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New approach for chiral separation: from polysaccharide-based materials to chirality-responsive polymers

Science China Chemistry 2014年第11期57卷 1492-1506页

作者： DING Peng CHANG BaiSong QING GuangYan sun taolei State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology School of Chemistry Chemical Engineering and Life Science Wuhan University of Technology

Chiral separation that is closely related to daily life is a meaningful research. Polysaccharide-(e.g., cellulose, amylose derivatives) based chiral packing materials afford powerful chiral stationary phases(CSPs) toward a broad range of racemic compounds. However, considering the explosive growth of specific chiral drugs, the separation efficiencies of these CSPs need further improvement, which calls for new approaches and strategies. Smart polymers can change their physical or chemical properties dynamically and reversibly according to the external stimuli(e.g., thermo-, pH, solvent, ion, light, critical parameters for chromatographic separation) exerted on them, subsequently resulting in tunable changes in the macroscopic properties of materials. In addition to their excellent controllability, the introduction of chiral characteristics into the backbones or side-chains of smart polymers provides a promising route to realize reversibly conformational transition in response to the chiral analytes. This dramatic transition may significantly improve the performance of materials in chiral separation through modulating the enantioselective interactions between materials and analytes. With the help of chirality-responsive polymers, intelligent and switchable CSPs could be developed and applied in column-liquid chromatography. In these systems, the elution order or enantioselectivity of chiral drugs can be precisely modulated, which will help to solve many challenging problems that involve complicated enantiomers. In this paper we introduce some typical examples of smart polymers that serve as the basis for a discussion of emerging developments of CPSs, and then briefly outline the recent CSPs based on natural and certain synthetic polymers.

关键词： chiral separation chiral stationary phases(CSPs) enantioseparation HPLC smart polymer

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Chiral polymer-based biointerface materials

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Science China Chemistry 2014年第4期57卷 540-551页

作者： LI MinMin QING GuangYan ZHANG MingXi sun taolei State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology

Chirality is a unique phenomenon in nature. Chiral interactions play an important role in biological and physiological process- es, which provides much inspiration for scientists to develop cbiral materials. As a breakthrough from traditional materials, bi- ointerface materials based on chiral polymers have attracted increasing interest over the past few years. Such materials ele- gantly combine the advantages of chiral surfaces and traditional polymers, and provide a novel solution not only for the inves- tigation of chiral interaction mechanisms but also for the design of biomaterials with diverse applications, such as in tissue en- gineering and biocompatible materials, bioregulation, chiral separation and chiral sensors. Herein, we summarize recent ad- vances in the study of chiral effects and applications of chiral polymer-based biointerface materials, and also present some challenges and perspectives.

关键词： chirality polymer chiral interaction biointerface materials chiral effects applications

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Au23（CR）14 nanocluster restores fibril Aβ's unfolded state with abolished cytotoxicity and dissolves endogenous Aβplaques

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National Science Review 2020年第4期7卷 763-774页

作者： Wenkang Zhang Guanbin Gao Zhongjie Ma Zhuoying Luo Meng He taolei sun State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology School of Chemistry Chemical Engineering and Life Science Wuhan University of Technology

The misfolding of amyloid-β（Aβ） peptides from the natural unfolded state to β-sheet structure is a critical step, leading to abnormal fibrillation and formation of endogenous Aβ plaques in Alzheimer's disease（AD）. Previous studies have reported inhibition of Aβ fibrillation or disassembly of exogenous Aβ fibrils in vitro. However, soluble Aβ oligomers have been reported with increased cytotoxicity; this might partly explain why current clinical trials targeting disassembly of Aβ fibrils by anti-Aβ antibodies have failed so *** we show that Au23（CR）14(a new Au nanocluster modified by Cys-Arg（CR） dipeptide) is able to completely dissolve exogenous mature Aβ fibrils into monomers and restore the natural unfolded state of Aβ peptides from misfolded β-sheets. Furthermore, the cytotoxicity of Aβ40fibrils when dissolved by Au23（CR）14is fully abolished. More importantly, Au23（CR）14is able to completely dissolve endogenous Aβ plaques in brain slices from transgenic AD model mice. In addition, Au23（CR）14has good biocompatibility and infiltration ability across the blood–brain barrier. Taken together, this work presents a promising therapeutics candidate for AD treatment, and manifests the potential of nanotechnological approaches in the development of nanomedicines.

关键词： gold nanoclusters Alzheimer’s disease restores fibril Aβ’s unfolded state abolished cytotoxicity dissolves endogenous Aβ plaques

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Interfacial charge effects of supported-metal-cluster heterostructures on azo hydrogenation catalyzation

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Nano Research 2024年第5期17卷 3853-3862页

作者： Zhenhua Gu Jingli Zhang Zijun Zhang Qingxue Mu Liangchong Yu taolei sun Lei Shen Guanbin Gao State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Hubei Key Laboratory of Nanomedicine for Neurodegenerative Diseases School of ChemistryChemical Engineering and Life ScienceWuhan University of TechnologyWuhan 430070China

The impact of interfacial charge on catalytic performance of supported-metal-cluster(SMC)heterostructures remains unclear,hindering efforts to develop high-performance SMC *** we systematically investigated interfacial charge effects of SMCs using a model system of graphene-supported gold-nanoclusters(AuNCs/rGO)for azo *** types of SMCs with different interfacial charges were synthesized by anchoring electropositive 2-aminoethanethiol(CSH),amphoteric cysteine(Cys),and electronegative 3-mercaptopropionic-acid(MPA)onto AuNCs/rGO,*** three SMCs exhibited high and selective catalytic activity to azo-hydrogenation in four representative azo *** catalytic activity of Cys@AuNCs/rGO was lower than that of CSH@AuNCs/rGO but higher than that of MPA@AuNCs/***,the cyclic stability of Cys@AuNCs/rGO was inferior to that of both CSH@AuNCs/rGO and MPA@AuNCs/*** mechanistic studies revealed that amino ligands modified CSH@AuNCs and Cys@AuNCs agglomerated into large-size gold nanoparticles on rGO surface during catalytic reaction under NaBH_(4) action,leading to reduced efficiency and cyclic ***,non-amino ligand modified MPA@AuNCs only partially detached from rGO surface without agglomeration,resulting in better cyclic *** of amino groups in ligands such as modifying-NH_(3)^(+)group in Cys into imine to form N-isobutyryl-L-cysteine(NIBC)substantially improved the cyclic stability while maintaining the high activity in the NIBC@AuNCs/rGO catalyst *** work provides an approach for developing a highly-active and stable SMC heterostructure catalyst via manipulating interfacial charges in SMC.

关键词： interfacial charge effect supported-metal-cluster catalyst azo hydrogenation graphene supported gold nanoclusters

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Chiral effect on Aβ fibrillation from molecular-scale to nanoscale

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Nano Research 2022年第7期15卷 6721-6729页

作者： Guanbin Gao Guowei Zhu Liangchong Yu Zijun Zhang Ting Zhang Xinglin Liu Cheng Zhang Lin Zhou taolei sun State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China School of Chemistry Chemical Engineering and Life ScienceWuhan University of TechnologyWuhan 430070China

β-Amyloid(Aβ)peptide fibrillation,one of the characteristic hallmarks of Alzheimer’s disease,is determined by many interfacial physical-chemical factors,e.g.,charge,hydrophobicity,*** extensive research,chiral effect in different-scales on the fibrillation process of Aβremains ***,molecular-scale,sub-nanoscale,and nanoscale chiral-structures were constructed to investigate their chiral effect on the fibrillation of Aβ_(40) *** structures from molecular-scale to nanoscale were obtained from the different periods of the chemosynthesis process of chiral ZnS quantum-dots(QDs),confirmed by real-time monitoring of circular dichroism *** molecular-scale,both L-penicillamine(L-P)and D-P ligands accelerated the fibrillation of Aβ_(40),and the speed-up effect of D-P was slightly stronger than *** sub-nanoscale,both two chiral Zncomplexes(L-Zn and D-Zn)induced the agglomeration of Aβ_(40) without chirality *** nanoscale,both L-ZnS and DZnS QDs inhibited the fibrillation of Aβ_(40),and the inhibition effect of L-ZnS was notably better than that of ***-situ kinetics experiments of Aβ_(40) co-incubated with two chiral QDs demonstrated that L-ZnS completely prevents the misfolding of Aβ_(40) from unfolded toβ-sheet,while D-ZnS cannot achieve *** site-replacement experiments and simulation results revealed the underlying molecular mechanisms of the different inhibition efficiency of chiral ZnS QDs on Aβ_(40) fibrillation,which mainly attribute to the stereoselectivity interaction between the chiral ligands of ZnS QDs and electro-positive amino acid residues(R5,K16,and K28)of Aβ_(40).This work offers a microscopic insight of chiral effect on Aβfibrillation exerted by structures in different-scales,and provides a guidance in precise regulation of protein fibrillation via manipulating chiral structures in different-scales.

关键词： chirality molecular-scale sub-nanoscale nanoscale Aβ_(40) fibrillation

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Binding between Prion Protein and Aβ Oligomers Contributes to the Pathogenesis of Alzheimer’s Disease

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Virologica Sinica 2019年第5期34卷 475-488页

作者： Chang Kong Hao Xie Zhenxing Gao Ming Shao Huan Li Run Shi Lili Cai Shanshan Gao taolei sun Chaoyang Li School of Chemistry Chemical Engineering and Life SciencesWuhan University of TechnologyWuhan 430070China State Key Laboratory of Virology Wuhan Institute of VirologyChinese Academy of SciencesWuhan 430071China Affiliated Cancer Hospital Institute of Guangzhou Medical UniversityGuangzhou 510095China

A plethora of evidence suggests that protein misfolding and aggregation are underlying mechanisms of various neurodegenerative diseases,such as prion diseases and Alzheimer's disease(AD).Like prion diseases,AD has been considered as an infectious disease in the past decades as it shows strain specificity and transmission *** it remains elusive how protein aggregation leads to AD,it is becoming clear that cellular prion protein(PrP^c)plays an important role in AD ***,we briefly reviewed AD pathogenesis and focused on recent progresses how PrP^c contributed to AD *** addition,we proposed a potential mechanism to explain why infectious agents,such as viruses,conduce AD *** infections cause AD deposition and upregulation of PrP^c,which lead to high affinity binding between AD oligomers and PrP^*** interaction between PrP^c and AP oligomers in turn activates the Fyn signaling cascade,resulting in neuron death in the central nervous system(CNS).Thus,silencing PrP^c expression may turn out be an effective treatment for PrP^c dependent AD.

关键词： Alzheimer’s disease(AD) Amyloid-βprotein Neurodegenerative disease Cellular prion protein(PrP^c)

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Endogenous formaldehyde responsive fluorescent probe for bioimaging

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Nano Research 2023年第12期16卷 13029-13041页

作者： Ning-Bo Yi Xing-Jie Hu Fei Wang Si-Yi Chen Xiao-Xue Xu Xin Li Hao Wang taolei sun Zeng-Ying Qiao Dong-Bing Cheng Hubei Key Laboratory of Nanomedicine for Neurodegenerative Diseases School of ChemistryChemical Engineering&Life ScienceWuhan University of TechnologyWuhan 430070China CAS Center for Excellence in Nanoscience Laboratory for Biological Effects of Nanomaterials and Nanosafety National Center for Nanoscience and Technology(NCNST)Beijing 100190China Department of Biology and the School of Natural Sciences Went Worth CollegeUniversity of YorkHeslingtonYorkYO105DDUK

Formaldehyde(FA),as the simplest endogenous carbonyl molecule,participates in many biosynthesis and metabolism in living organisms,such as nucleotides and adenosine triphosphate(ATP).FA concentrations are sub-millimolar in the normal healthy body,but can rise significantly in a number of disease *** a result,detecting endogenous FA is critical for illness diagnosis and rehabilitation therapy *** studies have focused on the FA-responsive turn-on fluorescence probe,which has huge promise in the detection and visualization of FA in living cells and organisms,as well as exceptional use in disease diagnosis and therapeutic *** review summarizes the fluorescence luminescence mechanism and design concepts of FA fluorescent probes,as well as their recent applications in bioimaging and illness ***,this article indicates the present dilemma of FA-responsive fluorescent probe,including selectivity,specificity,and detection mode,which may provide references for the development of FA-responsive fluorescent probes.

关键词： endogenous formaldehyde fluorescent probe tumor cell bioimaging

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β-HgS量子点的制备、性质及应用

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化学进展 2017年第7期29卷 776-784页

作者：刘康高冠斌孙涛垒武汉理工大学材料复合新技术国家重点实验室武汉430070

β-HgS量子点因其具有可调谐的可见-近红外荧光和带间荧光而在光转换和荧光成像等多个领域有着广阔的应用前景。本文综述了β-HgS量子点的制备、性质及应用,重点梳理了β-HgS量子点在有机相和水相中的两大类共计五种制备方法,阐述了其... 详细信息

β-HgS量子点因其具有可调谐的可见-近红外荧光和带间荧光而在光转换和荧光成像等多个领域有着广阔的应用前景。本文综述了β-HgS量子点的制备、性质及应用,重点梳理了β-HgS量子点在有机相和水相中的两大类共计五种制备方法,阐述了其不同于块状β-HgS的独特性质,总结了其在离子探测、细胞成像、活体成像、光转换器和荧光油墨等领域的最新应用。最后针对制约β-HgS量子点应用的主要问题(如应用于光转换器件中的转换效率和荧光量子产率不高、应用于生物荧光成像中的特异性识别能力不足和生物相容性较差等),提出了我们的解决方案:一方面,将β-HgS量子点自组装形成特定的纳米结构,以期提高其光转换效率和荧光量子产率;另一方面,通过将手性生物分子引入到β-HgS量子点表面来制备手性β-HgS量子点,以期增强其在体内和体外荧光成像中的特异性识别能力和改善其生物相容性。本文将为β-HgS量子点的发展提供新的思路。

关键词： β-HgS量子点制备性质应用

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基于透明质酸的缺氧响应型胶束的制备及性能研究

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化学学报 2018年第1期76卷 35-42页

作者：张蓓常柏松孙涛垒武汉理工大学化学化工与生命科学学院武汉430070 武汉理工大学材料复合新技术国家重点实验室武汉430070

以透明质酸(HA)及硝基咪唑(NI)衍生物为原料,通过酰胺反应合成了一种两亲性接枝聚合物(HA-NI).该聚合物具有缺氧响应性和肿瘤靶向性.利用傅里叶红外光谱(FT-IR)和核磁共振(NMR)对接枝聚合物的结构进行了表征,同时基于1H NMR计算出接枝... 详细信息

以透明质酸(HA)及硝基咪唑(NI)衍生物为原料,通过酰胺反应合成了一种两亲性接枝聚合物(HA-NI).该聚合物具有缺氧响应性和肿瘤靶向性.利用傅里叶红外光谱(FT-IR)和核磁共振(NMR)对接枝聚合物的结构进行了表征,同时基于1H NMR计算出接枝聚合物中NI的取代度.HA-NI在水中自组装形成胶束,利用动态光散射仪(DLS)表征胶束大小并对胶束的稳定性进行了研究,利用原子力显微镜(AFM)和透射电镜(TEM)观察胶束形貌.载药胶束的载药率(DL)和包封率(EE)通过紫外-可见吸收光谱(UV)测试并计算得到.胶束的缺氧响应性利用DLS、AFM、TEM、UV等探究.实验证明,该聚合物胶束具有缺氧响应性并对药物表现出良好的控制释放能力,在常氧环境下,胶束稳定存在;而在缺氧环境下,胶束散开,药物快速且完全地释放.

关键词：药物传输体系缺氧响应透明质酸硝基咪唑胶束

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Ag_(2)Se@Ag_(2)S核壳量子点的室温合成及其近红外荧光性能优化

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化学学报 2023年第7期81卷 763-770页

作者：郑文山高冠斌邓浩孙涛垒武汉理工大学材料复合新技术国家重点实验室武汉430070 武汉理工大学化学化工与生命科学学院神经退行性疾病纳米医药湖北省重点实验室武汉430070

在Ag_(2)Se量子点表面生长宽禁带无机壳层以消除表面缺陷是提高其光致发光性能的有效方法.与Ag_(2)Se相比,Ag_(2)S带隙更宽,晶格常数相似,是Ag_(2)Se量子点的理想壳层.然而,室温下精确制备Ag_(2)Se@Ag_(2)S核壳量子点仍然是一个挑战.分... 详细信息

在Ag_(2)Se量子点表面生长宽禁带无机壳层以消除表面缺陷是提高其光致发光性能的有效方法.与Ag_(2)Se相比,Ag_(2)S带隙更宽,晶格常数相似,是Ag_(2)Se量子点的理想壳层.然而,室温下精确制备Ag_(2)Se@Ag_(2)S核壳量子点仍然是一个挑战.分别采用胶体原子层沉积(c-ALD)法和一锅水相法在室温下合成了油溶性和水溶性的Ag_(2)Se@Ag_(2)S核壳量子点,并通过调控配体链长优化了水溶性Ag_(2)Se@Ag_(2)S核壳量子点近红外荧光性能.在c-ALD法中,以1-十二硫醇(DDT)包裹的Ag_(2)Se量子点作为种子,以油胺(OAM)配位的Ag(OAM-Ag)和Na2S作为壳层前驱体,制备的油溶性Ag_(2)Se@Ag_(2)S核壳结构量子点暂无荧光发射,随后尝试通过高温退火但仍无法恢复其荧光发射能力.接着,在一锅水相法中,以巯基羧酸(HS-(CH2)x-COOH)配位的水溶性Ag_(2)Se量子点为种子,巯基羧酸配位的Ag+和Na2S作为壳层前驱体,成功制备出在1270 nm处具有近红外荧光增强的水溶性Ag_(2)Se@Ag_(2)S核壳量子点.通过改变直链配体巯基羧酸的链长度(x=2, 5, 10, 13),发现以中等链长(x=10)的11-巯基十一酸(MUA)为配体的水溶性Ag_(2)Se@Ag_(2)S核壳量子点具有最强的荧光发射.本文为Ag_(2)Se@Ag_(2)S核壳量子点制备提供了参考.

关键词： Ag_(2)Se@Ag_(2)S 核壳量子点室温合成近红外荧光配体优化

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