制备稳定的表面活性剂囊泡是进一步发展囊泡技术的关键.本工作制备了两种酰胺基分别在疏水链和连接基团的阳离子Gemini表面活性剂(C_(12)A-C_(2)-AC_(2)和C_(2)-AC_(12)A-C_(2))与阴离子谷氨酸表面活性剂(C_(2)Glu)混合体系囊泡,系统研...制备稳定的表面活性剂囊泡是进一步发展囊泡技术的关键.本工作制备了两种酰胺基分别在疏水链和连接基团的阳离子Gemini表面活性剂(C_(12)A-C_(2)-AC_(2)和C_(2)-AC_(12)A-C_(2))与阴离子谷氨酸表面活性剂(C_(2)Glu)混合体系囊泡,系统研究了酰胺基位置和羧基间氢键对囊泡形成与热稳定性的影响.结果表明,位于疏水链上的酰胺基通过氢键可有效促进表面活性剂混合体系囊泡形成和热稳定性,C_(12)A-C_(2)-AC_(2)&C_(2)Glu囊泡在升高温度过程中保持蓝色乳光不变,但对于酰胺基位于连接基团上的C_(2)-AC_(12)A-C_(2)&C_(2)Glu囊泡溶液,其蓝色乳光随温度升高逐渐转变为乳白色或出现沉淀,降低温度溶液再次恢复蓝色乳光.含有两个羧基的C_(2)Glu的带电量及分子间氢键随p H此消彼长,p H 5.0时C_(2)Glu羧基形成的分子间氢键促进了C_(12)A-C_(2)-AC_(2)&C_(2)Glu和C_(2)-AC_(12)A-C_(2)&C_(2)Glu囊泡的形成和热稳定性,在升温过程中混合体系囊泡溶液均没有产生沉淀,而p H 10.0时这两个体系形成的囊泡溶液随温度升高分别出现蓝色乳光加深和沉淀现象.这类具有温度响应性、高效形成囊泡的体系具有重要的实际应用价值.展开更多
Low-molecular weight surfactants have significant potential as building blocks for prebiotic organization.However,reports about surfactant-based coacervates as protocell models capable of reversible transformation are...Low-molecular weight surfactants have significant potential as building blocks for prebiotic organization.However,reports about surfactant-based coacervates as protocell models capable of reversible transformation are scarce.Herein,we develop a simple system made of a surfactant(-)-N-dodecylN-methylephedrinium bromide(DMEB)and inorganic salts that is capable of spontaneous formation of vesicles,coacervates,and the reversible transformation between the two states.展开更多
The diversity of protocell membrane structures is crucial for the regulation of cell activities and indispensable to the origin of life.Prior to the evolution of complex cellular machinery,spontaneous protocell membra...The diversity of protocell membrane structures is crucial for the regulation of cell activities and indispensable to the origin of life.Prior to the evolution of complex cellular machinery,spontaneous protocell membrane evolution results from the intrinsic physicochemical properties of simple molecules under specific environmental conditions.Here,we report the evolution of the morphology of cell-sized model protocell membranes from giant vesicles to pearling and helical nanostructures,resembling morphologies of eukaryocytes,nostoc,and spirilla.This evolution occurs in a single binary aqueous system composed of an achiral single-chain amphiphile and a biogenic polyamine(spermidine or spermine)upon evaporating water,feeding amphiphiles,or increasing pH in response to various primitive fluctuating conditions.In contrast,nonbiogenic polyamines(triamine,triethylenetetramine,and hexamethyltriethylenetetramine)with slight differences in the number of methylene groups or protonated amine groups do not induce such a kind of evolution.The evolution of the shape transformation strongly relies on the balance between electrostatic attraction and hydrogen bonding,attributed to the odd/even effect of polyamines in the assembly.Strikingly,both pearling and helical structures emerge from multilamellar vesicles undergoing different processes,where the helix shows stronger permeability and encapsulation capability due to its multicompartmentalized structure.Thus,subtle adjustment of weak intramolecular interactions not only yields significant changes in the morphological evolution of protocell membranes but also brings new insights into the natural inevitability of biogenic small molecules.展开更多
文摘制备稳定的表面活性剂囊泡是进一步发展囊泡技术的关键.本工作制备了两种酰胺基分别在疏水链和连接基团的阳离子Gemini表面活性剂(C_(12)A-C_(2)-AC_(2)和C_(2)-AC_(12)A-C_(2))与阴离子谷氨酸表面活性剂(C_(2)Glu)混合体系囊泡,系统研究了酰胺基位置和羧基间氢键对囊泡形成与热稳定性的影响.结果表明,位于疏水链上的酰胺基通过氢键可有效促进表面活性剂混合体系囊泡形成和热稳定性,C_(12)A-C_(2)-AC_(2)&C_(2)Glu囊泡在升高温度过程中保持蓝色乳光不变,但对于酰胺基位于连接基团上的C_(2)-AC_(12)A-C_(2)&C_(2)Glu囊泡溶液,其蓝色乳光随温度升高逐渐转变为乳白色或出现沉淀,降低温度溶液再次恢复蓝色乳光.含有两个羧基的C_(2)Glu的带电量及分子间氢键随p H此消彼长,p H 5.0时C_(2)Glu羧基形成的分子间氢键促进了C_(12)A-C_(2)-AC_(2)&C_(2)Glu和C_(2)-AC_(12)A-C_(2)&C_(2)Glu囊泡的形成和热稳定性,在升温过程中混合体系囊泡溶液均没有产生沉淀,而p H 10.0时这两个体系形成的囊泡溶液随温度升高分别出现蓝色乳光加深和沉淀现象.这类具有温度响应性、高效形成囊泡的体系具有重要的实际应用价值.
基金supported by National Natural Science Foundation of China(grant nos.21972149,21988102,21811530002,21633002,and 21761142007).
文摘Low-molecular weight surfactants have significant potential as building blocks for prebiotic organization.However,reports about surfactant-based coacervates as protocell models capable of reversible transformation are scarce.Herein,we develop a simple system made of a surfactant(-)-N-dodecylN-methylephedrinium bromide(DMEB)and inorganic salts that is capable of spontaneous formation of vesicles,coacervates,and the reversible transformation between the two states.
基金supported by the National Natural Science Foundation of China(Nos.21972149 and 21988102).
文摘The diversity of protocell membrane structures is crucial for the regulation of cell activities and indispensable to the origin of life.Prior to the evolution of complex cellular machinery,spontaneous protocell membrane evolution results from the intrinsic physicochemical properties of simple molecules under specific environmental conditions.Here,we report the evolution of the morphology of cell-sized model protocell membranes from giant vesicles to pearling and helical nanostructures,resembling morphologies of eukaryocytes,nostoc,and spirilla.This evolution occurs in a single binary aqueous system composed of an achiral single-chain amphiphile and a biogenic polyamine(spermidine or spermine)upon evaporating water,feeding amphiphiles,or increasing pH in response to various primitive fluctuating conditions.In contrast,nonbiogenic polyamines(triamine,triethylenetetramine,and hexamethyltriethylenetetramine)with slight differences in the number of methylene groups or protonated amine groups do not induce such a kind of evolution.The evolution of the shape transformation strongly relies on the balance between electrostatic attraction and hydrogen bonding,attributed to the odd/even effect of polyamines in the assembly.Strikingly,both pearling and helical structures emerge from multilamellar vesicles undergoing different processes,where the helix shows stronger permeability and encapsulation capability due to its multicompartmentalized structure.Thus,subtle adjustment of weak intramolecular interactions not only yields significant changes in the morphological evolution of protocell membranes but also brings new insights into the natural inevitability of biogenic small molecules.
