Lee Seul-Yi, Lee Jong-Hoon, Kim Yeong-Hun, Mahajan Roop L, Park Soo-Jin
Department of Chemistry, Inha University, Incheon 22212, South Korea.
Department of Mechanical Engineering and Institute for Critical Technology and Applied Science, Virginia Tech, Blacksburg, VA 24061, United States.
J Colloid Interface Sci. 2022 Dec 15;628(Pt A):758-768. doi: 10.1016/j.jcis.2022.07.183. Epub 2022 Aug 1.
Graphene is of great interest for many far-reaching applications that involve interparticle interactions in adsorbents, coatings, and composites. A deep understanding of the surface components has been crucial but achieving the most accurate and reliable values of these, unaffected by experimental conditions or the analytical techniques used, remains a major challenge. To this end, we have proposed in this paper a novel approach for the first time, to the best of our knowledge, to determine London dispersive and specific (polar) components including the Lewis acid-base character of the surface free energy of graphene materials (graphene oxide (GO), reduced graphene oxide (rGO), and graphite) using inverse gas chromatography (IGC) technique at an infinite dilution. We have estimated the London dispersive surface energy values of graphite, GO, and rGO as van der Waals interaction to be 156-179, 89-106, and 110-119 mJ m, respectively, in the temperature range of 320-360 K. These are attributable to the surface properties impacted by the oxygen moieties, defects, and micropores on the carbon frameworks. Further, the acceptor (K) and donor (K) parameters of GO were found to be 0.71 and 0.96, respectively, while those of rGO were 0.54 and 1.05. Notably, the GO is more of the Lewis acid character that could be amphoteric, while the Lewis base characteristics of both GO and rGO are not significantly changed. These results provide foundational knowledge to understand the physicochemical properties of graphene surfaces, which should be helpful to designing interface engineering in various applications.
石墨烯在许多具有深远意义的应用中备受关注,这些应用涉及吸附剂、涂层和复合材料中的粒子间相互作用。深入了解表面成分至关重要,但要获得不受实验条件或所用分析技术影响的最准确、最可靠的这些值,仍然是一项重大挑战。为此,据我们所知,本文首次提出了一种新颖的方法,使用无限稀释反相气相色谱(IGC)技术来确定石墨烯材料(氧化石墨烯(GO)、还原氧化石墨烯(rGO)和石墨)表面自由能的伦敦色散和特定(极性)成分,包括其路易斯酸碱特性。我们估计在320 - 360 K的温度范围内,作为范德华相互作用的石墨、GO和rGO的伦敦色散表面能值分别为156 - 179、89 - 106和110 - 119 mJ/m²。这些归因于碳骨架上的氧部分、缺陷和微孔对表面性质的影响。此外,发现GO的受体(K)和供体(K)参数分别为0.71和0.96,而rGO的分别为0.54和1.05。值得注意的是,GO更具有可能是两性的路易斯酸特性,而GO和rGO的路易斯碱特性没有明显变化。这些结果为理解石墨烯表面的物理化学性质提供了基础知识,这应该有助于设计各种应用中的界面工程。