TY - JOUR
T1 - The adsorption and activation of oxygen molecular on nickel clusters doped graphene-based support by DFT
AU - Gao, Zhengyang
AU - Li, Ang
AU - Li, X.
AU - Liu, Xiaoshuo
AU - Ma, Chuanzhi
AU - Yang, Jianmeng
AU - Yang, Weijie
AU - Li, Hao
N1 - Funding Information:
This work was supported by the Beijing Municipal Natural Science Foundation ( 2182066 ), the Natural Science Foundation of Hebei Province of China ( B2018502067 ) and the Fundamental Research Funds for the Central Universities ( JB2015RCY03 and 2017XS121 ). This work was carried out at LvLiang Cloud Computing Center of China, and the calculations were performed on TianHe-2.
Publisher Copyright:
© 2019
PY - 2019/10
Y1 - 2019/10
N2 - The catalytic activation of O2 on nickel nanoclusters doped upon diff; erent functionalized graphene substrates (monovacancy as well as one, two and three pyridinic nitrogen decorated) was investigated through the density functional theory calculation. We can observed the adsorption characteristics and the catalytic activation of O2 on catalysts is related to the support effect of diff; erent functionalized graphene supports. The charge of Ni aotms has a good correlation with the adsorption energy of O2 on Nin clusters with different graphene-based support. The electron mainly transferred from the Ni clusters to the O2, and the graphene-based substrates plays a minor role in the electron transfer process. In addition, the Transition State Scaling are suitable for O2 dissociation reaction, and Transition State Scaling verify the accuracy of the O2 dissociation reaction calculation. Furthermore, in accordance with the energy barrier and the thermodynamic analysis of O2 activation reaction, the Ni3 clusters catalyst anchored single vacancy graphene decorated with three nitrogen atoms may be the most promising catalyst for O2 activation reaction. At the same time, this research will cast insight into activation reaction mechanism of O2 on metal nanoclusters catalysts and lay the foundation for the investigation of metal nanoclusters catalysts for the activation reaction of O2.
AB - The catalytic activation of O2 on nickel nanoclusters doped upon diff; erent functionalized graphene substrates (monovacancy as well as one, two and three pyridinic nitrogen decorated) was investigated through the density functional theory calculation. We can observed the adsorption characteristics and the catalytic activation of O2 on catalysts is related to the support effect of diff; erent functionalized graphene supports. The charge of Ni aotms has a good correlation with the adsorption energy of O2 on Nin clusters with different graphene-based support. The electron mainly transferred from the Ni clusters to the O2, and the graphene-based substrates plays a minor role in the electron transfer process. In addition, the Transition State Scaling are suitable for O2 dissociation reaction, and Transition State Scaling verify the accuracy of the O2 dissociation reaction calculation. Furthermore, in accordance with the energy barrier and the thermodynamic analysis of O2 activation reaction, the Ni3 clusters catalyst anchored single vacancy graphene decorated with three nitrogen atoms may be the most promising catalyst for O2 activation reaction. At the same time, this research will cast insight into activation reaction mechanism of O2 on metal nanoclusters catalysts and lay the foundation for the investigation of metal nanoclusters catalysts for the activation reaction of O2.
KW - Adsorption characteristics
KW - Catalytic activation
KW - Density functional theory
KW - Nin nanoclusters
KW - Thermodynamic analysis
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U2 - 10.1016/j.mcat.2019.110547
DO - 10.1016/j.mcat.2019.110547
M3 - Article
AN - SCOPUS:85070218820
SN - 2468-8231
VL - 477
JO - Molecular Catalysis
JF - Molecular Catalysis
M1 - 110547
ER -