| 引用本文格式: Zhang Ying,Liu Jia-Xi,Sun Zhi-Hai,Huang Qiang,Xia Yong-Peng,Li Bin,Zou Yong-Jin,Zhang Huan-Zhi,Huang Peng-Ru,Xu Fen,Sun Li-Xian. First-principles study on the electronic structure and hydrogen-adsorption properties of amorphous carbon monolayers [J]. J. At. Mol. Phys., 2022, 39: 041004 (in Chinese) [张颖,刘佳溪,孙志海,黄强,夏永鹏,李彬,邹勇进,张焕芝,黄鹏儒,徐芬,孙立贤. 无序碳单层的电子结构及氢原子吸附的第一性原理 [J]. 原子与分子物理学报, 2022, 39: 041004] |
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| 无序碳单层的电子结构及氢原子吸附的第一性原理 |
| First-principles study on the electronic structure and hydrogen-adsorption properties of amorphous carbon monolayers |
| 摘要点击 111 全文点击 12 投稿时间：2021-06-19 修订日期：2021-07-10 |
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| DOI编号
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| 中文关键词
第一性原理 无序碳 电子性质 氢原子吸附 析氢反应 |
| 英文关键词
First-principle calculations Amorphous carbon Electronic properties Hydrogen adsorption Hydrogen evolution reaction |
| 基金项目
国家自然科学基金 |
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| 中文摘要
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| 本研究运用第一性原理计算方法，系统地研究了无序碳单层材料不同位点的电子结构及其析氢性能。计算结果显示无序结构中的C-C键相比于石墨烯中的C-C键在26.7%的范围内有不同程度的拉伸或压缩，使得C原子电荷在-0.17~+0.16个电子范围内变化，导致部分C原子电子局域化。电子的局域化增强了C原子的化学活性，从而表现出了较强的吸附性能。通过对一些位点吸附H原子的研究，发现调节三配位碳原子的键角可以调控其对氢的吸附强度进而改变析氢性能。对于三配位的碳原子，其中三个价电子通过sp2杂化轨道与最邻近的碳原子结合形成较强的共价键，而余下的一个pz轨道电子可以与H原子在垂直于原子层的方向形成较弱的化学键。无序结构可以打破三个sp2杂化轨道的对称性，进而影响pz轨道与氢的成键。本研究在一定程度上揭示了二维无序碳材料结构-性能的构效关系，为实验上设计特定性能的无序碳功能材料提供理论指导。 |
| 英文摘要
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| First-principles calculations were performed to systematically study the electronic structure and hydrogen evolution properties of the amorphous carbon monolayers. Our results show that the C-C bonds in the disordered structure undergo different degrees of stretching or compression, in the range of 26.7%, comparing to a pristine graphene. The atomic charge of C atoms changed in the range of -0.17~+0.16 electrons, resulting in electron localization on some C atoms. The localization of electrons enhances the chemical activity of the C atoms and hence the adsorption to alien atoms. The bonding of H atom with C, and the hydrogen evolution performance was found to be correlated with the bond angles of the C atoms. For a triple-coordinate carbon atom, three valence electrons combine strongly with the nearest carbon atom through the sp2 hybridization and the remaining pz orbital electron being unbonded. This electron could bond with adsorbates with relatively weak bonding. We found that the adsorption strength of this bond could be modified by tuning the angles of C-C bonds. Our results could provide deep insight into the correlation of structures and properties of amorphous carbon monolayer. |
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