Middleton James R, Ghadiri Mojtaba, Scott Andrew J
School of Chemical and Process Engineering, University of Leeds, Leeds LS2 9JT, UK.
Pharmaceutics. 2024 Mar 21;16(3):433. doi: 10.3390/pharmaceutics16030433.
Triboelectrification is a ubiquitous and poorly understood phenomenon in powder processing, particularly for pharmaceutical powders. Charged particles can adhere to vessel walls, causing sheeting; they can also cause agglomeration, threatening the stability of powder formulations, and in extreme cases electrostatic discharges, which present a serious fire and explosion hazard. Triboelectrification is highly sensitive to environmental and material conditions, which makes it very difficult to compare experimental results from different publications. In this work, density functional theory (DFT) is used to investigate the charge transfer characteristics of several functional groups of paracetamol in order to better understand the mechanisms of charging at the nanoscale and the influence of the environmental and material properties on charge transfer. This is achieved by studying the structure and electronic properties at the molecule-substrate interface. Using this molecule-substrate approach, the charging contributions of individual functional groups are explored by examining the Hirschfeld charges, the charge density difference between the molecule and substrate, the density of states, and the location of the frontier orbitals (HOMO and LUMO) of a paracetamol molecule. Charge density difference calculations indicate a significant transfer of charge from the molecule to the surface. Observable regions of electron density enrichment and depletion are evident around the electron-donating and -withdrawing groups, respectively. The density of states for the paracetamol molecule evolves as it approaches the surface, and the band gap disappears upon contact with the substrate. Hirshfeld charge analysis reveals asymmetry in the charge redistribution around the molecule, highlighting the varying charging tendencies of different atoms.
摩擦起电是粉末加工过程中一种普遍存在但却了解甚少的现象,在药物粉末方面尤为如此。带电粒子会附着在容器壁上,导致成片现象;它们还会引起团聚,威胁粉末制剂的稳定性,在极端情况下会产生静电放电,带来严重的火灾和爆炸危险。摩擦起电对环境和材料条件高度敏感,这使得比较不同出版物中的实验结果非常困难。在这项工作中,采用密度泛函理论(DFT)来研究扑热息痛几个官能团的电荷转移特性,以便更好地理解纳米尺度下的充电机制以及环境和材料特性对电荷转移的影响。这是通过研究分子 - 底物界面处的结构和电子性质来实现的。利用这种分子 - 底物方法,通过检查Hirschfeld电荷、分子与底物之间的电荷密度差、态密度以及扑热息痛分子的前沿轨道(HOMO和LUMO)位置,探索各个官能团的充电贡献。电荷密度差计算表明电荷从分子向表面有显著转移。在供电子基团和吸电子基团周围分别明显存在电子密度富集和耗尽的可观察区域。扑热息痛分子的态密度在其接近表面时会发生变化,与底物接触时带隙消失。Hirshfeld电荷分析揭示了分子周围电荷重新分布的不对称性,突出了不同原子不同的充电倾向。