未成对电子
氢原子
化学
自旋态
Atom(片上系统)
自旋(空气动力学)
单层
氢
催化作用
化学物理
结晶学
原子物理学
分子
无机化学
物理
群(周期表)
有机化学
热力学
生物化学
计算机科学
嵌入式系统
作者
Tao Zhang,Lei Li,Tao Huang,Hui Wan,Wu-Yu Chen,Yaping Zhong,Gui‐Fang Huang,Wangyu Hu,Wei Hang
出处
期刊:Cornell University - arXiv
日期:2023-01-01
标识
DOI:10.48550/arxiv.2311.01654
摘要
Spin plays a key role in physical and chemical reactions, such as oxygen evolution and hydrogen evolution reactions (OER/HER); but the spin-activity correlation has remained unclear. Based on a transition metal (TM)-doped PtN2 monolayer model with a well-defined spin center as adsorption site, we here reveal that only active spin state can enhance the strength of hydrogen adsorption, while inert spin state offers very little influence. Specifically, the unpaired electron along the out-of-plane direction such as in dZ2 orbital, acting as an active spin state, will strongly hybridize with hydrogen, resulting in enhanced hydrogen binding energy because dZ2 orbital is just enough to accommodate two electrons to form a bonding orbital. While the in-plane unpaired electron such as in dX2-Y2 orbital, plays a negligible role in adsorbing hydrogen atom. This is verified by a series of single atom catalysts comprising of PtN2 monolayer by replacing Pt atom with a TM (Fe, Co, Ni, Ru, Rh, Pd, Os, or Ir) atom, or subsequent adsorbing a Cl atom. One of the most promising materials is Pd@PtN2-Cl that offers superior HER activity, even better than pure Pt. This work uncovers the nature of spin-activity correlation, thus paving the way for the design of high-performance catalysts through spin-engineering.
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