Chiral mesoporous silica ribbons and rods with inversed handedness have been synthesized with the same enantio pure N-acylaminoacidat temperatures of 0℃and 20℃ respectively. With involving Cu^(2+)and meso-tetra(4-su...Chiral mesoporous silica ribbons and rods with inversed handedness have been synthesized with the same enantio pure N-acylaminoacidat temperatures of 0℃and 20℃ respectively. With involving Cu^(2+)and meso-tetra(4-sulfonatophenyl)porphyrin(TPPS) as probes, ribbons and rods revealed opposite signals in diffuse-reflectance circular dichroism(DRCD) spectra, indicating the existence of inversed supramolecular chiral imprintings through helical stacking of amphiphiles. The structural evolution was systematically studied by the freeze-dried products sampled at different time after the addition of silica precursors. The H-bonding-depended molecular orientation probably controls the chiral sense upon forming chiral molecular stacking, which would be the origin of such handedness inversion展开更多
Fibonacci number spiral patterns can be found in nature,particularly in plants,such as the sunflowers and phyllotaxis.Here,we demonstrated this pattern can be reproduced spontaneously within self-assembling peptide na...Fibonacci number spiral patterns can be found in nature,particularly in plants,such as the sunflowers and phyllotaxis.Here,we demonstrated this pattern can be reproduced spontaneously within self-assembling peptide nanofibril films.By high-temperature water vapor annealing of an amorphous film containing both peptide and cationic diamines,well-defined amyloid-like nanofibrils can be assembled spontaneously,during which the nanofibrils will hierarchically stack with each other following the Fibonacci number patterns.The formation of the patterns is a selftemplated process,which involves stepwise chiral amplification from the molecular scale to the nano-and micro-scales.Moreover,by controlling the diameter,length,and handedness of the nanofibrils,various complex hierarchical structures could be formed,including vertically aligned nanoarray,mesoscale helical bundles,Fibonacci number spirals,and then helical toroids.The results provide new insights into the chiral self-assembly of simple biological molecules,which can advance their applications in optics and templated synthesis.展开更多
基金supported by the National Natural Science Foundation of China (Nos. 21471099, 21601123)
文摘Chiral mesoporous silica ribbons and rods with inversed handedness have been synthesized with the same enantio pure N-acylaminoacidat temperatures of 0℃and 20℃ respectively. With involving Cu^(2+)and meso-tetra(4-sulfonatophenyl)porphyrin(TPPS) as probes, ribbons and rods revealed opposite signals in diffuse-reflectance circular dichroism(DRCD) spectra, indicating the existence of inversed supramolecular chiral imprintings through helical stacking of amphiphiles. The structural evolution was systematically studied by the freeze-dried products sampled at different time after the addition of silica precursors. The H-bonding-depended molecular orientation probably controls the chiral sense upon forming chiral molecular stacking, which would be the origin of such handedness inversion
基金supported by the National Natural Science Foundation of China(21621004 and 22078239)Tianjin Development Program for Innovation and Entrepreneurship(2018)the State Key Laboratory of Chemical Engineering(SKL-Ch E-20Z04 and SKL-Ch E-21T03)。
文摘Fibonacci number spiral patterns can be found in nature,particularly in plants,such as the sunflowers and phyllotaxis.Here,we demonstrated this pattern can be reproduced spontaneously within self-assembling peptide nanofibril films.By high-temperature water vapor annealing of an amorphous film containing both peptide and cationic diamines,well-defined amyloid-like nanofibrils can be assembled spontaneously,during which the nanofibrils will hierarchically stack with each other following the Fibonacci number patterns.The formation of the patterns is a selftemplated process,which involves stepwise chiral amplification from the molecular scale to the nano-and micro-scales.Moreover,by controlling the diameter,length,and handedness of the nanofibrils,various complex hierarchical structures could be formed,including vertically aligned nanoarray,mesoscale helical bundles,Fibonacci number spirals,and then helical toroids.The results provide new insights into the chiral self-assembly of simple biological molecules,which can advance their applications in optics and templated synthesis.
