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AI for organic and polymer synthesis

Science China chemistry 2024年第8期67卷 2461-2496页

作者： Xin Hong Qi Yang Kuangbiao Liao Jianfeng Pei Mao Chen Fanyang Mo Hua Lu Wen-Bin Zhang Haisen Zhou Jiaxiao Chen Lebin Su Shuo-Qing Zhang Siyuan Liu Xu Huang Yi-Zhou Sun Yuxiang Wang Zexi Zhang Zhunzhun Yu Sanzhong Luo Xue-Feng Fu Shu-Li You Center of chemistry for Frontier Technologies Department of ChemistryZhejiang UniversityHangzhou 310027China Center of Basic Molecular Science Department of ChemistryTsinghua UniversityBeijing 100084China Guangzhou National Laboratory Guangzhou 510005China Center for Quantitative Biology Academy for Advanced Interdisciplinary StudiesPeking UniversityBeijing 100871China State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200433China School of Materials Science and Engineering Peking UniversityBeijing 100871China Beijing National Laboratory for Molecular Sciences Center for Soft Matter Science and EngineeringKey Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China AI for Science(AI4S)-Preferred Program Shenzhen Graduate SchoolPeking UniversityShenzhen 518055China State Key Laboratory of Chemical Biology Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai 200032China Department of Chemical Sciences National Natural Science Foundation of ChinaBeijing 100085China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Recent years have witnessed the transformative impact from the integration of artificial intelligence with organic and polymer synthesis. This synergy offers innovative and intelligent solutions to a range of classic problems in synthetic chemistry. These exciting advancements include the prediction of molecular property, multi-step retrosynthetic pathway planning, elucidation of the structure-performance relationship of single-step transformation, establishment of the quantitative linkage between polymer structures and their functions, design and optimization of polymerization process, prediction of the structure and sequence of biological macromolecules, as well as automated and intelligent synthesis platforms. Chemists can now explore synthetic chemistry with unprecedented precision and efficiency, creating novel reactions, catalysts, and polymer materials under the datadriven paradigm. Despite these thrilling developments, the field of artificial intelligence(AI) synthetic chemistry is still in its infancy, facing challenges and limitations in terms of data openness, model interpretability, as well as software and hardware support. This review aims to provide an overview of the current progress, key challenges, and future development suggestions in the interdisciplinary field between AI and synthetic chemistry. It is hoped that this overview will offer readers a comprehensive understanding of this emerging field, inspiring and promoting further scientific research and development.

关键词： organic synthesis polymer synthesis machine learning prediction chemical database automated synthesis

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Beyond Conventional Degradation:Catalytic Solutions for Polyolefin Upcycling

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CCS chemistry 2024年第2期6卷 313-333页

作者： Lan Gan Zhongwen Dong Haofeng Xu Huidong Lv Guixia Liu Fan Zhang Zheng Huang State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai 200032 School of chemistry and Material Sciences Hangzhou Institute of Advanced StudyHangzhou 310024 National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan) College of ChemistrySichuan UniversityChengdu 610064

Polyolefins(POs,i.e.,polyethylenes,ethylene/α-olefin copolymers,and polypropylenes)are the most ubiquitous synthetic macromolecular materials in modern *** widespread use and low recovery rate after extensive usage have caused significant resource waste and environmental *** recycling of POs provides an efficient approach to unravelling the polymer chain to various ***,conventional chemical recycling methods,including pyrolysis,hydrocracking,and oxidation,require high-energy input(typically>500℃)and/or the use of environmentally unfriendly chemicals,leading to complex product *** this minireview,based on recent representative works,we summarize and highlight catalytic strategies addressing these issues in PO recycling from two perspectives:(1)employing advanced catalysts or technique designs to overcome the challenges in conventional chemical deconstruction approaches;and(2)developing novel tandem/cascade catalytic systems for highly selective PO upcycling under relatively mild *** hope that this minireview will help researchers better understand the state of the art of PO chemical recycling and inspire more innovative and efficient ideas for this fast-developing field.

关键词： catalytic strategies chemical recycling deconstruction polyolefins upcycling

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Heterocyclic Molecules Tethered Branched Polymers with Innate Immune Stimulating Activity

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CCS chemistry 2024年第5期6卷 1278-1288页

作者： Jiayu Zhao Liping Liu Yibo Wang Zichao Huang Yu Zhang Ruirui Qiao Thomas P.Davis Zhaohui Tang Wantong Song Xuesi Chen Key Laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022 School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026 Laboratory of Chemical Biology Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022 Jilin Biomedical Polymers Engineering Laboratory Changchun 130022 Australian institute of Bioengineering and Nanotechnology The University of QueenslandBrisbaneQueensland 4072

We report herein an interesting finding that heterocyclic molecules tethered branched polymers exhibit innate immune stimulating *** we conjugated a series of five-,six-,or seven-membered heterocyclic molecules to branched polyethylenimine(bPEI),over 70%of them could induce the secretion of interferon-β(IFN-β)from murine dendritic and human leukemia monocytic(DC2.4 and THP-1)cells through activating the stimulator of interferon genes(STING)*** further proved that this kind of innate stimulating activity was dependent on the macromolecular architecture as heterocyclic molecules tethered linear PEI(lPEI)or dendritic polyamidoamine(PAMAM)induced no or much less IFN-β***,we prepared a series of poly-L-lysine(PLL)-derivatives with different branches to tether with heterocyclic molecules and proved that this kind of bPEI-like structure was important in en hancing the binding affinity with STING proteins and for exhibiting innate stimulating activity.

关键词： bioactive materials polymers heterocycles branched structure immunity

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Green synthesis of luminescent La-MOF nanoparticle from waste poly(ethylene terephthalate) for high-performance in Fe(Ⅲ) detection

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Rare Metals 2024年第8期43卷 3833-3843页

作者： Zhi Gong Zhi-Kui Dai Zhi-Yue Dong Qiu-Xuan Liu Valentin A.Milichko Hua-Jian Liu Jie Liu Ran Niu Jiang Gong Key Laboratory of Material chemistry for Energy Conversion and Storage Hubei Key Laboratory of Material Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsSemiconductor Chemistry CenterSchool of Chemistry and Chemical EngineeringMinistry of EducationHuazhong University of Science and Technology School of Chemical Engineering and Pharmacy Wuhan Institute of Technology Collaborative Innovation Center for Advanced Organic Chemical Materials Co-constructed by the Province and Ministry Ministry of Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules and College of Chemistry and Chemical EngineeringHubei University School of Physics and Engineering ITMO University School of Materials Science and Engineering Hubei University Guangdong Provincial Key Laboratory of Technique and Equipment for macromolecular Advanced Manufacturing School of Mechanical and Automotive EngineeringKey Laboratory of Polymer Processing EngineeringMinistry of EducationSouth China University of Technology

Developing luminescent metal-organic frameworks（MOFs） capable of high-efficiency Fe3+sensing has aroused great attraction in the fields of biology,chemistry,***,previous solvothermal methods are limited by organic solvent usage,time consuming,high pressure,and high-energy ***,we propose the waste-toMOF strategy towards the scale-up production of La-MOF nanoparticles through the ball milling of recycled poly（-ethylene terephthalate）(PET) bottles and La（NO3）3·*** goes on alkaline hydrolysis to form 1,4-benzenedicarboxylic acid sodium salt（Na2BDC） and ethylene glycol by ball ***,BDC reacts with La3+to form *** as-prepared La-MOF crystal nanoparticles possess a rod-like morphology with the size of few hundred ***,La-MOF nanoparticles display high selectivity and sensitivity for Fe3+*** quenching constant and limit of detection are 5.29×10～3(mol·L-1)-1and 0.147 μmol·L-1,respectively,thus surpassing many advanced Fe3+*** to the result of density functional theory,the high Fe3+detection performance of La-MOF is related to the complexing of Fe3+with La-MOF,which leads to the gradual dissociation of the coordination bond between terephthalic acid and La3+.It is anticipated that the mechanochemistry milling-based wasteto-MOF strategy provides a new platform for the massive production of functional MOFs in a green manner.

关键词： Metal–organic framework Waste polyester Mechanochemistry milling Fluorescence sensor

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Heterogeneous MXene-based films with graded electrical conductivity towards highly efficient EMI shielding and electrothermal heating

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Nano Research 2024年第8期17卷 7264-7274页

作者： Yu Zhang Guangcheng Zhang Zhonglei Ma Jianbin Qin Xi Shen Department of Aeronautical and Aviation Engineering The Hong Kong Polytechnic UniversityHung HomKowloonHong KongChina Shaanxi Key Laboratory of macromolecular Science and Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710072China Research institute for Sports Science and Technology The Hong Kong Polytechnic UniversityHung HomKowloonHong KongChina

The increasing need for electromagnetic interference(EMI)shielding of electronics in cold environments such as those in aircraft,space exploration,and wearable heaters to avoid hazardous icing conditions or hypothermia requires the development of thin and lightweight EMI shielding materials preferably by absorbing rather than reflecting electromagnetic(EM)waves while also generating heat through energy-efficient electrothermal ***,it is challenging to achieve absorption-dominant EMI shielding and energy-efficient electrothermal heating simultaneously in a thin and lightweight ***,we develop a heterogeneous composite film comprising a porous multi-walled carbon nanotubes(MWCNTs)/bacterial cellulose(BC)film and an aligned MXene/Ag nanowires(NWs)backing via a sequential vacuum filtration *** porous film contains random conductive networks of MWCNTs with moderate conductivity while the aligned MXene sheets atop Ag NWs network affords high conductivity in the backing,giving rise to graded electrical conductivity for absorption-dominant EMI *** increasing Ag NW coverage leads to significantly increased electrical conductivity without increasing the EM wave reflection as well as the density and thickness of the film,yielding excellent specific EMI shielding effectiveness(>8500 dB/(g·cm^(2))),low driving voltage for energy-efficient electrothermal heating(163℃at 2.5 V),and fast response time(60 s)at a low areal density of 0.015 mg/cm^(2).Combining EMI shielding and electrothermal heating,the heterogeneous film developed here are promising contenders for the protection of electronic equipment in low-temperature environment.

关键词： heterogenous composite film MXene electromagnetic interference(EMI)shielding thermal management

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The superiority of nonconjugated structures in fluorescence:through-space vs. through-bond charge transfer

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Science China chemistry 2024年第9期67卷 3121-3130页

作者： Weihao Tu Zuping Xiong Lei Wang Jianyu Zhang Jing Zhi Sun Haoke Zhang Ben Zhong Tang MOE Key Laboratory of macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Zhejiang-Israel Joint Laboratory of Self-Assembling Functional Materials ZJU-Hangzhou Global Scientific and Technological Innovation Center Zhejiang University Centre of Healthcare Materials Shaoxing Institute Zhejiang University Department of chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and ReconstructionThe Hong Kong University of Science and Technology School of Science and Engineering Shenzhen Institute of Aggregate Science and Technology The Chinese University of Hong KongShenzhen(CUHK-Shenzhen)

Constructing charge transfer（CT） state by introducing donor（D） and acceptor（A） is an efficient strategy to regulate the photophysical properties of luminescent materials. Traditional CT-type luminophores are built on π-conjugated fused-ring structures, which always show hybrid CT/locally excited（LE） states and luminescence quenching effect in the aggregate state. In this work, eight conjugated biphenyl（BP） and nonconjugated diphenylmethane（DPM） derivatives with different donors and acceptors are synthesized to investigate the CT properties. Systematic photophysical characterization and theoretical calculation demonstrate that the through-space CT（TSCT） in nonconjugated DA-DPM exhibit superior photophysical performance than the conjugated DA-BP with through-bond CT（TBCT）, the main manifestations are as follows:（1） TSCT luminophores produce longer maximum emission wavelength(λem) than the corresponding TBCT ones. For example, the longest λemof DMA-CN-DPM（DMA, dimethylamino） is 621 nm but the corresponding λemof DMA-CN-BP is only 480 nm.（2） TSCT-based DA-DPM demonstrates more sensitive responsiveness to environmental stimuli such as temperature and polarity.（3） Complete separation of the the highest occupied molecular orbital（HOMO） and the lowest unoccupied molecular orbital（LUMO） distribution exists in all kinds of conformation of DA-DPM, which was hard to realize in conjugated DA-BP.

关键词： through-space charge transfer through-space conjugation clusteroluminescence diphenylmethane

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Cellulose-MXene composites: New platforms with outstanding multifunctional characteristics

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Journal of Bioresources and Bioproducts 2024年第3期9卷 243-245页

作者： Farzad Seidi Wensi Jiang Zhaochuan Yu Chao Deng Jiangsu Co-Innovation Center for Efficient Processing and Utilization of Forest Resources and International Innovation Center for Forest Chemicals and Materials Nanjing Forestry UniversityNanjing 210037China macromolecular chemistry and Bavarian Polymer institute University of BayreuthBayreuth 95440Germany

The progress of society has caused a quick rise in the requirement for materials with superior *** composite materials demonstrate exceptional performance due to the synergistic effects resulting from the combination of unique properties exhibited by their constituent *** advantageous characteristic enables these materials to leverage the collective strengths of each component,leading to their outstanding *** leveraging the strengths of each individual component,the shortcomings can be overcome and the strong points can be shared effectively.

关键词： composites MXene composite

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Polysulfide modified PtCu intermetallic nanocatalyst with enrichment realizes efficient electrooxidation ethanol to CO_(2)

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Nano Research 2024年第4期17卷 2320-2327页

作者： Shuanglong Zhou Zheng Lv Liang Zhao Dan Zhang Zuocao Wang Yu Dai Bin Li Olga Starostenko Jianping Lai Lei Wang Key Laboratory of Eco-chemical Engineering Ministry of EducationTaishan scholar advantage and characteristic discipline team of Eco-chemical process and technologyLaboratory of Inorganic Synthesis and Applied ChemistryCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Foreign Languages Qingdao City UniversityQingdao 266106China College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China institute of macromolecular chemistry of the National Academy of Sciences of Ukraine Kyiv 02160Ukraine Shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042China

The main problem faced by ethanol oxidation reaction(EOR)includes low activity,poor selectivity,and *** the study,we found that polysulfide modified on the surface of PtCu intermetallic(IM)/C can simultaneously enrich hydroxyl and ethanol,which could effectively improve the catalytic activity,CO_(2) selectivity,and durability of *** mass activity and the specific activity of the product in 1 M KOH electrolyte reached 17.83 A·mgPt^(-1) and 24.67 mA·cm^(-2).The CO_(2) selectivity of polysulfide modified product achieved 93.5%,which was 30 folds higher than Pt/*** addition,the catalyst showed high catalytic *** mechanism study demonstrates that the surface modified polysulfide could significantly boost the enrichment effect of ethanol and hydroxyl species,accelerating C–C bond cleavage and CO oxidation.

关键词： Pt CO_(2) selectivity enrichment effect ethanol oxidation reaction(EOR) electrocatalyst

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Author Spotlight

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CCS chemistry 2024年第3期6卷 532-536页

Yanli Tang(唐艳丽)*** received her *** in chemical engineering in 2001 from the Department of chemistry and Chemical Engineering at Henan University,China,and her *** in chemistry in 2004 from Lanzhou institute of Che... 详细信息

关键词： Henan Lanzhou Spotlight

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Renewable Biomass as a Platform for Preparing Green chemistry

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Journal of Renewable Materials 2024年第2期12卷 325-328页

作者： Qiaoguang Li Puyou Jia Ying Luo Yue Liu College of chemistry and Chemical Engineering Zhongkai University of Agriculture and EngineeringGuangzhou510225China institute of Chemical Industry of Forestry Products Chinese Academy of ForestryNanjingChina College of Materials and Energy South China Agricultural UniversityGuangzhou510642China College of Chemical Engineering Qingdao University of Science and TechnologyQingdao266061China

1 About the Special Issue Editor Qiaoguang Li is an associate professor and master’s supervisor in the Department of College of chemistry and Chemical Engineering,Zhongkai University of Agriculture and *** received his PhD from institute of Chemical Industry of Forestry Products,Chinese Academy of Forestry in *** has been focusing his research on the chemical basis and application of natural *** has published nearly 30 international peer reviewed papers and applied for 10 patents.

关键词： Biomass Platform patent

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