Zhang Yan, Zhang Hong, Chen Tao, An Libao
College of Mechanical Engineering, North China University of Science and Technology, Tangshan, 063210, China.
College of Life Sciences, North China University of Science and Technology, Tangshan, 063210, China.
J Mol Model. 2023 Aug 23;29(9):289. doi: 10.1007/s00894-023-05694-2.
The co-adsorption of sulfate and metal ions on intrinsic and Al-doped graphene is investigated through first principles calculations. When SO ions exist only, both of intrinsic and Al-doped graphene can form stable adsorption configurations with SO. However, the presence of Cu/Ca/Zn/Mg ions attenuates the interaction between intrinsic graphene and SO, resulting in weak physical adsorption between them, while Al-doped graphene can still constitute co-adsorption chemically with both SO and Cu/Ca/Zn/Mg ions simultaneously. The sensitivity of Al-doped graphene towards co-adsorbed ions is in the order of SO-Cu > SO-Zn > SO-Ca > SO-Mg. The research indicates Al-doped graphene could be a promising material for sensing sulfate ions under the presence of various metal ions.
All of the calculations were carried out by using a first principles method based on density functional theory (DFT). The generalized gradient approximation (GGA) with the Perdew-Burke-Ernzerhof (PBE) functional was selected to describe electron exchange-correlation energy. The double numerical plus polarization (DNP) was employed as the basis set. The conductor-like screening model (COSMO) was implemented to simulate the aqueous solvent effect.
通过第一性原理计算研究了硫酸根离子和金属离子在本征石墨烯和铝掺杂石墨烯上的共吸附情况。当仅存在硫酸根离子时，本征石墨烯和铝掺杂石墨烯都能与硫酸根形成稳定的吸附构型。然而，铜/钙/锌/镁离子的存在减弱了本征石墨烯与硫酸根之间的相互作用，导致它们之间形成弱物理吸附，而铝掺杂石墨烯仍能与硫酸根和铜/钙/锌/镁离子同时形成化学共吸附。铝掺杂石墨烯对共吸附离子的敏感度顺序为硫酸根-铜＞硫酸根-锌＞硫酸根-钙＞硫酸根-镁。该研究表明，铝掺杂石墨烯可能是一种在各种金属离子存在下用于检测硫酸根离子的有前景的材料。
所有计算均采用基于密度泛函理论（DFT）的第一性原理方法进行。选择采用佩德韦-伯克-恩泽霍夫（PBE）泛函的广义梯度近似（GGA）来描述电子交换关联能。采用双数值加极化（DNP）基组。采用类导体屏蔽模型（COSMO）来模拟水溶剂效应。
