Tong Tianyue, Linghu Yaoyao, Wu Guangping, Wang Chao, Wu Chao
School of Materials Science and Engineering, North University of China, Taiyuan 030051, P. R. China.
Advanced Energy Materials and Systems Institute, North University of China, Taiyuan 030051, P. R. China.
Phys Chem Chem Phys. 2022 Aug 10;24(31):18943-18951. doi: 10.1039/d2cp01500e.
Nitric oxide electrochemical reduction (NOER) reactions are usually catalyzed by noble metals. However, the commercial applications are limited by the low atomic utilization and high price, which prompt researchers to turn their attentions to single-atom catalysts (SACs). Recently, a novel two-dimensional semiconducting material MoSiN (MSN) has been synthesized and is suitable for the substrate of SACs due to its high stability, carrier mobility and mechanical strength. Herein, we employed first principles calculations to investigate the catalytic properties of transition metal doped MoSiN monolayers (labelled as TM-MSN, where TM is a transition metal atom from 3d to 5d except Y, Tc, Cd, La-Lu and Hg) in NO reduction. The calculated results demonstrate that the introduction of Zr, Pd, Pt, Mn, Au, or Mo atoms can greatly improve the catalytic NOER performance of a pristine MSN monolayer. Zr-MSN and Pt-MSN monolayers at low coverage exhibit the most superior catalytic activity and selectivity for NH production with a limiting potential of 0 and -0.10 V. This work may help guide the application of MSN monolayer in the area of energy conversion.
一氧化氮电化学还原（NOER）反应通常由贵金属催化。然而，其商业应用受到低原子利用率和高价格的限制，这促使研究人员将注意力转向单原子催化剂（SAC）。最近，一种新型二维半导体材料MoSiN（MSN）已被合成，由于其高稳定性、载流子迁移率和机械强度，它适用于SAC的基底。在此，我们采用第一性原理计算来研究过渡金属掺杂的MoSiN单层（标记为TM-MSN，其中TM是除Y、Tc、Cd、La-Lu和Hg之外的从3d到5d的过渡金属原子）在NO还原中的催化性能。计算结果表明，引入Zr、Pd、Pt、Mn、Au或Mo原子可以大大提高原始MSN单层的催化NOER性能。低覆盖率下的Zr-MSN和Pt-MSN单层对NH生成表现出最优异的催化活性和选择性，极限电位分别为0和-0.10 V。这项工作可能有助于指导MSN单层在能量转换领域的应用。
