论文标题

$ \ MATHCAL {P}^2 $:将压力和电化学结合在一起,以合成超水

$\mathcal{P}^2$: Combining pressure and electrochemistry to synthesize superhydrides

论文作者

Guan, Pin-Wen, Hemley, Russell J., Viswanathan, Venkatasubramanian

论文摘要

最近,在非常高的压力下,已在计算上鉴定了超水,并随后与多种金属合成。在这项工作中,我们评估了通过唯一结合电化学和施加压力来合成超水的可能性。我们使用密度功能理论和粒子群优化计算对钯超水的计算搜索进行了广泛的压力和电极电位。我们使用贝叶斯误差估计形式主义来纳入交换功能不确定性,以量化与已确定的稳定相相关的不确定性。基于热力学分析,我们构建了压力电位相图,并提供了替代合成概念,即$ \ Mathcal {p}^2 $(压力电位),以访问具有较高氢含量的新相。钯 - 氢气是一种广泛研究的材料系统,最高的氢化物相为PD $ _3 $ h $ _4 $。对于该系统而言,最引人注目的是,在高于氢进化的电位和$ \ sim $ 300 MPA压力下,我们发现有可能制作钯超氢(例如PDH $ _ {10} $)。我们证明了这种方法对La-H,Y-H和MG-H的普遍性,而稳定相的压力则减少了10-100倍。此外,$ \ MATHCAL {P}^2 $策略允许稳定无法纯粹是通过压力或潜力来完成的新阶段,并且是一种一般方法,很可能适合以适度的压力合成其他超级氢化物。

Recently, superhydrides have been computationally identified and subsequently synthesized with a variety of metals at very high pressures. In this work, we evaluate the possibility of synthesizing superhydrides by uniquely combining electrochemistry and applied pressure. We perform computational searches for palladium superhydrides using density functional theory and particle swarm optimization calculations over a broad range of pressures and electrode potentials. We incorporate exchange-correlation functional uncertainty using the Bayesian error estimation formalism to quantify the uncertainty associated with the identified stable phases. Based on a thermodynamic analysis, we construct pressure-potential phase diagrams and provide an alternate synthesis concept, $\mathcal{P}^2$ (pressure-potential), to accessing novel phases having high hydrogen content. Palladium-hydrogen is a widely-studied material system with the highest hydride phase being Pd$_3$H$_4$. Most strikingly for this system, at potentials above hydrogen evolution and $\sim$300 MPa pressure, we find the possibility to make palladium superhydrides (e.g., PdH$_{10}$). We demonstrate the generalizability of this approach for La-H, Y-H and Mg-H with 10-100 fold reduction in required pressure for stabilizing phases. In addition, the $\mathcal{P}^2$ strategy allows stabilizing new phases that cannot be done purely by either pressure or potential and is a general approach that is likely to work for synthesizing other superhydrides at modest pressures.

扫码加入交流群

加入微信交流群

微信交流群二维码

扫码加入学术交流群,获取更多资源