Clean Combustion Research Center (CCRC), Physical Science and Engineering (PSE) Division, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi Arabia.
J Phys Chem A. 2021 Apr 22;125(15):3177-3188. doi: 10.1021/acs.jpca.1c01650. Epub 2021 Apr 9.
Nicotine exposure results in health risks not only for smokers but also for second- and third-hand smokers. Unraveling nicotine's degradation mechanism and the harmful chemicals that are produced under different conditions is vital to assess exposure risks. We performed a theoretical study to describe the early chemistry of nicotine degradation by investigating two important reactions that nicotine can undergo: hydrogen abstraction by hydroxyl radicals and unimolecular dissociation. The former contributes to the control of the degradation mechanism below 800 K due to a non-Arrhenius kinetics, which implies an enhancement of reactivity as temperature decreases. The latter becomes important at higher temperatures due to its larger activation energy. This change in the degradation mechanism is expected to affect the composition of vapors inhaled by smokers and room occupants. Conventional cigarettes, which operate at temperatures higher than 1000 K, are more prone to yield harmful pyridinyl radicals via nicotine dissociation, while nicotine in electronic cigarettes and vaporizers, with operating temperatures below 600 K, will be more likely degraded by hydroxyl radicals, resulting in a vapor with a different composition. Although low-temperature nicotine delivery devices have been claimed to be less harmful due to their nonburning operating conditions, the non-Arrhenius kinetics that we observed for the degradation mechanism below 873 K suggests that nicotine degradation may be more rapidly initiated as temperature is reduced, indicating that these devices may be more harmful than it is commonly assumed.
尼古丁暴露不仅对吸烟者,而且对二手烟和三手烟者都存在健康风险。揭示尼古丁的降解机制以及不同条件下产生的有害化学物质对于评估暴露风险至关重要。我们通过研究尼古丁可能经历的两个重要反应:羟基自由基的氢提取和单分子离解,进行了理论研究以描述尼古丁的早期降解化学。前者由于非阿仑尼乌斯动力学,在 800 K 以下控制降解机制,这意味着随着温度降低反应性增强。后者由于其较大的活化能,在较高温度下变得重要。这种降解机制的变化预计会影响吸烟者和室内居住者吸入的蒸气的组成。传统香烟的操作温度高于 1000 K,通过尼古丁离解更容易产生有害的吡啶基自由基,而电子烟和蒸发器中的尼古丁,操作温度低于 600 K,更可能被羟基自由基降解,导致蒸气的组成不同。尽管声称低温尼古丁输送装置由于其非燃烧的操作条件而危害较小,但我们在 873 K 以下观察到的降解机制的非阿仑尼乌斯动力学表明,随着温度降低,尼古丁降解可能会更快地开始,这表明这些装置可能比通常认为的更有害。