Ab initio insights into the interaction mechanisms between boron, nitrogen and oxygen doped diamond surfaces and water molecules
Ab initio insights into the interaction mechanisms between boron, nitrogen and oxygen doped diamond surfaces and water molecules
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DOI：
10.1016/j.carbon.2020.09.044
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发表时间：
2021-01-01
期刊：
影响因子：
10.9
通讯作者：
Righi, M. C.
中科院分区：
文献类型：
--
作者：
Latorre, Carlos Ayestaran;Ewen, James P.;Righi, M. C.
金刚石和类金刚石碳涂层用于从生物医学到摩擦学的许多应用中。已经测试了各种各样的掺杂剂来改变这些表面的亲水性，因为这是它们在水性环境中的生物相容性和摩擦学性能的核心。尽管有大量的实验研究，不同的掺杂剂对碳膜的亲水性的影响仍然缺乏原子的理解。在这项研究中，我们采用从头计算来阐明B，N和O掺杂剂的影响，可以修改与水分子的相互作用，从而亲水性的几种机制。这些包括完整的水分子在表面上的吸附，水解离的最小能量途径，以及随后的氢化和羟基化表面与水分子的相互作用。我们发现，所有的掺杂剂考虑提高亲水性，但他们这样做，通过不同的手段。最值得注意的是，B掺杂剂可以自发地化学吸收B完整的水分子，并增加其在氢键网络中的相互作用。(C)2020由Elsevier Ltd.出版
Diamond and diamond-like carbon coatings are used in many applications ranging from biomedicine to tribology. A wide range of dopants have been tested to modify the hydrophilicity of these surfaces, since this is central to their biocompatibility and tribological performance in aqueous environments. Despite the large number of experimental investigations, an atomistic understanding of the effects of different dopants on carbon film hydrophilicity is still lacking. In this study, we employ ab initio calculations to elucidate the effects of B, N, and O dopants in several mechanisms that could modify interactions with water molecules and thus hydrophilicity. These include the adsorption of intact water molecules on the surfaces, minimum energy pathways for water dissociation, and subsequent interactions of hydrogenated and hydroxylated surfaces with water molecules. We find that all of the dopants considered enhance hydrophilicity, but they do so through different means. Most notably, B dopants can spontaneously chemisorb intact water molecules and increase its interactions in H-bond networks. (C) 2020 Published by Elsevier Ltd.