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Science China Chemistry 2024年第10期67卷 3482-3492页

作者： Weilong Ma Xinyi Li Aiyou Hao pengyao xing School of Chemistry and Chemical Engineering Shandong UniversityJinan 250100China

Unveiling the role of weak non-covalent forces in chiral self-assembly is pivotal in the design and fabrication of functional chiroptical *** nature of arene-perfluoroarene(AP)force is the electrostatic attraction betweenπ-hole andπplanes of perfluoroarenes and polyaromatic hydrocarbons(PAHs),which is emerging in constructing supramolecular motifs and coassembled optical *** this work,we reveal the potential of AP forces in building diversified levels of chiral coassemblies adaptive to the geometries of *** naphthalene-F8was covalently conjugated with a chiral amine,which folded into a semi-rectangular geometry via two intramolecular F···H *** of naphthalene,anthracene,pyrene,carbazole,perylene and benzoperylene were introduced to afford coassemblies in the crystalline state.X-ray structures suggest the formation of supramolecular boxes that encapsulate the PAHs with a 2:1 stoichiometric ratio,as well as the formation of consecutive layered ladders with a 1:1 stoichiometric *** preference is adaptive to the geometries of PAHs,and experimental and computational results evidenced the ladder structures possess strong binding *** this top,the selective chiral recognition in the mixtures of PAHs was realized,which shows promising applications in the separation of PAHs and rational design of crystalline chiroptical materials.

关键词： arene-perfluoroarene force coassembly supramolecular chirality selectivity

Chiroluminophores based on non-conjugated benzenes

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Science China Chemistry 2023年第7期66卷 2130-2140页

作者： Yiping Liu Aiyou Hao pengyao xing School of Chemistry and Chemical Engineering Shandong UniversityJinan 250100China

Point-chiral groups as pendants conjugated to the aromatic luminophore generate weak chiroptical signals without self-assembly,showing the dependence on the flexibility of tethers,which hinders the development of point-chiral molecular materials with chiroptical properties such as the circularly polarized luminescence(CPL).Herein we introduce the molecular chiroptical materials based on the point chirality on a single benzene luminophore *** were stepwise conjugated to single benzene luminophores to boost the steric hindrance and tension,whereby the chirality transfer efficiency from point-chiral substituents to luminophores was *** intramolecular CH-πinteractions anchor the whole asymmetric geometry with ultra-high rotation energy barriers and excellent *** g-factors of circular dichroism and CPL spectra up to 10^(-3)order of magnitude were realized in solutions,which are comparable to the inherent-chiral luminophores such as helicene and binaphthyl *** acridine-appended single benzene system shows the emergence of thermally activated delayed fluorescence(TADF),which extends the potentials of the single benzene chiral system in the TADF-based chiroptical devices.

关键词： point chirality single-benzene based luminophores chirality transfer circularly polarized luminescence thermally activated delayed fluorescence

Helical secondary structures and supramolecular tilted chirality in N-terminal aryl amino acids with diversified optical activities

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Chinese Chemical Letters 2021年第4期32卷 1390-1396页

作者： Zhuoer Wang Aiyou Hao pengyao xing School of Chemistry and Chemical Engineering Shandong UniversityJi'nan 250100China

Helix structures at atomic/molecular level have not been found in self-assembled peptide seque nce with less than three ***β-sheet supramolecular secondary structures have been discovered in solidstate amino acids,we here report the conjugation of simple N-terminal aryl protecting group could give rise to helical supramolecular secondary structures in solid-state,which determines the optical activities of the adjacent aryl *** carboxylic acid-involved asymmetric H-bonds in N-te rminal aryl amino acids induce the emergence of super-helical structures of amino acid residues and aryl *** most cases,supramolecular tilted chirality of aryl groups is opposite to that of amino acid sequences,of which handedness and helical pitch are determined by the H-bond *** correlation between supramolecular tilted chirality of aryl segments and their chiroptical activities is firstly unveiled,which was verified by the computational results based on density functional *** aryl amino acids self-assembled by nanoprecipitation method via crystallization induced self-assembly into rigid one-dimensional microstructures with ultra-high Young's *** study reveals the generic existence of chiral supramolecular structure s in aggregated amino acid derivatives and gives an in-depth investigation into the structural-property relationships,which could guide the rational design and screening of chiroptical supramolecular materials.

关键词： Amino acids Self-assembly Chirality Chiroptical properties H-bonds

Fmoc-protected amino acids as luminescent and circularly polarized luminescence materials based on charge transfer interaction

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Chinese Chemical Letters 2022年第11期33卷 4918-4923页

作者： Yiran Xia Aiyou Hao pengyao xing Key Laboratory of Colloid and Interface Chemistry of Ministry of Education and School of Chemistry and Chemical Engineering Shandong UniversityJi'nan 250100China

Fluorenylmethyloxycarbonyl(Fmoc)-protected amino acids are effective building blocks in self-assembled architectures at hierarchical levels,which however show limited luminescent properties and chiroptical *** we introduce a charge-transfer strategy to build two-component luminescent materials with emerged circularly polarized luminescence properties.A library of Fmoc-amino acids was built,which selectively form charge-transfer complexes with the electron-deficient *** in amorphous polymer matrix or physical grinding could trigger the charge-transfer luminescence with adjusted wavelengths in a general manner.X-ray diffraction results suggest the multiple binding modes between donor and ***,the solution-processed coassembly could selectively exhibit circularly polarized luminescence with high dissymmetry *** work illustrates a noncovalent charge-transfer strategy to construct luminescent and chiroptical organic composites based on the easy-accessible and economic chiral N-terminal aromatic amino acids.

关键词： Fmoc-amino acids Charge-transfer interaction Supramolecular chirality Multiple component coassembly

Chiroptical coassemblies between organic carboxylic acids and amino acid derivatives with C_(3)-symmetry

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Chinese Chemical Letters 2023年第6期34卷 319-322页

作者： Yiran Xia Aiyou Hao pengyao xing School of Chemistry and Chemical Engineering Shandong UniversityJi’nan 250100China

Benzimidazole amino acid derivatives behave as supramolecular hosts to include organic acids via complementary hydrogen bonding whereby supramolecular chirality and chiroptical properties could be *** acids enhanced the chiral assembly that showed tunable circularly polarized luminescence with high dissymmetry g-factors at 10^(-2)grade.

关键词： Supramolecular chirality Organic carboxylic acid Amino acid Coassembly Chiroptical property

Distorted aryl homochirality controlled byβ-sheet folding

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Chinese Chemical Letters 2023年第11期34卷 147-152页

作者： Yunying Xu Aiyou Hao pengyao xing School of Chemistry and Chemical Engineering Shandong UniversityJi’nan 250100China

Distortion of planar aromatics occurs in the fused rings conjugated with bulky substituents,which generates racemic enantiomers with high transformation energy ***,direct synthesis of homochiral distorted aryl compounds is a very challenging ***,we presented a molecular folding strategy to control distorted aryl *** acids and their derivatives conjugated on the polycyclic aromatic hydrocarbons including benzenes,naphthalenes and triphenylenes,which formed parallelβ-sheet arrays through intramolecular hydrogen *** folding behavior enabled distorted or twisted geometry of aromatics,of which the handedness was associated with the absolute chirality of amino acids.X-ray crystallography,theoretical calculations and circular dichroism spectroscopy verified the distorted homochirality in the solid and solution *** relatively small rotational barrier between the enantiomers made the molecule sensitive to the environment and thus realized the solvent-controlled chiral ***β-sheet folding strategy can be widely used in polycyclic aromatic hydrocarbons with various functions,which provided a promising strategy to control inherent chirality of aromatics with adaptive chiroptical responses.

关键词： Distorted chirality Folding Solvent strategy Chiroptical activity

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多组分手性超分子的构筑及其应用

科学通报 2021年第14期66卷 1666-1677页

作者：成秋鸿郝爱友邢鹏遥山东大学化学与化工学院济南250100

手性与生命现象密切相关,如氨基酸、蛋白质和核酸的手性结构,以及宏观的海螺等.分子模块的不对称性堆积称为超分子手性.对超分子手性的出现、放大、转移以及反转的调控是超分子手性中几个重要的研究方向.超分子手性组装体通常由多种非... 详细信息

手性与生命现象密切相关,如氨基酸、蛋白质和核酸的手性结构,以及宏观的海螺等.分子模块的不对称性堆积称为超分子手性.对超分子手性的出现、放大、转移以及反转的调控是超分子手性中几个重要的研究方向.超分子手性组装体通常由多种非共价相互作用协同驱动形成,是一类具有独特手性微环境的软物质.其中,含两种或两种以上组分的超分子组装体既可能经过协同组装作用也可能发生自分类.其存在多种组装路径,相对于单组分体系复杂得多.因此,与发展更为成熟的单组分体系相比,多组分超分子手性组装体在基础和应用方面的研究都受到了限制.然而,研究多组分中的超分子手性既可以模拟复杂的手性生物体系,也可以加深对自然界中手性起源的理解,从而进一步应用于仿生学和手性材料,具有重要的意义.因此本文主要对多组分手性超分子共组装体系的构建以及可能的应用进行了综述和总结.

关键词：超分子手性多组分自组装手性调控圆偏振发光

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主客体超分子囊泡及其药物载运性能研究

化学进展 2014年第8期26卷 1317-1328页

作者：马明放邢鹏遥李尚洋初晓晓王波郝爱友山东大学化学与化工学院济南250100

伴随着新型主体分子的不断出现,主客体超分子囊泡的研究受到越来越多的关注。环糊精、杯芳烃、葫芦脲和柱芳烃等主体分子均可以和特定结构的客体分子通过主客体识别作用构筑超分子双亲分子,得到的超分子双亲分子可以进一步自组装为主客... 详细信息

伴随着新型主体分子的不断出现,主客体超分子囊泡的研究受到越来越多的关注。环糊精、杯芳烃、葫芦脲和柱芳烃等主体分子均可以和特定结构的客体分子通过主客体识别作用构筑超分子双亲分子,得到的超分子双亲分子可以进一步自组装为主客体超分子囊泡。主客体超分子囊泡是一类具有敏感响应性的囊泡体系,具有制备简单、生物相容性好和易于控制组装等优点。该囊泡体系对外界刺激具有良好的响应性,从而可以实现药物分子的可控运输和释放,使其成为一种性能独特的药物载运系统。本文结合近年来主体分子的发展,首先介绍了环糊精、杯芳烃、葫芦脲和柱芳烃等主客体超分子囊泡的研究进展,然后对该类超分子囊泡的载药途径进行了总结。该囊泡体系不仅可以在囊泡膜层和空腔中载药,还可以在主体分子的空腔中载药。同时,对载药主客体超分子囊泡的不同刺激响应性进行了归纳概括。最后结合该体系现阶段的研究状况,对该类超分子囊泡的发展前景进行了展望。

关键词：主客体识别超分子囊泡主体分子药物载运刺激响应

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基于β-环糊精的有机小分子凝胶

化学进展 2019年第2期31卷 225-235页

作者：马明放栾天翔邢鹏遥李兆楼初晓晓郝爱友济宁医学院新型抗肿瘤药物分子设计与合成实验室&济宁医学院基础医学院济宁272067 胶体与界面化学教育部重点实验室山东大学化学与化工学院济南250100

环糊精是直链淀粉在环糊精葡萄糖基转移酶作用下生成的含有7个D-吡喃葡萄糖单元的环状低聚糖,具有斜截锥形空间立体结构,腔内疏水,腔外亲水。β-环糊精以其低廉的价格、良好的水溶性和生物相容性,在超分子化学领域得到广泛的应用。β-... 详细信息

环糊精是直链淀粉在环糊精葡萄糖基转移酶作用下生成的含有7个D-吡喃葡萄糖单元的环状低聚糖,具有斜截锥形空间立体结构,腔内疏水,腔外亲水。β-环糊精以其低廉的价格、良好的水溶性和生物相容性,在超分子化学领域得到广泛的应用。β-环糊精可用于凝胶的构筑,通常的方法是将β-环糊精接枝到高分子链上,再以得到的高分子链为凝胶因子构筑高分子凝胶。虽然基于β-环糊精的高分子凝胶得到了广泛的关注和研究,但是,直接以β-环糊精为凝胶因子构筑的有机小分子凝胶却鲜有报道。2010年,本课题组首次报道了一种基于β-环糊精和二苯胺的热致有机凝胶。此后,本课题组在β-环糊精有机小分子凝胶领域做了大量的研究工作。本文在实验室研究工作的基础上,首先介绍了β-环糊精有机小分子凝胶的分类和不同因素对凝胶形成的影响,然后深入探讨了β-环糊精有机小分子凝胶的形成机理,系统介绍了β-环糊精有机小分子凝胶的刺激响应性以及在药物载运领域的应用,最后,对β-环糊精有机小分子凝胶的发展前景进行了展望。

关键词： β-环糊精有机小分子凝胶刺激响应药物载运

7075高强铝合金管约束混凝土柱轴压承载力计算

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工业建筑 2020年第11期50卷 162-167页

作者：李翔宇邢国华张蓬瑶张广泰新疆大学建筑工程学院乌鲁木齐830046 长安大学建筑工程学院西安710061

高强铝合金由于具有耐腐蚀、强度高、延性好等优点,在大型基础设施工程中具有十分广阔的应用前景。在对比分析钢管约束混凝土柱轴压承载力常用计算理论的基础上,提出了铝合金管约束混凝土柱承载力计算方法,应用有限元程序ABAQUS对7075... 详细信息

高强铝合金由于具有耐腐蚀、强度高、延性好等优点,在大型基础设施工程中具有十分广阔的应用前景。在对比分析钢管约束混凝土柱轴压承载力常用计算理论的基础上,提出了铝合金管约束混凝土柱承载力计算方法,应用有限元程序ABAQUS对7075高强铝合金管约束混凝土柱的轴压性能进行了数值模拟计算,并将有限元模拟计算结果与理论分析结果进行了对比。研究结果表明:欧洲标准(EC4)没有考虑钢管对混凝土的约束作用,故所得计算承载力值偏于安全;"统一理论"矩形钢管计算式并不适用于铝合金约束混凝土矩形柱;而按DL/T 5085—1999《钢-混凝土组合结构设计规程》和GJB 4142—2000《战时军港抢修早强型组合结构技术规程》所得的铝合金管约束混凝土柱承载力比有限元模拟值仅高出4%左右,计算结果与理论分析吻合较好。最后基于DL/T 5085—1999和GJB 4142—2000,以约束效应系数为参数,提出了铝合金管约束混凝土柱轴压承载力计算方法。

关键词： 7075高强铝合金约束混凝土柱承载力有限元分析