(benzo[1,2-b:3,4-b':5,6-b'']trithiophene-2,5,8-triyl)tris(2-(3-(dimethylamino)propyl)-1H-benzo[de]isoquinoline-1,3(2H)-dione)(3PNIN),distinguished by their molecular planarity,as a promising foundation for crafting highly efficient OSCs.This study illuminates the superiority of 3PNIN with more plane structure,exemplified by its enhanced molar extinction coefficient,deeper lowest unoccupied molecular orbital(LUMO)and highest occupied molecular orbital(HOMO)energy levels,intensified self-doping effect,heightened electron mobility,and elevated conductivity,in comparison to its counterpart,3ONIN.As a result,3PNIN and 3ONIN-treated OSC devices yield efficiencies of 17.73%and 16.82%,respectively.This finding serves as a compelling validation of the critical role played by molecular planarity in influencing CIM performance.

关键词： propeller-shaped molecules naphthalimide(NI)isomers cathode interfacial materials organic solar cells

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Data cleaning method for the process of acid production with flue gas based on improved random forest

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中国化学工程学报:英文版 2023年第7期59卷 72-84页

作者： Xiaoli Li minghua liu Kang Wang Zhiqiang liu Guihai Li Faculty of Information Technology Beijing University of TechnologyBeijing 100124China Beijing Key Laboratory of Computational Intelligence and Intelligent System Engineering Research Center of Digital CommunityMinistry of EducationBeijing 100124China Guixi Smelter Jiangxi Copper Co.LtdGuixi 335400China Beijing RTlink Technology Co. LtdBeijing 100102China

Acid production with flue gas is a complex nonlinear process with multiple variables and strong coupling.The operation data is an important basis for state monitoring,optimal control,and fault diagnosis.However,the operating environment of acid production with flue gas is complex and there is much equipment.The data obtained by the detection equipment is seriously polluted and prone to abnormal phenomena such as data loss and outliers.Therefore,to solve the problem of abnormal data in the process of acid production with flue gas,a data cleaning method based on improved random forest is proposed.Firstly,an outlier data recognition model based on isolation forest is designed to identify and eliminate the outliers in the dataset.Secondly,an improved random forest regression model is established.Genetic algorithm is used to optimize the hyperparameters of the random forest regression model.Then the optimal parameter combination is found in the search space and the trend of data is predicted.Finally,the improved random forest data cleaning method is used to compensate for the missing data after eliminating abnormal data and the data cleaning is realized.Results show that the proposed method can accurately eliminate and compensate for the abnormal data in the process of acid production with flue gas.The method improves the accuracy of compensation for missing data.With the data after cleaning,a more accurate model can be established,which is significant to the subsequent temperature control.The conversion rate of SO_(2) can be further improved,thereby improving the yield of sulfuric acid and economic benefits.

关键词： Acid production Data cleaning Isolation forest Random forest Data compensation

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Stride the chirality transfer across length scales by merging the boundaries between solution and interfacial self-assembly

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Chinese Journal of Structural Chemistry 2023年第4期42卷 1-3页

作者： Guanghui Ouyang minghua liu CAS Key Laboratory of Colloid Interface and ThermodynamicsInstitute of ChemistryChinese Academy of SciencesNo.2 North First StreetZhongguancunBeijing100190China

The chiral self-assembly of functional molecules,polymers and clus-ters into nanoscale objects with well-defined ordering,asymmetry and in some cases out-of-equilibrium characteristics is an important strategy to fabricate novel materials[1],which might address key challenges at the heart of energy,environmental and biomedical applications.In recent years,subsequent utilization of these nanoscale units as new building blocks to fabricate advanced structures and realize more complex func-tions like those in the biology systems has aroused interests.These at-tempts are originated from the concept of molecular nanotechnology but have gone beyond its boundaries towards the breakthroughs of self-assembled machines,advanced nanoarchitectonics and molecular nanotopology[2,3].

关键词： interfacial breakthrough subsequent

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Chiral porphyrin assemblies

聚集体(英文)

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聚集体(英文) 2023年第1期4卷 27-40页

作者： Li Zhang TianyuWang Jianzhuang Jiang minghua liu Beijing National Laboratory for Molecular Science(BNLMS) CAS Key Laboratory of ColloidInterface and Chemical ThermodynamicsInstitute of ChemistryChinese Academy of SciencesBeijingP.R.China Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of ChemistryUniversity of Science and Technology BeijingBeijingP.R.China

Porphyrins are among the most important macrocycles because they perform many essential functions in living systems and serve as building blocks in many functional materials.Incorporating the chirality into porphyrins can aid biomimetic research and the exploration of new functional materials.In this review,recent developments in chiral porphyrin assemblies are highlighted.The review is mainly divided into two sections:the different strategies for constructing chiral porphyrin assemblies and the applications.The formation of chiral porphyrin assemblies can be from porphyrin molecules substituted with chiral groups;achiral porphyrins induced by chiral additives and spontaneous deracemizations of achiral porphyrins during the assemblies.We also provide an overview of the applications of chiral porphyrin assemblies in chiral sensing,asymmetry catalysis,circularly polarized luminescence,and so on.The further challenge in the field is discussed.

关键词： chiral circularly polarized luminescence helical porphyrins self-assembly

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Intelligent 3D garment system of the human body based on deep spiking neural network

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虚拟现实与智能硬件（中英文） 2024年第1期6卷 43-55页

作者： minghua JIANG Zhangyuan TIAN Chenyu YU Yankang SHI Li liu Tao PENG Xinrong HU Feng YU School of Computer and Artificial Intelligence Wuhan Textile UniversityWuhan 430200China Engineering Research Center of Hubei Province for Clothing Information Wuhan 430200China

Background Intelligent garments,a burgeoning class of wearable devices,have extensive applications in domains such as sports training and medical rehabilitation.Nonetheless,existing research in the smart wearables domain predominantly emphasizes sensor functionality and quantity,often skipping crucial aspects related to user experience and interaction.Methods To address this gap,this study introduces a novel real-time 3D interactive system based on intelligent garments.The system utilizes lightweight sensor modules to collect human motion data and introduces a dual-stream fusion network based on pulsed neural units to classify and recognize human movements,thereby achieving real-time interaction between users and sensors.Additionally,the system incorporates 3D human visualization functionality,which visualizes sensor data and recognizes human actions as 3D models in real time,providing accurate and comprehensive visual feedback to help users better understand and analyze the details and features of human motion.This system has significant potential for applications in motion detection,medical monitoring,virtual reality,and other fields.The accurate classification of human actions contributes to the development of personalized training plans and injury prevention strategies.Conclusions This study has substantial implications in the domains of intelligent garments,human motion monitoring,and digital twin visualization.The advancement of this system is expected to propel the progress of wearable technology and foster a deeper comprehension of human motion.

关键词： Intelligent garment system Internet of things Human action recognition Deep learning 3D visualization

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Atomically Dispersed Pt and NiO Clusters Synergistically Enhanced C–O Bond Hydrogenolysis

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CCS Chemistry 2024年第3期6卷 709-718页

作者： Junjuan Yang Sen Luan minghua Dong Yuxuan Wu Xueqing Xing Xingwu liu Junfeng Xiang Zhijuan Zhao Shaopeng Li Bin Zhang Huizhen liu Buxing Han Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and ThermodynamicsInstitute of ChemistryChinese Academy of SciencesBeijing 100190 School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049 Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsBeijing 100049 National Energy Center for Coal to Liquids Synfuels China Co.Ltd.Huairou DistrictBeijing 101400 Center for Physicochemical Analysis and Measurement Institute of ChemistryChinese Academy of SciencesBeijing 100190 Physical Science Laboratory Huairou National Comprehensive Science CenterUniversity of Chinese Academy of SciencesBeijing 100049

C–Obond activation is a highly efficient,fundamental strategy in the depolymerization and hydrodeoxygenation of chemicals with oxygen-containing functional groups such as oil,coal,and biomass.Developing efficient catalysts for C–Oactivation with ultralow-loading noble and non-noble metals is highly desirable for the improvement of metal atomic utilization.Herein,bimetallic catalysts with atomically dispersed Pt and NiO clusters on different supports were fabricated,and the prepared Pt^(δ+)-NiO/Nb_(2)O_(5)and Pt^(δ+)-NiO/TiO_(2)showed outstanding activity for the hydrogenolysis of benzyl phenyl ether with>99%yield of phenol and toluene due to the excellent cooperation of atomically dispersed Pt and NiO clusters.The synergy mechanism between Pt and Ni and their respective roles in the bimetallic catalyst for C–O hydrogenolysis were clearly clarified.These findings deepen our understanding of the synergy of the two active components and are expected to provide new design concepts for the development of multicomponents catalysts.

关键词： bimetallic catalysis synergistic effect C-O bond activation hydrogenolysis hydrogen spillover

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