离域电子
结晶学
Atom(片上系统)
材料科学
电子结构
兴奋剂
物理
机器学习
凝聚态物理
化学
计算机科学
量子力学
嵌入式系统
作者
Cynthia Wang,Mei Yang,Shuo Cao,Xiaoxu Wang,Hao Fu,Yang Bai,Turab Lookman,Ping Qian,Yanjing Su
出处
期刊:Physical Review Materials
[American Physical Society]
日期:2023-08-02
卷期号:7 (8)
标识
DOI:10.1103/physrevmaterials.7.085801
摘要
Two-dimensional (2D) Mo-based MXenes $({\mathrm{Mo}}_{n+1}{C}_{n}{T}_{x})$ are recognized to have significant potential as hydrogen evolution reaction (HER) activity electrocatalysts. However, appropriate descriptors are absent to predict the H-adsorption Gibbs energy $(\mathrm{\ensuremath{\Delta}}{G}_{\mathrm{H}})$ due to the unique delocalized electronic properties of the Mo atom. In this paper, we used first-principles calculations and machine learning to study the HER activity of ${\mathrm{Mo}}_{2}\mathrm{C}{\mathrm{O}}_{2}$ with single transition metal-doped (${\mathrm{Mo}}_{2}\mathrm{C}{\mathrm{O}}_{2}$-STM), and elucidate the mechanisms by which single transition metals (STMs) regulate the hydrogen evolution reaction. Our results revealed that $\mathrm{\ensuremath{\Delta}}{G}_{\mathrm{H}}$ has a ``W'' shape as a function of the doped atom changing in one period. The electronic structure analysis indicates that the electronic delocalized Mo has a longer range affecting not only the nearest atoms, but the second-nearest neighbor (STM-Mo) bonding effect controls the periodic distribution of $\mathrm{\ensuremath{\Delta}}{G}_{\mathrm{H}}$. Using machine-learning method, we quantized the STM regulation mechanism using five key structural and electronic descriptors, and predicted the $\mathrm{\ensuremath{\Delta}}{G}_{\mathrm{H}}$ of ${\mathrm{Mo}}_{2}\mathrm{C}{\mathrm{O}}_{2}$-STM, which were also extended to ${\mathrm{W}}_{2}\mathrm{C}{\mathrm{O}}_{2}$-STM successfully. Our findings highlight the importance of considering second-nearest-neighbor bonding effects in similar delocalized materials systems research.
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