التفاصيل البيبلوغرافية
| العنوان: |
Spin Polarization-Induced Facile Dioxygen Activation in Boron-Doped Graphitic Carbon Nitride |
| المؤلفون: |
Xinrui Cao (1688581), Jiacai Shen (9626905), Xiao-Fei Li (671655), Yi Luo (143206) |
| سنة النشر: |
2020 |
| المجموعة: |
Smithsonian Institution: Digital Repository |
| مصطلحات موضوعية: |
Biophysics, Biochemistry, Medicine, Cell Biology, Immunology, Science Policy, Virology, Computational Biology, Environmental Sciences not elsewhere classified, Chemical Sciences not elsewhere classified, Physical Sciences not elsewhere classified, design g-C 3 N 4, doping concentration, graphitic carbon nitride, surface oxygen-containing groups, Boron-Doped Graphitic Carbon Nitrid., first-principles results show, O 2 activation, catalyst, O 2, Spin Polarization-Induced Facile Di., site, net-spin, oxidation reactions, g-C 3 N 4 |
| الوصف: |
Dioxygen (O 2 ) activation is a vital step in many oxidation reactions, and a graphitic carbon nitride (g-C 3 N 4 ) sheet is known as a famous semiconductor catalytic material. Here, we report that the atomic boron (B)-doped g-C 3 N 4 (B/g-C 3 N 4 ) can be used as a highly efficient catalyst for O 2 activation. Our first-principles results show that O 2 can be easily chemisorbed at the B site and thus can be highly activated, featured by an elongated O–O bond (∼1.52 Å). Interestingly, the O–O cleavage is almost barrier free at room temperatures, independent of the doping concentration. It is revealed that the B atom can induce considerable spin polarization on B/g-C 3 N 4 , which accounts for O 2 activation. The doping concentration determines the coupling configuration of net-spin and thus the magnitude of the magnetism. However, the distribution of net-spin at the active site is independent of the doping concentration, giving rise to the doping concentration-independent catalytic capacity. The unique monolayer geometry and the existing multiple active sites may facilitate the adsorption and activation of O 2 from two sides, and the newly generated surface oxygen-containing groups can catalyze the oxidation coupling of methane to ethane. The present findings pave a new way to design g-C 3 N 4 -based metal-free catalysts for oxidation reactions. |
| نوع الوثيقة: |
article in journal/newspaper |
| اللغة: |
unknown |
| Relation: |
https://figshare.com/articles/journal_contribution/Spin_Polarization-Induced_Facile_Dioxygen_Activation_in_Boron-Doped_Graphitic_Carbon_Nitride/13221049 |
| DOI: |
10.1021/acsami.0c16216.s001 |
| الاتاحة: |
https://doi.org/10.1021/acsami.0c16216.s001 |
| Rights: |
CC BY-NC 4.0 |
| رقم الانضمام: |
edsbas.FFC7075 |
| قاعدة البيانات: |
BASE |