Altarawneh Mohammednoor, Radny Marian W, Smith Phillip V, Mackie John C, Kennedy Eric M, Dlugogorski Bogdan Z, Soon Aloysius, Stampfl Catherine
School of Engineering, Process Safety and Environment Protection Group, The University of Newcastle, Callaghan, New South Wales 2308, Australia.
J Chem Phys. 2009 May 14;130(18):184505. doi: 10.1063/1.3123534.
First-principles density functional theory and a periodic-slab model have been employed to explore the adsorption of a two-chlorophenol molecule on a Cu(2)O(110) surface containing surface Cu-O bonds, namely, the Cu(2)O(110):CuO surface. The two-chlorophenol molecule is found to interact very weakly with the Cu(2)O(110):CuO surface, forming several vertical and flat orientations. These weakly bound states tend to result from interaction between the phenolic hydrogen and an oxygen surface atom. The formation of a two-chlorophenoxy moiety and an isolated hydrogen on the Cu(2)O(110):CuO surface from a vacuum two-chlorophenol molecule is determined to have an endothermicity of 8.2 kcal/mol (0.37 eV). The energy required to form a two-chlorophenoxy radical in the gas phase is also found to be much smaller when assisted by the Cu(2)O(110):CuO surface than direct breaking of the hydroxyl bond of a free two-chlorophenol molecule. The calculated binding energy of a two-chlorophenoxy radical adsorbed directly onto the Cu(2)O(110):CuO surface is -12.5 kcal/mol (0.54 eV). The Cu(2)O(110):CuO and Cu(100) surfaces are found to have similar energy barriers for forming a surface-bound two-chlorophenoxy moiety from the adsorption of a two-chlorophenol molecule.
第一性原理密度泛函理论和周期性平板模型已被用于研究二氯苯酚分子在含有表面Cu - O键的Cu₂O(110)表面(即Cu₂O(110):CuO表面)上的吸附。发现二氯苯酚分子与Cu₂O(110):CuO表面的相互作用非常弱,形成了几种垂直和平坦的取向。这些弱束缚态往往源于酚羟基氢与表面氧原子之间的相互作用。确定从真空中的二氯苯酚分子在Cu₂O(110):CuO表面形成二氯苯氧基部分和一个孤立氢的过程具有8.2千卡/摩尔(0.37电子伏特)的吸热性。还发现,在Cu₂O(110):CuO表面的辅助下,在气相中形成二氯苯氧基自由基所需的能量比直接断裂游离二氯苯酚分子的羟基键要小得多。计算得出直接吸附在Cu₂O(110):CuO表面的二氯苯氧基自由基的结合能为 - 12.5千卡/摩尔(0.54电子伏特)。发现Cu₂O(110):CuO和Cu(100)表面对于从二氯苯酚分子的吸附形成表面结合的二氯苯氧基部分具有相似的能垒。