Abstract Protons transport profoundly affects diverse fields from proton-exchange membrane fuel cells to storing liquid hydrogen. Recent advances have extended proton-exclusive transport to the two-dimensional channels that use hydrous mechanisms for fast proton transport, where the main challenge is the limited selectivity. However, the physical and chemical properties of 2D nanosheets like GO have the potential to implement full selective and ultrafast proton transport. Here, we uncover the physical potential of anhydrous proton transfer mechanism inside two-dimensional space between graphene nanosheets to exploit the exceptional full proton-selective ability and ultrafast conveyance speed of the Grotthuss mechanism. Reactive molecular dynamics simulations illustrate that the interlayer space between two graphene oxide nanosheets, carpeted with hydroxyl functional groups as additional hopping stages to enable the Grotthuss mechanism, can convey protons without water. Further, we dissect three essential factors that provide a deeper insight into ultrafast proton transport: (i) transitional phase to full anhydrous transport, (ii) outlet size for containing undesired species, and (iii) elastic behavior of the membranes under external strain. Our results show that changes in surface geometry can dramatically increase the diffusion rate in the presence of a small electric field by ~70% compared to hydrous transport. These findings can be used not only to guide the efforts in manufacturing a new generation of sustainable nanochannels but also to advance the pioneering technologies revolving around hydrogen.

中文翻译：

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在 Grotthuss 机制下通过无水氧化石墨烯膜的完美选择性和超快质子传输洞察

摘要 质子传输深刻地影响着从质子交换膜燃料电池到储存液氢的各个领域。最近的进展已将质子专有传输扩展到使用含水机制进行快速质子传输的二维通道，其中主要挑战是有限的选择性。然而，像 GO 这样的二维纳米片的物理和化学性质有可能实现完全选择性和超快的质子传输。在这里，我们揭示了石墨烯纳米片之间二维空间内无水质子转移机制的物理潜力，以利用 Grotthuss 机制的卓越全质子选择性能力和超快传输速度。反应分子动力学模拟表明，两个氧化石墨烯纳米片之间的层间空间，覆盖有羟基官能团作为额外的跳跃阶段以启用 Grotthuss 机制，可以在没有水的情况下传输质子。此外，我们剖析了三个基本因素，可以更深入地了解超快质子传输：（i）过渡阶段到完全无水传输，（ii）包含不需要的物种的出口尺寸，以及（iii）膜在外部应变下的弹性行为。我们的结果表明，与含水传输相比，在存在小电场的情况下，表面几何形状的变化可以显着增加约 70% 的扩散速率。这些发现不仅可用于指导制造新一代可持续纳米通道的工作，还可用于推进围绕氢的开创性技术。