Immobilization of single argon atoms in nano-cages of two-dimensional zeolite model systems.

Immobilization of single argon atoms in nano-cages of two-dimensional zeolite model systems.
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DOI:
10.1038/ncomms16118
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发表时间:
2017-07-17
影响因子:
16.6
通讯作者:
Boscoboinik JA
Boscoboinik JA
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Zhong JQ;Wang M;Akter N;Kestell JD;Boscoboinik AM;Kim T;Stacchiola DJ;Lu D;Boscoboinik JA

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与块状材料相比,在非低温下将惰性气体限制在纳米结构表面是一项艰巨的挑战。在这项工作中,单个Ar原子被囚禁在300 K的纳米笼子中,该笼子由(铝)硅酸盐六角棱镜组成,在平面上形成二维阵列。利用基于同步加速器的常压X射线光电子能谱原位探测了Ar原子的俘获。当加热到400 K时,原子仍然留在笼子中。结合表面科学方法和密度泛函理论计算,研究了Ar的捕获和释放。虽然Ar原子的加入保持了骨架的完整性,但气体(例如CO)通过骨架的渗透性受到了显著影响,使这些结构也成为可调原子和分子筛的有趣候选者。这些发现使使用表面科学方法研究单独受限的稀有气体原子成为可能,为基础研究开辟了新的机会。虽然惰性气体可以被困在3D多孔结构中,但将它们固定在2D表面上是一个巨大的挑战。在这里,作者在室温下将单个Ar原子囚禁在2D模型沸石骨架中,为利用表面科学方法对孤立的惰性气体原子进行基础研究提供了令人兴奋的机会。
The confinement of noble gases on nanostructured surfaces, in contrast to bulk materials, at non-cryogenic temperatures represents a formidable challenge. In this work, individual Ar atoms are trapped at 300 K in nano-cages consisting of (alumino)silicate hexagonal prisms forming a two-dimensional array on a planar surface. The trapping of Ar atoms is detected in situ using synchrotron-based ambient pressure X-ray photoelectron spectroscopy. The atoms remain in the cages upon heating to 400 K. The trapping and release of Ar is studied combining surface science methods and density functional theory calculations. While the frameworks stay intact with the inclusion of Ar atoms, the permeability of gasses (for example, CO) through them is significantly affected, making these structures also interesting candidates for tunable atomic and molecular sieves. These findings enable the study of individually confined noble gas atoms using surface science methods, opening up new opportunities for fundamental research. While noble gases can be trapped in 3D porous structures, immobilizing them on 2D surfaces represents a formidable challenge. Here, the authors cage individual argon atoms in 2D model zeolite frameworks at room temperature, providing exciting opportunities for the fundamental study of isolated noble gas atoms using surface science methods.
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