| 论文简介 |
The severe environmental problems and the demand for energy urgently require electrocatalysis to
replace Haber-Bosch for the nitrogen reduction reaction (NRR). The descriptors and important properties
of single-atom and homonuclear double-atom catalysts have been preliminarily explored, but the relationship between the inherent properties and catalytic activity of heteronuclear double-atom catalysts
with better performance remains unclear. Therefore, it is very significant to explore the prediction
expressions of catalytic activity of heteronuclear double-atom catalysts based on their inherent properties and find the rule for selecting catalytic centers. Herein, by summarizing the free energy for the key
steps of NRR on 55 catalysts calculated through the first-principle, the expressions of predicting the free
energy and the corresponding descriptors are deduced by the machine learning, and the strategy for
selecting the appropriate catalytic center is proposed. The selection strategy for the central atom of
heteronuclear double-atom catalysts is that the atomic number of central B atom should be between
group VB and VIIIB, and the electron difference between central A atom and B atom should be large
enough, and the selectivity of NRR or hydrogen evolution reaction (HER) could be calculated through
the prediction formula. Moreover, five catalysts are screened to have low limiting potential and excellent
selectivity, and are further analyzed by electron transfer. This work explores the relationship between the
inherent properties of heteronuclear double-atom catalysts and the catalytic activity, and puts forward
the rules for selecting the heteronuclear double-atom catalytic center, which has guiding significance
for the experiment. |
(创新港)
