1. Regular pattern of the single-atom M-N3/C (M = Sc ∼ Cu) toward the activation of O2
- Author
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Jin-Tao Gou, Ting-Hao Liu, Shuai Fu, Yin-Sheng Zhang, Wei Tai, Chang-Wei Hu, and Hua-Qing Yang
- Subjects
GGA-PBE/DNP ,Activation of O2 ,N-doped graphene ,First-row transition metal ,Chemistry ,QD1-999 - Abstract
The single-atom metal M-N-C catalyst displays a certain activity for the aerobic oxidation. A single-atom M-N3/C (M = Sc ∼ Cu) surface was modeled as a M-N-C catalyst, in which a metal adatom was located on a monovacancy defective nitrogen-doped graphene. Over M-N3/C (M = Sc ∼ Cu), the activation mechanism has been theoretically studied at the GGA-PBE/DNP level. The stability of M-N3/C increases as Cu < Mn < Fe = Ni < Cr < Co < Sc < V < Ti. Here, Ti-N3/C is the most favorable among the first-row transition metal (Sc ∼ Cu), whereas Co-N3/C is the most stable among the late first-row transition metal Mn ∼ Cu. For M-N3/C (M = Sc ∼ Cu), both the adsorption strength of O2 and the activity of O2 dissociation decrease sequentially with the increase of atomic number, i.e., Sc > Ti > V > Cr > Mn > Fe > Co > Ni > Cu, which have a negative correlation with either charge or the energy level difference (ɛd) for the center of the d-bands relative to the Fermi level of metal-site. Thermodynamically, the possibility for the dissociation of O2 decreases as Mn > Ti > Cu > Ni > Cr > V = Fe > Co > Sc.
- Published
- 2023
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