论文标题
纳米结构的PT掺杂2D Mose $ _2 $：用于氢进化和氧还原反应的有效双功能电催化剂
Nanostructured Pt-Doped 2D MoSe$_2$: An Efficient Bifunctional Electrocatalyst for both Hydrogen Evolution and Oxygen Reduction Reactions
论文作者
论文摘要
TMD是一个新的2D材料家族，其功能使它们吸引了纳米材料科学和工程领域的潜在应用。尽管2D TMD的边缘显示出出色的电催化性能，但它们的基础平面是惰性的，它阻碍了电催化的工业应用。在这里，我们在计算上设计了2D单层Mose $ _2 $，并通过电催化活性研究了其电子特性。 PT-ATOM已在原始的2D Mose $ _2 $中掺杂，以激活惰性基础平面，导致零带隙。这项研究表明，PT-Mose $ _2 $是借助DFT的氢进化反应（HER）和氧还原反应（ORR）的极好双功能电催化剂。已经应用了定期混合DFT方法来计算原始摩西$ _2 $和pt-mose $ _2 $的电子特性。为了确定PT-Mose2材料表面上的HER和ORR机制，通过考虑分子PT1-MO $ _9 $ SE $ se $ {21} $ cluster模型，已经执行了非周期性DFT计算。本研究表明，2D PT-MOSE $ _2 $遵循Volmer-Heyrovsky机制为她提供了约9.29 kcal/mol和10.55 kcal.mol-1在H Migration和Heyrovsky反应期间的能量屏障。 ORR是通过四电子转移机制来实现的，形成了大约14.94 kcal/mol和11.10 kcal/mol的两个过渡能屏障。在反应期间，较低的能障和高的周转频率暴露出PT-MOSE $ _2 $可以用作HER和ORR的有效双功能电催化剂。本研究表明，可以通过PT掺杂来增强她和ORR的活动和稳定性和稳定性性能，可以通过PT掺杂来增强，为H2生产和降低O2的高性能催化剂的明智设计开辟了一个有希望的概念。
TMDs are a new family of 2D materials with features that make them appealing for potential applications in nanomaterials science and engineering. Although, the edges of the 2D TMDs show excellent electrocatalytic performance, their basal plane is inert which hinders the industrial applications for electrocatalysis. Here, we have computationally designed the 2D monolayer MoSe$_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.
