期刊
ACS NANO
卷 15, 期 11, 页码 17678-17688出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.1c05543
关键词
nanopore; molecular theory; weak polyampholyte; composition gradient; asymmetry
类别
资金
- National Science Foundation [CBET-1833214]
- Shenzhen Bay Laboratory
Researchers designed an artificial nanopore coated with an asymmetric polyampholyte brush to study asymmetric mass transport. They developed a nonequilibrium steady-state molecular theory and presented a comprehensive theoretical description of the stimuli-responsive structural behaviors and transport properties inside the nanopore with all molecular details considered. The model demonstrated the possibility of achieving asymmetric charge patterns and functional structures in a pH-responsive manner, leading to the nanopore acting as an ionic rectifier with a rectification factor above 1000 at optimized pH and salt concentration.
Molecular organizations and charge patterns inside biological nanopores are optimized by evolution to enhance ionic and molecular transport. Inspired by the nuclear pore complex that employs asymmetrically arranged disordered proteins for its gating, we here design an artificial nanopore coated by an asymmetric polyampholyte brush as a model system to study the asymmetric mass transport under nano-confinement. A nonequilibrium steady-state molecular theory is developed to account for the intricate charge regulation effect of the weak polyampholyte and to address the coupling between the polymer conformation and the external electric field. On the basis of this state-of-the-art theoretical method, we present a comprehensive theoretical description of the stimuli-responsive structural behaviors and transport properties inside the nanopore with all molecular details considered. Our model demonstrates that by incorporating a gradient of pH sensitivity into the polymer coatings of the nanopore, a variety of asymmetric charge patterns and functional structures can be achieved, in a pH-responsive manner that allows for multiple functions to be implemented into the designed system. The asymmetric charge pattern inside the nanopore leads to an electrostatic trap for major current carriers, which turns the nanopore into an ionic rectifier with a rectification factor above 1000 at optimized pH and salt concentration. Our theory further predicts that the nanopore design behaves like a double-gated nanofluidic device with pH-triggered opening of the gates, which can serve as an ion pump and pH-responsive molecular filter. These results deepen our understanding of asymmetric transport in nanoconfined systems and provide guidelines for designing polymer-coated smart nanopores.
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