Replicating extraordinarily high membrane transport selectivity of protein channels in artificial channel is a challenging task.In this work,we demonstrate that a strategic application of steric code-based social self...Replicating extraordinarily high membrane transport selectivity of protein channels in artificial channel is a challenging task.In this work,we demonstrate that a strategic application of steric code-based social self-sorting offers a novel means to enhance ion transport selectivities of artificial ion channels,alongside with boosted ion transport activities.More specifically,two types of mutually compatible sterically bulky groups(benzo-crown ether and tert-butyl group)were appended onto a monopeptide-based scaffold,which can order the bulky groups onto the same side of a one-dimensionally aligned H-bonded structure.Strong steric repulsions among the same type of bulky groups(either benzo-crown ethers or tert-butyl groups),which are forced into proximity by H-bonds,favor the formation of hetero-oligomeric ensem-bles that carry an alternative arrangement of sterically compatible benzo-crown ethers and tert-butyl groups,rather than homo-oligomeric ensembles containing a single type of either benzo-crown ethers or tert-butyl groups.Coupled with side chain tuning,this social self-sorting strategy delivers highly ac-tive hetero-oligomeric K+-selective ion channel(5F12-BF12)_(n),displaying the highest K+/Na+selectivity of 20.1 among artificial potassium channels and an excellent ECso value of 0.50μmol/L(0.62 mo1%relative to lipids)in terms of single channel concentration.展开更多
We describe here a class of unconventional ion transporters,molecular rotors that transport ions through a rotating function rather than via traditional carrier or channel mechanisms.Mimicking macroscopic rotors,these...We describe here a class of unconventional ion transporters,molecular rotors that transport ions through a rotating function rather than via traditional carrier or channel mechanisms.Mimicking macroscopic rotors,these molecular rotors consist of three modularly tunable components,i.e.,a membrane-anchoring stator,a crown ether-containing rotator for ion binding and transport,and a triple bond-based axle that allows the rotator to freely rotate around the stator in the lipid membrane.Lipid bilayer experiments reveal the generally high ability of all molecular rotors in promoting the highly efficient transmembrane K^(+)flux(EC50 values=0.49-1.37 mol%relative to lipid).While molecular rotors differing only in the ion-binding unit exhibit similar ion transport activities,those differing in the rotator’s length display activity differences by up to 174%.展开更多
The traditional approach to utilizing an ion-relay mechanism for ion transport requires three or more ion-relay stations.Herein,we describe a novel strategy,incorporating a swing action to realize a minimal ion-relay ...The traditional approach to utilizing an ion-relay mechanism for ion transport requires three or more ion-relay stations.Herein,we describe a novel strategy,incorporating a swing action to realize a minimal ion-relay mechanism via only two relay stations.This swing-relay mechanism was achieved using a class of crown ether-appended,long-armed molecular tetrahedrons(MTs).These MTs comprise ion-relaying crown units attached to a rigid tetrahedral core via flexible alkyl linkers,which act as the mobile arms and endow the crown units with great mobility to swing.展开更多
基金supported by the National Natural Science Foundation of China(No.22271049)Fuzhou University,Xiamen University and Northwestern Polytechnical University.
文摘Replicating extraordinarily high membrane transport selectivity of protein channels in artificial channel is a challenging task.In this work,we demonstrate that a strategic application of steric code-based social self-sorting offers a novel means to enhance ion transport selectivities of artificial ion channels,alongside with boosted ion transport activities.More specifically,two types of mutually compatible sterically bulky groups(benzo-crown ether and tert-butyl group)were appended onto a monopeptide-based scaffold,which can order the bulky groups onto the same side of a one-dimensionally aligned H-bonded structure.Strong steric repulsions among the same type of bulky groups(either benzo-crown ethers or tert-butyl groups),which are forced into proximity by H-bonds,favor the formation of hetero-oligomeric ensem-bles that carry an alternative arrangement of sterically compatible benzo-crown ethers and tert-butyl groups,rather than homo-oligomeric ensembles containing a single type of either benzo-crown ethers or tert-butyl groups.Coupled with side chain tuning,this social self-sorting strategy delivers highly ac-tive hetero-oligomeric K+-selective ion channel(5F12-BF12)_(n),displaying the highest K+/Na+selectivity of 20.1 among artificial potassium channels and an excellent ECso value of 0.50μmol/L(0.62 mo1%relative to lipids)in terms of single channel concentration.
基金This work was supported by Northwestern Poly-technical University.
文摘We describe here a class of unconventional ion transporters,molecular rotors that transport ions through a rotating function rather than via traditional carrier or channel mechanisms.Mimicking macroscopic rotors,these molecular rotors consist of three modularly tunable components,i.e.,a membrane-anchoring stator,a crown ether-containing rotator for ion binding and transport,and a triple bond-based axle that allows the rotator to freely rotate around the stator in the lipid membrane.Lipid bilayer experiments reveal the generally high ability of all molecular rotors in promoting the highly efficient transmembrane K^(+)flux(EC50 values=0.49-1.37 mol%relative to lipid).While molecular rotors differing only in the ion-binding unit exhibit similar ion transport activities,those differing in the rotator’s length display activity differences by up to 174%.
基金Northwestern Polytechnical University and the NanoBio Lab(Biomedical Research Council,Agency for Science,Technology,and Research).
文摘The traditional approach to utilizing an ion-relay mechanism for ion transport requires three or more ion-relay stations.Herein,we describe a novel strategy,incorporating a swing action to realize a minimal ion-relay mechanism via only two relay stations.This swing-relay mechanism was achieved using a class of crown ether-appended,long-armed molecular tetrahedrons(MTs).These MTs comprise ion-relaying crown units attached to a rigid tetrahedral core via flexible alkyl linkers,which act as the mobile arms and endow the crown units with great mobility to swing.