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Rational Design of Plasmonic Nanoparticle-Molecule Complexes for Chirality Sensing

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Chinese Journal of Chemistry 2024年第8期42卷 903-919页

作者： Chen Wang dandan lu Lichao Sun Qingfeng Zhang College of Chemistry and Molecular Sciences Wuhan UniversityWuhanHubei430072 China

Comprehensive Summary,Sensing the chirality of molecules is of great importance to fields such as enantioselective synthesis,pharmaceutical industry,and biomedicine.Plasmonic nanoparticles are ideal candidates for molecular sensing due to their inherent plasmonic properties that significantly enhance their sensitivity to surrounding molecules.Developing plasmonic nanoparticle-molecule complexes for chirality sensing has drawn enormous attention in recent years due to their intriguing properties and potential applications.Thus,in this review,we believe it is timely to circumnavigate the rational design of plasmonic nanoparticle-molecule complexes and widen the scope of their emerging applications in chirality sensing.First,we present different fundamental mechanisms for plasmon-based chirality that are built on the system of plasmonic nanoparticle-molecule complexes.Second,we review the typical applications of plasmonic nanoparticle-molecule complexes in chirality sensing.Third,we discuss the emerging biomedical applications that the plasmon-based chirality has attracted enormous interest.Finally,we provide an outlook on the challenges and opportunities in the field of plasmonic approaches for chirality sensing.

关键词： Chirality Surface plasmon resonance Nanoparticles Chiral molecules Chirality sensing

Elucidating ligand effects in rhodium(Ⅲ)-catalyzed arene-alkene coupling reactions

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Chinese Chemical Letters 2024年第5期35卷 130-134页

作者： Kongchuan Wu dandan lu Jianbin Lin Ting-Bin Wen Wei Hao Kai Tan Hui-Jun Zhang Department of Chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Molecular Recognition and FunctionInstitute of ChemistryChinese Academy of Sciences(CAS)Beijing 100190China

Rhodium(Ⅲ)-catalyzed C-H couplings of arenes with alkenes are among the most powerful methods for C-C bond formation.For these transformations,subtle manipulation of ancillary ligands can lead to dramatic changes in reactivity and selectivity.However,detailed mechanistic studies concerning the ligand effects are rare.In this study,we investigated the origin of ligand-controlled product-selectivity in rhodium(Ⅲ)-catalyzed C-H couplings of arenes with alkenes,using a series of well-defined[CpXRhⅢ]complexes that feature electronically or sterically distinct Cp^(X)(Cp(η^(5)-C_(5)H_(5)),Cp^(CF3)(η^(5)-C_(5)Me_(4)CF_(3))and Cp^(∗)(η^(5)-C_(5)Me_(5)))ligands.A combination of experimental and theoretical investigations showed that(i)rhodium hydride species containing the electron rich Cp^(∗)ligand can undergo reinsertion of the alkene,thereby allowing rhodium-walking,(ii)rhodium hydride species involving the electron-deficient Cp or Cp^(CF3) ligands prefer reductive elimination rather than alkene insertion.These findings offer valuable insights on future rational catalyst design for selective arene-alkene cross coupling reactions.

关键词： Organometallics Transition metal catalysis Arene-alkene coupling β-H elimination Rhodium hydride

Major Diseases and Pests of Blueberry in Guizhou Province and Progress in Their Prevention and Control

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Plant Diseases and Pests 2024年第3期15卷 1-4,7页

作者： Yanling REN Shoumei WAN Tao WANG Min ZHANG Lidan MA Zhi LI Youwen TIAN Haibin FU Xingning WANG Jing PENG Lingling XIAO dandan lu Jinyu ZHAO Guizhou Institute of Light Industry Gui an 550025China Shenyang Agricultural University Shenyang 110866China Dandong Customs Comprehensive Technical Service Center Dandong 118000China Guiyang Customs Comprehensive Technology Center Guiyang 550002China Shenyang Customs Technology Center Shenyang 110866China

As the blueberry industry continues to evolve,the effective control of its diseases and pests has become an essential component of local agricultural development.This paper provides a comprehensive overview of the principal types of blueberry diseases and pests in Guizhou Province,along with the corresponding control measures,in order to serve as a valuable reference for blueberry growers.

关键词： Blueberries Diseases and pests Prevention and control Guizhou Province

Geographically varying relationships between population flows from Wuhan and COVID-19 cases in Chinese cities

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Geo-Spatial Information Science 2022年第2期25卷 121-131页

作者： Gang Xu Wenwu Wang dandan lu Binbin lu Kun Qin Limin Jiao School of Remote Sensing and Information Engineering Wuhan UniversityWuhanChina Wuhan Geomatics Institute WuhanChina School of Resource and Environmental Sciences Wuhan UniversityWuhanChina

The COVID-19 epidemic widely spread across China from Wuhan,Hubei Province,because of huge migration before 2020 Chinese New Year.Previous studies demonstrated that population outflows from Wuhan determined COVID-19 cases in other cities but neglected spatial hetero-geneities of their relationships.Here,we use Geographically Weighted Regression(GWR)model to investigate the spatially varying influences of outflows from Wuhan.Overall,the GWR model increases explanatory ability of outflows from Wuhan by 20%,with the adjusted R2 increasing from~0.6 of Ordinary Least Squares(OLS)models to~0.8 of GWR models.The coefficient between logarithmic of outflows from Wuhan and COVID-19 cases in other cities is generally less than 1.The sub-linear scaling relationship indicates the increasing returns of outflows was restrained,proving the epidemic was efficiently controlled outside Hubei at the beginning without obvious local transmissions.Coefficients in GWR models vary in cities.Not only cities around Wuhan but also cities having close connections with Wuhan experienced higher coefficients,showing a higher vulnerability of these cities.The secondary or multi-level trans-mission networks deserve to be further explored to fully uncover influences of migrations on the COVID-19 pandemic.

关键词： COVID-19 population flow scaling law Geographically Weighted Regression(GWR) spatial heterogeneity

Regulatory dynamics of the higher-plant PSI-LHCI supercomplex during state transitions

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Molecular Plant 2023年第12期16卷 1937-1950页

作者： Jianghao Wu Shuaijiabin Chen Chao Wang Weijun Lin Chao Huang Chengxu Fan Dexian Han dandan lu Xiumei Xu SenFang Sui Lixin Zhang State Key Laboratory of Crop Stress Adaptation and Improvement School of Life SciencesHenan UniversityJinming AvenueKaifeng 475004China School of Life Science Southern University of Science and TechnologyShenzhen 518055China State Key Laboratory of Membrane Biology Beijing Advanced Innovation Center for Structural BiologyBeijing Frontier Research Center for Biological StructureSchool of Life SciencesTsinghua UniversityBeijing 100084China Cryo-EM Center Southern University of Science and TechnologyShenzhen 518055China Photosynthesis Research Center Key Laboratory of PhotobiologyInsttute of BotanyChinese Academy of SciencesBejing 100093China

State transition is a fundamental light acclimation mechanism of photosynthetic organisms in response to the environmental light conditions.This process rebalances the excitation energy between photosystemI(PSl)and photosystem Il through regulated reversible binding of the light-harvesting complex Il(LHCll)to PSl.However,the structural reorganization of PSI-LHCI,the dynamic binding of LHCll,and the regulatory mechanisms underlying state transitions are less understood in higher plants.In this study,using cryoelectron microscopy we resolved the structures of PSI-LHCI in both state 1(PSI-LHCI-ST1)and state 2(PSILHCI-LHCll-ST2)from Arabidopsis thaliana.Combined genetic and functional analyses revealed novel contacts between Lhcb1 and PsaK that further enhanced the binding of the LHCll trimer to the PSI core with the known interactions between phosphorylated Lhcb2 and the PsaL/PsaH/PsaO subunits.Specifically,PsaO was absent in the PSI-LHCI-ST1 supercomplex but present in the PSI-LHCI-LHCIl-ST2 supercomplex,in which the PsaL/PsaK/PsaA subunits undergo several conformational changes to strengthen the binding of PsaO in ST2.Furthermore,the PSI-LHCI module adopts a more compact configuration with shorter Mg-to-Mg distances between the chlorophylls,which may enhance the energy transfer efficiency from the peripheral antenna to the PSl core in ST2.Collectively,our work provides novel structural and functional insights into the mechanisms of light acclimation during state transitions in higher plants.

关键词： state transitions dynamic conformation photosystem l regulatory mechanism Arabidopsis thaliana

Precision Methylome and In Vivo Methylation Kinetics Characterization of Klebsiella pneumoniae

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Genomics, Proteomics & Bioinformatics 2022年第2期20卷 418-434页

作者： Jing Fu Ju Zhang Li Yang Nan Ding Liya Yue Xiangli Zhang dandan lu Xinmiao Jia Cuidan Li Chongye Guo Zhe Yin Xiaoyuan Jiang Yongliang Zhao Fei Chen Dongsheng Zhou CAS Key Laboratory of Genome Sciences and Information Beijing Institute of GenomicsChinese Academy of Sciences and China National Center for BioinformationBeijing 100101China Department of Oncology Henan Provincial People’s HospitalPeople’s Hospital of Zhengzhou UniversityPeople’s Hospital of Henan UniversityZhengzhou 450001China University of Chinese Academy of Sciences Beijing 100049China Department of Medical Research Center Peking Union Medical College HospitalPeking Union Medical College&Chinese Academy of Medical SciencesBeijing 100730China State Key Laboratory of Pathogen and Biosecurity Beijing Institute of Microbiology and EpidemiologyBeijing 100071China CAS Key Laboratory of Genomic and Precision Medicine Beijing Institute of GenomicsChinese Academy of Sciences and China National Center for BioinformationBeijing 100101China

Klebsiella pneumoniae(K.pneumoniae)is an important pathogen that can cause severe hospital-and community-acquired infections.To systematically investigate its methylation features,we determined the whole-genome sequences of 14 K.pneumoniae strains covering varying serotypes,multilocus sequence types,clonal groups,viscosity/virulence,and drug resistance.Their methylomes were further characterized using Pacific Biosciences single-molecule real-time and bisulfite technologies.We identified 15 methylation motifs[13 N6-methyladenine(6mA)and two 5-methylcytosine(5mC)motifs],among which eight were novel.Their corresponding DNA methyltransferases were also validated.Additionally,we analyzed the genomic distribution of GATC and CCWGG methylation motifs shared by all strains,and identified differential distribution patterns of some hemi-/un-methylated GATC motifs,which tend to be located within intergenic regions(IGRs).Specifically,we characterized the in vivo methylation kinetics at single-base resolution on a genome-wide scale by simulating the dynamic processes of replication-mediated passive demethylation and MTase-catalyzed re-methylation.The slow methylation of the GATC motifs in the replication origin(oriC)regions and IGRs implicates the epigenetic regulation of replication initiation and transcription.Our findings illustrate the first comprehensive dynamic methylome map of K.pneumoniae at single-base resolution,and provide a useful reference to better understand epigenetic regulation in this and other bacterial species.

关键词： DNA methylation Epigenomics 6mA 5mC Epigenetic regulation

Phase separation in plants:New insights into cellular compartmentalization

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Journal of Integrative Plant Biology 2021年第11期63卷 1835-1855页

作者： Xiumei Xu Canhui Zheng dandan lu Chun‐Peng Song Lixin Zhang State Key Laboratory of Crop Stress Adaptation and Improvement School of Life SciencesHenan UniversityKaifeng 475004China

A fundamental challenge for cells is how to coordinate various biochemical reactions in space and time. To achieve spatiotemporal control, cells have developed organelles that are surrounded by lipid bilayer membranes. Further, membraneless compartmentalization, a process induced by dynamic physical association of biomolecules through phase transition offers another efficient mechanism for intracellular organization. While our understanding of phase separation was predominantly dependent on yeast and animal models, recent findings have provided compelling evidence for emerging roles of phase separation in plants. In this review, we first provide an overview of the current knowledge of phase separation, including its definition, biophysical principles, molecular features and regulatory mechanisms. Then we summarize plant-specific phase separation phenomena and describe their functions in plant biological processes in great detail. Moreover, we propose that phase separation is an evolutionarily conserved and efficient mechanism for cellular compartmentalization which allows for distinct metabolic processes and signaling pathways, and is especially beneficial for the sessile lifestyle of plants to quickly and efficiently respond to the changing environment.

关键词： cellular compartmentalization changing environment condensates liquid droplets phase separation

The quantitative proteome atlas of a model cyanobacterium

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Journal of Genetics and Genomics 2022年第2期49卷 96-108页

作者： Jinlong Wang Xiahe Huang Haitao Ge Yan Wang Weiyang Chen Limin Zheng Chengcheng Huang Haomeng Yang Lingyu Li Na Sui Yu Wang Yuanya Zhang dandan lu Longfa Fang Wu Xu Yuqiang Jiang Fang Huang Yingchun Wang State Key Laboratory of Molecular Developmental Biology The Innovative Academy of Seed DesignInstitute of Genetics and Developmental BiologyChinese Academy of SciencesBeijing 100101China School of Life Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhouZhejiang 310024China University of Chinese Academy of Sciences Beijing 100049China Key Laboratory of Photobiology Institute of BotanyChinese Academy of SciencesBejing 100093China Shandong Provincial Key Laboratory of Plant Stress College of Life ScienceShandong Normal UniversityJinanShandong 250014China State Key Laboratory of Crop Stress Adaptation and Improvement School of Life SciencesHenan UniversityKaifengHenan 475004China Department of Chemistry University of Louisiana at LafayetteLafayetteLA 70504USA

Cyanobacteria are a group of oxygenic photosynthetic bacteria with great potentials in biotechnological applications and advantages as models for photosynthesis research. The subcellular localizations of the majority of proteins in any cyanobacteria remain undetermined, representing a major challenge in using cyanobacteria for both basic and industrial researches. Here, using label-free quantitative proteomics, we map 2027 proteins of Synechocystis sp. PCC6803, a model cyanobacterium, to different subcellular compartments and generate a proteome atlas with such information. The atlas leads to numerous unexpected but important findings, including the predominant localization of the histidine kinases Hik33 and Hik27 on the thylakoid but not the plasma membrane. Such information completely changes the concept regarding how the two kinases are activated. Together, the atlas provides subcellular localization information for nearly 60% proteome of a model cyanobacterium, and will serve as an important resource for the cyanobacterial research community.

关键词： Proteome atlas Cyanobacteria Proteomics Membranes Synechocystis

Comprehensive Investigations of the Cl+CH_(3)OH→HCl+CH_(3)O/CH_(2)OH Reaction:Validation of Experiment and Dynamic Insights

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CCS Chemistry 2020年第5期2卷 882-894页

作者： dandan lu Jun Li Hua Guo School of Chemistry and Chemical Engineering&Chongqing Key Laboratory of Theoretical and Computational Chemistry Chongqing UniversityChongqing 401331 Department of Chemistry and Chemical Biology University of New MexicoAlbuquerqueNew Mexico 87131

Cl+CH_(3)OH→HCl+CH_(3)O/CH_(2)OH is a prototypical multiple-channel reaction.Experimentally,ample dynamical and kinetic information is available,but there are still many uncertainties concerning the reaction mechanism.Theoretical investigations are rare due to the absence of a potential energy surface(PES),which has greatly hindered our understanding of the reaction dynamics.Using a machine-learning approach,an accurate full-dimensional PES for the title reaction based on tens of thousands of high-level ab initio data is reported.Comprehensive dynamical calculations were performed on the PES using quasi-classical trajectories,and the results provide insights into the reaction kinetics and dynamics.The calculated non-Arrhenius rate coefficients are consistent with the experimental data,attributable to a complex-forming mechanism at low temperatures.At high energies,the reaction is dominated by a direct mechanism,which results in dominant forward scattering via a stripping mechanism augmented by less prominent sideways and backward scattering via a rebound mechanism.At collision energies of 5.6 and 8.7 kcal/mol,the measured product translational energy and ro-vibrational state distributions of HCl are well reproduced.In addition,mode specificity is revealed and rationalized by the sudden vector projection model.This work sheds valuable light on the microscopic mechanism and dynamics of this prototypical multichannel reaction.

关键词： potential energy surface transition state multichannel reaction mode specificity mechanism reaction dynamics kinetics