2017 Fiscal Year Research-status Report
Large range functionalization of h-BN monolayer by Carbon doping
| Project/Area Number |
17K14429
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| Research Institution | Hokkaido University |
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Principal Investigator |
高 敏 北海道大学, 大学院理学研究院, 助教 (40784202)
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| Project Period (FY) |
2017-04-01 – 2019-03-31
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| Keywords | h-BN / oxygen molecule / Carbon atoms / activation area |
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| Outline of Annual Research Achievements |
The activation and dissociation of molecular oxygen on two-dimensional (2D) surface is a topic of interests due to its wide industrial applications, such as oxidation of carbon dioxide, and oxygen reduction reaction (ORR) in fuel cells and many others. An ideal 2D surface for O2 activation should meet at least two conditions: (1) suitable adsorption energy to make sure the O2 can be activated and dissociate from surface after reaction. (2) large activation area to make sure reaction involving O2 can occur in high efficiency.Very recently, we found that C atom doping in the B position of h-BN (CB@h-BN) produces n-type semiconductor BN material with noticeable catalytic activity for O2 activation in the large area extended far away from the C impurity.
However, synthesis of one atom doped h-BN surface is still a challenge for experimentist. In the current plan, by using density functional theory, we tried to simulate multiple C atoms doped h-BN surface which is more close to the realistic ones. In this year, we clarified the factors controlling the catalytic activity, catalytic area of multiple C doped h-BN surface. Also, the concentration of C atoms from 10% to 50% are investigated. The catalytic activity of C atoms doped h-BN surface are also investigated.
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| Current Status of Research Progress |
Current Status of Research Progress
2: Research has progressed on the whole more than it was originally planned.
Reason
The research is on progress as planed, until now, we have found out the correlation between the number of doped C atoms and electronic structure of h-BN monolayer. From the investigation of small concatenation, the factors that influence the catalytic activity of C doped h-BN surface are determined. By considering these factors, it is much more efficient to investigate the concentration effect of C doped h-BN surfaces. The correlation between electronic structure and doped atom in h-BN surface has been clarified from the fundamental view. The factors that are responsible for the large activation area for oxygen activation has been elucidated. However, the spin multiplicity becomes complicated when the concentration, it is necessary to find out the influence factors. Also, the application of catalytic reactions should be done.
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| Strategy for Future Research Activity |
To apply the effective C atom doped h-BN surfaces to the typical reaction involving oxygen molecule. Although the adsorption activation of O2 in the reaction involving oxygen molecule is always the initial necessary step, it is not a sufficient condition to determine the catalytic properties of C doped h-BN surface. In this part, the h-BN surfaces with different C concentration will be considered for the following four reactions:
(i) O2+4H++4e -> H2O (ii) O2+CH3OH -> HCOOH
(iii) O2+2CO -> 2CO2 (iv) O2+2C2H4 -> 2C2H4O/2CH3COOH
All the possible reaction mechanism will be considered on the selected reaction sites. Similar to the investigation of oxygen molecule adsorption and activation, the effect of distance between doped C atoms and catalytic sites will be investigated. The reaction mechanism, energy profiles and reaction rate constant will be studied. The energy barrier will be compared to ones of the reported best catalyst for each reaction. It shows an extremely promising direction in the process of searching and designing a new catalyst material, through the combination of theoretical calculation and experiment. Finally, after a clearly understanding of the property of single type hetero-atom doped h-BN surface, the theoretical investigation of dual-atom doped h-BN surface will also be able to be studied.
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