Ando Sumiya, Yamamoto Eisuke, Kobayashi Makoto, Osada Minoru
Department of Materials Chemistry & Institute of Materials and Systems for Sustainability (IMaSS), Nagoya University, Nagoya 464-8601, Japan.
Research Institute for Quantum and Chemical Innovation, Institutes of Innovation for Future Society, Nagoya University, Nagoya 464-8601, Japan.
Nano Lett. 2024 Sep 11;24(36):11239-11245. doi: 10.1021/acs.nanolett.4c02741. Epub 2024 Aug 5.
Thickness control of two-dimensional (2D) metal nanosheets (metallenes) has scientific significance for energy and catalyst applications, yet is unexplored owing to the lack of an efficient approach for the tailored synthesis of metallenes with controlled atomic layers. Here we report a 2D template-directed synthesis of ultrathin Pd nanosheets with well-controlled thicknesses. Molecularly thin single-crystalline Pd nanosheets with well-defined hexagonal morphologies were synthesized via a one-pot method with 2,4,6-trichlorophenyl formate. Such Pd nanosheets were used as hard templates for the tailored synthesis of the Pd nanosheets with controlled thicknesses (9, 11, 13, and 15 atomic layers). Hard X-ray photoelectron spectroscopy and density functional theory calculations revealed unique electronic states in thickness-controlled Pd nanosheets; these states included reduced surface charges to bulk, increased work functions, and decreased -band centers. Thus, atomic layer engineering of Pd nanosheets enabled the fine-tuning of the surface electronic states to improve the hydrogen evolution reaction.
二维（2D）金属纳米片（金属烯）的厚度控制对于能量和催化剂应用具有科学意义，但由于缺乏一种有效的方法来定制合成具有可控原子层数的金属烯，这方面尚未得到探索。在此，我们报告了一种二维模板导向合成具有精确控制厚度的超薄钯纳米片的方法。通过使用甲酸2,4,6 - 三氯苯酯的一锅法合成了具有明确六边形形态的分子级薄的单晶钯纳米片。这种钯纳米片被用作硬模板，用于定制合成具有可控厚度（9、11、13和15个原子层）的钯纳米片。硬X射线光电子能谱和密度泛函理论计算揭示了厚度可控的钯纳米片中独特的电子态；这些态包括表面电荷向体相的减少、功函数的增加以及能带中心的降低。因此，钯纳米片的原子层工程能够微调表面电子态以改善析氢反应。
