MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing, and Department of Applied Physics, Nanjing University of Science and Technology, Nanjing 210094, China.
Phys Chem Chem Phys. 2023 Mar 8;25(10):7477-7486. doi: 10.1039/d2cp05137k.
Charged asymmetric channels are extensively investigated for the design of artificial biological channels, ionic diodes, artificial separation films, These applications are attributed to the unique ionic current rectification phenomenon, where the surface charge density of the channel has a deep influence. In this work, we use molecular dynamics simulations to study the rectification phenomenon in asymmetric graphene oxide channels. A fascinating finding is that the ionic current rectification direction reverses from the negative to positive electric field direction with an increase in surface charge density. Specifically, at low charge density, the ionic flux reaches greater values in the negative electric field due to the enrichment of cations and anions, which provides a sufficient electrostatic shielding effect inside the channel and increases the possibility of ion release by the residues. However, at high charge density, the extremely strong residue attraction induces a Coulomb blockade effect in the negative electric field, which seriously impedes the ion transport and eventually leads to a smaller ionic current. Consequently, this ionic current order transition ultimately results in the rectification reversion phenomenon, providing a new route for the design of some novel nanofluidic devices.
带电不对称通道被广泛研究用于设计人工生物通道、离子二极管、人工分离膜等。这些应用归因于独特的离子电流整流现象,其中通道的表面电荷密度具有深远的影响。在这项工作中,我们使用分子动力学模拟研究了不对称氧化石墨烯通道中的整流现象。一个有趣的发现是,随着表面电荷密度的增加,离子电流整流方向从负电场方向反转到正电场方向。具体来说,在低电荷密度下,由于阳离子和阴离子的富集,离子通量在负电场中达到更大的值,这在通道内部提供了足够的静电屏蔽效应,并增加了残基释放离子的可能性。然而,在高电荷密度下,极强的残基吸引力在负电场中诱导库仑阻塞效应,严重阻碍离子输运,最终导致较小的离子电流。因此,这种离子电流顺序的转变最终导致整流反转现象,为一些新型纳流控器件的设计提供了新途径。
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