Polyvinyl alcohol(PVA)/laponite(LP)nanocomposite coatings were fabricated via a facile one-step coassembly process.The formed nanocoatings contain a high concentration of LP nanosheets,which can be well aligned along ...Polyvinyl alcohol(PVA)/laponite(LP)nanocomposite coatings were fabricated via a facile one-step coassembly process.The formed nanocoatings contain a high concentration of LP nanosheets,which can be well aligned along the substrate surface during the coassembly process.Due to the highly orientated structure,the flexible nanocoatings exhibit ultra-high transparency and superior mechanical properties,and can also act as excellent gas barriers.Such nanocoatings can be exceptional candidates for a variety of applications,such as food packaging.展开更多
Unveiling the role of weak non-covalent forces in chiral self-assembly is pivotal in the design and fabrication of functional chiroptical materials.The nature of arene-perfluoroarene(AP)force is the electrostatic attr...Unveiling the role of weak non-covalent forces in chiral self-assembly is pivotal in the design and fabrication of functional chiroptical materials.The 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 devices.In this work,we reveal the potential of AP forces in building diversified levels of chiral coassemblies adaptive to the geometries of PAHs.The naphthalene-F8was covalently conjugated with a chiral amine,which folded into a semi-rectangular geometry via two intramolecular F···H bonds.PAHs 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 ratio.The preference is adaptive to the geometries of PAHs,and experimental and computational results evidenced the ladder structures possess strong binding affinity.On 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.展开更多
Benzimidazole amino acid derivatives behave as supramolecular hosts to include organic acids via complementary hydrogen bonding whereby supramolecular chirality and chiroptical properties could be manipulated.Organic ...Benzimidazole amino acid derivatives behave as supramolecular hosts to include organic acids via complementary hydrogen bonding whereby supramolecular chirality and chiroptical properties could be manipulated.Organic acids enhanced the chiral assembly that showed tunable circularly polarized luminescence with high dissymmetry g-factors at 10^(-2)grade.展开更多
Hybrid adsorbents for COcapture were prepared by coassembling laponite（LP） nanosheets and 1-nbutyl-3-methylimidazolium chloride（BMIMCl）. The prepared BMIMCl/LP layered hybrids were systematically characterized. Th...Hybrid adsorbents for COcapture were prepared by coassembling laponite（LP） nanosheets and 1-nbutyl-3-methylimidazolium chloride（BMIMCl）. The prepared BMIMCl/LP layered hybrids were systematically characterized. The interlayer distance of the BMIMCl/LP layered hybrids expanded with an increasing concentration of BMIMCl, indicating that cumulative BMIMCl was intercalated into the LP layers. The efficiency of BMIMCl toward COcapture was significantly enhanced after it was immobilized within LP layers.展开更多
Fluorenylmethyloxycarbonyl(Fmoc)-protected amino acids are effective building blocks in self-assembled architectures at hierarchical levels,which however show limited luminescent properties and chiroptical activities....Fluorenylmethyloxycarbonyl(Fmoc)-protected amino acids are effective building blocks in self-assembled architectures at hierarchical levels,which however show limited luminescent properties and chiroptical activities.Here 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 acceptor.Embedding 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 acceptor.And,the solution-processed coassembly could selectively exhibit circularly polarized luminescence with high dissymmetry g-factors.This 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.展开更多
Baoquan Ding(丁宝全)Prof.Baoquan Ding received his bachelor’s degree in chemistry from Jilin University,China,in 2000.He obtained his Ph.D.in 2006 from the Department of Chemistry,New York University,USA,under the su...Baoquan Ding(丁宝全)Prof.Baoquan Ding received his bachelor’s degree in chemistry from Jilin University,China,in 2000.He obtained his Ph.D.in 2006 from the Department of Chemistry,New York University,USA,under the supervision of Professor Nadrian Seeman.He then worked as a Postdoctoral Research Fellow at the Molecular Foundry,Lawrence Berkeley National Laboratory,USA.He joined the Biodesign Institute at Arizona State University,USA,as a Research Assistant Professor in October 2009.He established his research group as a Professor at the National Center for Nanoscience and Technology,China,in November 2010.His research interests include DNA nanotechnology,coassembled biomolecules,and drug delivery.展开更多
Stimulating and harnessing circularly polarized luminescence(CPL)is not only a sine qua non for fundamentally unveiling chirogenesis in physical chemistry,but also a pivotal prerequisite for implementation of such phe...Stimulating and harnessing circularly polarized luminescence(CPL)is not only a sine qua non for fundamentally unveiling chirogenesis in physical chemistry,but also a pivotal prerequisite for implementation of such phenomenon in research fields including chiral optoelectronics and theranostics.Herein,red-emissive carbonized polymer dots(CPDs)-based helical structures were synthesized in this work via biomolecule-tailored organic–inorganic co-assembly strategy.The surface statesrelated chirality exhibits enhanced circular dichroism(CD)and CPL activities with anisotropic factors as high as gCD,max=5.4×10^(−3) and glum,max=1.5×10^(−2),respectively.The obtained CPL signals can be further manipulated in an excitationdependent manner,indicating that a synergistic-competition phenomenon exists between configurational chirality and intermolecular energy-transfer dynamics,which is further supported by simulations based on density function theory(DFT).Such tunable CPL behavior triggers revolutionary designs and applications of these chiral CPDs into the realm of chirality-related biological issues and next-generation chiral optoelectronics.展开更多
Proteins possess many biological functions.However, they can easily degrade or aggregate, thus losing their bioactivity. Therefore, it is very important to develop materials capable of interacting with proteins and fo...Proteins possess many biological functions.However, they can easily degrade or aggregate, thus losing their bioactivity. Therefore, it is very important to develop materials capable of interacting with proteins and forming nanostructures for protein storage and delivery. In this study,we serendipitously found a novel peptide-based supramolecular protein glue(Nap-GFFYK(γE)2-NH2, compound 1) that could co-assemble with proteins into nanofibers and hydrogels. We found that compound 1 rapidly folded into a β-sheet conformation upon contact with many proteins but not with polymers. Total internal reflection fluorescence microscopy(TIRFM) images clearly show the formation of co-assembled nanofibers by proteins and the peptide. The supramolecular protein glue could improve the dispersion of enzymes(lipase and lysozyme) and therefore enhance their catalytic activity,especially at high temperatures. More importantly, the supramolecular protein glue could co-assemble with two enzymes, glucose oxidase/horseradish peroxidase(GOx/HRP)and GOx/cytochrome c(cyt c), to form nanofibers that significantly enhanced the catalytic activity of tandem enzymatic reactions. We envisioned the great potential of our supramolecular protein glue for protein storage, delivery, and bioactivity manipulation.展开更多
文摘Polyvinyl alcohol(PVA)/laponite(LP)nanocomposite coatings were fabricated via a facile one-step coassembly process.The formed nanocoatings contain a high concentration of LP nanosheets,which can be well aligned along the substrate surface during the coassembly process.Due to the highly orientated structure,the flexible nanocoatings exhibit ultra-high transparency and superior mechanical properties,and can also act as excellent gas barriers.Such nanocoatings can be exceptional candidates for a variety of applications,such as food packaging.
基金supported by the National Natural Science Foundation of China(21901145,22171165,22371170)the financial support from the Youth Cross-Scientific Innovation Group of Shandong University。
文摘Unveiling the role of weak non-covalent forces in chiral self-assembly is pivotal in the design and fabrication of functional chiroptical materials.The 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 devices.In this work,we reveal the potential of AP forces in building diversified levels of chiral coassemblies adaptive to the geometries of PAHs.The naphthalene-F8was covalently conjugated with a chiral amine,which folded into a semi-rectangular geometry via two intramolecular F···H bonds.PAHs 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 ratio.The preference is adaptive to the geometries of PAHs,and experimental and computational results evidenced the ladder structures possess strong binding affinity.On 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.
基金supported by the National Natural Science Foundation of China(Nos.21901145,22171165)the financial support from Youth Cross-Scientific Innovation Group of Shandong University(No.2020QNQT003)。
文摘Benzimidazole amino acid derivatives behave as supramolecular hosts to include organic acids via complementary hydrogen bonding whereby supramolecular chirality and chiroptical properties could be manipulated.Organic acids enhanced the chiral assembly that showed tunable circularly polarized luminescence with high dissymmetry g-factors at 10^(-2)grade.
基金sponsored by the National Science Foundation(CMMI-1562907)the financial support from the National Natural Science Foundation of China(51678511 and 51308484)+4 种基金the Open Fund of Key Laboratory of Mineralogy and Metallogeny in Chinese Academy of Sciences(KLMM20150104)the Natural Science Foundation of Hunan Province(13JJ4049)the Education Department Fund of Hunan Province(14C1094)the Major Talent Training Program of Xiangtan University(16PYZ09)the Specialized Research Fund for the Doctoral Program of Xiangtan University(12QDZ18)
文摘Hybrid adsorbents for COcapture were prepared by coassembling laponite（LP） nanosheets and 1-nbutyl-3-methylimidazolium chloride（BMIMCl）. The prepared BMIMCl/LP layered hybrids were systematically characterized. The interlayer distance of the BMIMCl/LP layered hybrids expanded with an increasing concentration of BMIMCl, indicating that cumulative BMIMCl was intercalated into the LP layers. The efficiency of BMIMCl toward COcapture was significantly enhanced after it was immobilized within LP layers.
基金supported by the Qilu Young Scholarship Funding of Shandong Universitysupported by the National Natural Science Foundation of China(Nos.21901145,22171165)+1 种基金Natural Science Foundation of Jiangsu Province(No.BK20190209)the financial support from Youth cross-scientific innovation group of Shandong University(No.2020QNQT003)。
文摘Fluorenylmethyloxycarbonyl(Fmoc)-protected amino acids are effective building blocks in self-assembled architectures at hierarchical levels,which however show limited luminescent properties and chiroptical activities.Here 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 acceptor.Embedding 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 acceptor.And,the solution-processed coassembly could selectively exhibit circularly polarized luminescence with high dissymmetry g-factors.This 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.
文摘Baoquan Ding(丁宝全)Prof.Baoquan Ding received his bachelor’s degree in chemistry from Jilin University,China,in 2000.He obtained his Ph.D.in 2006 from the Department of Chemistry,New York University,USA,under the supervision of Professor Nadrian Seeman.He then worked as a Postdoctoral Research Fellow at the Molecular Foundry,Lawrence Berkeley National Laboratory,USA.He joined the Biodesign Institute at Arizona State University,USA,as a Research Assistant Professor in October 2009.He established his research group as a Professor at the National Center for Nanoscience and Technology,China,in November 2010.His research interests include DNA nanotechnology,coassembled biomolecules,and drug delivery.
基金National Natural Science Foundation of China,Grant/Award Number:22075240Shenzhen Fundamental Research Foundation,Grant/Award Number:JCYJ20180508162801893+3 种基金National Natural Science Foundation of Hubei Province,Grant/Award Numbers:2020CFB200,2021CFB018Guangdong Basic and Applied Basic Research Foundation,Grant/Award Number:2019A1515012094Project of Department of Education of Guangdong Province,Grant/Award Number:2018KTSCX198Shenzhen Basic Research Project of Science and Technology,Grant/Award Number:JCYJ20210324094414039。
文摘Stimulating and harnessing circularly polarized luminescence(CPL)is not only a sine qua non for fundamentally unveiling chirogenesis in physical chemistry,but also a pivotal prerequisite for implementation of such phenomenon in research fields including chiral optoelectronics and theranostics.Herein,red-emissive carbonized polymer dots(CPDs)-based helical structures were synthesized in this work via biomolecule-tailored organic–inorganic co-assembly strategy.The surface statesrelated chirality exhibits enhanced circular dichroism(CD)and CPL activities with anisotropic factors as high as gCD,max=5.4×10^(−3) and glum,max=1.5×10^(−2),respectively.The obtained CPL signals can be further manipulated in an excitationdependent manner,indicating that a synergistic-competition phenomenon exists between configurational chirality and intermolecular energy-transfer dynamics,which is further supported by simulations based on density function theory(DFT).Such tunable CPL behavior triggers revolutionary designs and applications of these chiral CPDs into the realm of chirality-related biological issues and next-generation chiral optoelectronics.
基金supported by the National Science Fund for Distinguished Young Scholars(31825012)the National Key Research and Development Program of China(2017YFC1103502)+4 种基金the National Natural Science Foundation of China(NSFC,51773097,51873156 and 21876116)Tianjin Science Fund for Distinguished Young Scholars(17JCJQJC44900)the National Program for Support of Topnotch Young Professionalsthe Fundamental Research Funds for the Central Universitiesthe Young Elite Scientists Sponsorship Program by Tianjin(TJSQNTJ-2017-16)
文摘Proteins possess many biological functions.However, they can easily degrade or aggregate, thus losing their bioactivity. Therefore, it is very important to develop materials capable of interacting with proteins and forming nanostructures for protein storage and delivery. In this study,we serendipitously found a novel peptide-based supramolecular protein glue(Nap-GFFYK(γE)2-NH2, compound 1) that could co-assemble with proteins into nanofibers and hydrogels. We found that compound 1 rapidly folded into a β-sheet conformation upon contact with many proteins but not with polymers. Total internal reflection fluorescence microscopy(TIRFM) images clearly show the formation of co-assembled nanofibers by proteins and the peptide. The supramolecular protein glue could improve the dispersion of enzymes(lipase and lysozyme) and therefore enhance their catalytic activity,especially at high temperatures. More importantly, the supramolecular protein glue could co-assemble with two enzymes, glucose oxidase/horseradish peroxidase(GOx/HRP)and GOx/cytochrome c(cyt c), to form nanofibers that significantly enhanced the catalytic activity of tandem enzymatic reactions. We envisioned the great potential of our supramolecular protein glue for protein storage, delivery, and bioactivity manipulation.
