纳米结构Pt掺杂二维MoSe $_2$：一种高效的析氢和氧还原双功能电催化剂
Nanostructured Pt-Doped 2D MoSe$_2$: An Efficient Bifunctional Electrocatalyst for both Hydrogen Evolution and Oxygen Reduction Reactions
摘要：
TMD是一种新的2D材料家族，其特性使其在纳米材料科学和工程中具有潜在的应用。虽然二维TMD的边缘显示出优异的电催化性能，但它们的基面是惰性的，这阻碍了电催化的工业应用。在这里，我们计算设计了二维单层MoSe $_2$，并研究了其电催化活性的电子性质。Pt原子已经被掺杂在原始的2D MoSe $_2$中以激活惰性基面，从而产生零带隙。研究表明，Pt-MoSe $_2$是一种优良的双功能电催化剂，可用于析氢反应（HER）和氧还原反应（ORR）。用周期混合密度泛函方法计算了原始MoSe $_2$和Pt-MoSe $_2$的电子性质.为了确定在Pt-MoSe 2材料表面上的HER和ORR机制，通过考虑分子Pt 1-Mo $_9$ Se ${21}$簇模型进行了非周期性DFT计算。研究表明，二维Pt-MoSe $_2$的氢迁移和Heyrovsky反应的势垒分别为9.29 kcal/mol和10.55 kcal·mol-1，符合Volmer-Heyrovsky机理. ORR是通过四电子转移机制实现的，形成了两个跃迁势垒，分别约为14.94 kcal/mol和11.10 kcal/mol。Pt-MoSe $_2$具有较低的能垒和较高的转化率，是一种高效的双功能电催化剂。目前的研究表明，由MoSe $_2$电催化剂显示的优异的HER和ORR活性和稳定性性能可以通过Pt掺杂来增强，为用于H2生产和O2还原的高性能催化剂的合理设计打开了一个有前途的概念。
英文摘要：
TMDs are a new family of 2D materials with features that make them appealing for potential applications in nanomaterials science and engineering. Although, the edges of the 2D TMDs show excellent electrocatalytic performance, their basal plane is inert which hinders the industrial applications for electrocatalysis. Here, we have computationally designed the 2D monolayer MoSe$_2$ and studied its electronic properties with electrocatalytic activities. Pt-atom has been doped in the pristine 2D MoSe$_2$ to activate the inert basal plane resulting zero bandgap. This study reveals that the Pt-MoSe$_2$ is an excellent bifunctional electrocatalyst for both the hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR) with the aid of the DFT. Periodic hybrid DFT method has been applied to compute the electronic properties of both the pristine MoSe$_2$ and Pt-MoSe$_2$. To determine both the HER and ORR mechanisms on the surface of the Pt-MoSe2 material, a non-periodic DFT calculation has been performed by considering a molecular Pt1-Mo$_9$Se${21}$ cluster model. The present study shows that the 2D Pt-MoSe$_2$ follows Volmer-Heyrovsky mechanism for HER with the energy barriers about 9.29 kcal/mol and 10.55 kcal.mol-1 during the H-migration and Heyrovsky reactions. The ORR is achieved by four-electron transfer mechanism with the formation of two transition energy barriers about 14.94 kcal/mol and 11.10 kcal/mol, respectively. The lower energy barriers and high turnover frequency during the reactions expose that the Pt-MoSe$_2$ can be adopted as an efficient bifunctional electrocatalyst for both the HER and ORR. The present studies demonstrate that the exceptional HER and ORR activity and stability performance shown by the MoSe$_2$ electrocatalyst can be enhanced by Pt-doping, opening a promising concept for the sensible design of high-performance catalyst for H2 production and O2 reduction.
机构、总结、中文摘要均由AI分析而来，可能存在错误，请以论文正文为准。
