Zhang Feixiang, Wang Panshuo, Zhu Yandi, Shi Jinlei, Pang Rui, Ren Xiaoyan, Li Shunfang
Key Laboratory of Material Physics, Ministry of Education, School of Physics, Zhengzhou University, Zhengzhou, China.
College of Physics and Electronic Engineering, Zhengzhou Normal University, Zhengzhou, China.
Nat Commun. 2025 Feb 12;16(1):1580. doi: 10.1038/s41467-025-56863-1.
In modern chemistry, the development of highly efficient room-temperature catalysts is of great significance and remains a long-standing challenge in various typical reactions. Here, we theoretically demonstrate that the two-dimensional (2D) multiferroic, Cr(half-fluoropyrazine) [Cr(h-fpyz)], is a promising single-atom catalyst (SAC) operating at room temperature for CO oxidation. The rate-limiting barrier is merely 0.325 eV, leading to a reaction rate (i.e., 3.47 × 10 s) of six orders of magnitude higher than its monoferroic derivative [Cr(pyz)], due to the synergetic effects of two aspects. First, the more flexible ligand rotations in Cr(h-fpyz) facilitate the activation of O molecule, simultaneously enhancing the charge transfer and spin-accommodation process. Second, on Cr(h-fpyz), O adsorption induces a distinctly lower local positive electric field, reducing the electrostatic repulsion of the polar CO molecule. These findings may also pave the way for establishing highly efficient SAC platforms based on 2D multiferroics where multidegree of freedom (e.g., spin, polarity) synergistically matter.
在现代化学中，开发高效的室温催化剂具有重要意义，并且在各种典型反应中仍然是一个长期存在的挑战。在此，我们从理论上证明，二维（2D）多铁性材料Cr(半氟吡嗪)[Cr(h-fpyz)]是一种有前景的室温下用于CO氧化的单原子催化剂（SAC）。限速势垒仅为0.325 eV，由于两方面的协同效应，导致其反应速率（即3.47×10 s）比其一铁性衍生物[Cr(pyz)]高六个数量级。首先，Cr(h-fpyz)中更灵活的配体旋转促进了O分子的活化，同时增强了电荷转移和自旋容纳过程。其次，在Cr(h-fpyz)上，O吸附诱导出明显更低的局部正电场，降低了极性CO分子的静电排斥。这些发现也可能为基于2D多铁性材料建立高效SAC平台铺平道路，在该平台中多自由度（如自旋、极性）协同起作用。
