Abstract

AbstractThe realization of quasicrystals has attracted a considerable attention due to their unusual structures and properties. The concept of quasicrystals in the atomically thin materials is even more appealing due to the in‐plane covalent bonds and weak interlayer interactions. Here, it is demonstrated that 2D quasicrystals can be created/isolated from bulk phases because of long‐range interlayer ordered aperiodic arrangements. An ultrasonication‐assisted exfoliation of polygrained icosahedral Al–Pd–Mn quasicrystals at room temperature shows the formation of a large area of mono‐ and few layers in threefold quasicrystalline plane. The formation of these layers from random grain orientation consistently indicates that the threefold plane is most stable in comparison to the twofold and fivefold planes in icosahedral clusters. The above experimental observations are further supported with help of theoretical simulations. The mono‐ and few‐layered aperiodic planes render plentiful active sites for the catalysis of hydrogen evolution reaction. The threefold 2D quasicrystalline plane exhibits a hydrogen evolution reaction overpotential of ≈100 mV (160 times less than bulk counterpart) and long‐term durability. These systems constitute the first demonstration of quasicrystalline monolayer ordering in a free‐standing thin layer without requiring the support of periodic or aperiodic substrate.

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