pH-Responsive DNA assembles have drawn growing attentions owing to their great potential in diverse areas.However,pH-responsive motifs are limited to specific DNA sequences and annealing is usually needed for DNA asse...pH-Responsive DNA assembles have drawn growing attentions owing to their great potential in diverse areas.However,pH-responsive motifs are limited to specific DNA sequences and annealing is usually needed for DNA assemblies;therefore,sequence-independent pH-responsive DNA assembly at room temperature is highly desired as a more general way.Here,we propose a reversible pH-responsive DNA assembly strategy at room-temperature using zwitterion,glycine betaine(GB),as charge-regulation molecules.The reversible assembly and disassembly of DNA nanostructures could be achieved by alternatively regulating the acidic and basic environments in the presence of GB,respectively.In an acidic environment,carboxylate group in GB was protonated and GB was positively charged,which facilitated to shield the inherent electrostatic repulsion of DNA strands.Molecular simulation showed that the newly formed carboxyl group in protonated GB could form hydrogen bonds with bases in DNA to promote the assembly of DNA strands.In a basic solution,carboxylate group in GB was deprotonated and GB was neutral,thus inducing the dissociation of DNA assembly.展开更多
Supramolecular DNA hydrogels have been synthesized based on the assembly of DNA building-blocks such as branched DNA and long DNA chains.The structures and functions of sole-module DNA hydrogels remain limitations.New...Supramolecular DNA hydrogels have been synthesized based on the assembly of DNA building-blocks such as branched DNA and long DNA chains.The structures and functions of sole-module DNA hydrogels remain limitations.New methodologies by integrating hybrid components are desired to expand the synthesis of DNA hydrogel.Herein,we synthesized a Ln^(3+)-containing luminescent supramolecular hydrogel by employing the coordination and electrostatic interactions between lanthanide ions(Tb^(3+)and Eu^(3+))and linear single-stranded DNA(ssDNA).Through the coordination between ssDNA and Ln^(3+),a series of luminescent supramolecular hydrogels were synthesized,among which the Tb-G_(n)/T_(n)and Eu-T_(n)hydrogels emitted the characteristic luminescence of Tb and Eu,respectively.The luminescent intensities of the hydrogels were adjusted by designing DNA sequences with programmable bases and chain lengths.Notably,the Tb/Eu co-doped luminescent supramolecular hydrogel displayed tunable luminescence from green to yellow by regulating the stoichiometric ratio of Tb/Eu.Moreover,the hydrogel had reversible luminescent stimulation responsiveness toward Ag^(+)/L-Cys.We expected that the synthesis of Ln^(3+)-containing luminescent supramolecular hydrogels enriched the strategies of the construction of DNA hydrogels,and promoted the development of stimuli-responsive supramolecular materials.展开更多
基金Supported by the National Natural Science Foundation of China(Nos.21621004,21575101,21622404,21905196 and 31971305).
文摘pH-Responsive DNA assembles have drawn growing attentions owing to their great potential in diverse areas.However,pH-responsive motifs are limited to specific DNA sequences and annealing is usually needed for DNA assemblies;therefore,sequence-independent pH-responsive DNA assembly at room temperature is highly desired as a more general way.Here,we propose a reversible pH-responsive DNA assembly strategy at room-temperature using zwitterion,glycine betaine(GB),as charge-regulation molecules.The reversible assembly and disassembly of DNA nanostructures could be achieved by alternatively regulating the acidic and basic environments in the presence of GB,respectively.In an acidic environment,carboxylate group in GB was protonated and GB was positively charged,which facilitated to shield the inherent electrostatic repulsion of DNA strands.Molecular simulation showed that the newly formed carboxyl group in protonated GB could form hydrogen bonds with bases in DNA to promote the assembly of DNA strands.In a basic solution,carboxylate group in GB was deprotonated and GB was neutral,thus inducing the dissociation of DNA assembly.
基金supported in part by Tianjin Natural Science Foundation(Basic Research Plan,Grant Nos.18JCJQJC47600 and 19JCQNJC02200)。
文摘Supramolecular DNA hydrogels have been synthesized based on the assembly of DNA building-blocks such as branched DNA and long DNA chains.The structures and functions of sole-module DNA hydrogels remain limitations.New methodologies by integrating hybrid components are desired to expand the synthesis of DNA hydrogel.Herein,we synthesized a Ln^(3+)-containing luminescent supramolecular hydrogel by employing the coordination and electrostatic interactions between lanthanide ions(Tb^(3+)and Eu^(3+))and linear single-stranded DNA(ssDNA).Through the coordination between ssDNA and Ln^(3+),a series of luminescent supramolecular hydrogels were synthesized,among which the Tb-G_(n)/T_(n)and Eu-T_(n)hydrogels emitted the characteristic luminescence of Tb and Eu,respectively.The luminescent intensities of the hydrogels were adjusted by designing DNA sequences with programmable bases and chain lengths.Notably,the Tb/Eu co-doped luminescent supramolecular hydrogel displayed tunable luminescence from green to yellow by regulating the stoichiometric ratio of Tb/Eu.Moreover,the hydrogel had reversible luminescent stimulation responsiveness toward Ag^(+)/L-Cys.We expected that the synthesis of Ln^(3+)-containing luminescent supramolecular hydrogels enriched the strategies of the construction of DNA hydrogels,and promoted the development of stimuli-responsive supramolecular materials.
