等离子体活化水的异位制备用于高效灭菌：高价态NOx的关键作用与新化学路径
Off-site production of plasma-activated water for efficient sterilization: the crucial role of high-valence NOx and new chemical pathways
AI总结：
本文提出通过混合等离子体产生富含高价态NOx的气体并异位制备等离子体活化水，揭示气态NO3自由基诱导的短寿命水相物种和N2O5诱导的酸性环境在灭菌中的关键作用，并开发出产量2 L/h、杀菌效率>99.9%的集成装置。
摘要：
以更清洁的方法高效灭活病原体是环境消毒和临床抗感染治疗中的关键问题。等离子体活化水（PAW）因其强大的灭菌能力且不引起任何急性毒性，在生产过程中仅消耗水和空气，被认为是化学消毒剂和抗生素的有前景替代方案。为了实现更高效的水活化，等离子体源通常被尽可能靠近或完全接触水面放置，但电极腐蚀和金属污染水体的风险威胁着PAW生产的安全性和稳定性。本文中，通过混合等离子体构型产生富含高价态NOx的等离子体活化气体，并将其引入水中以实现PAW的异位生产。研究发现，等离子体产生的O3在气相反应中对高价态NOx的形成起主导作用。随着O3浓度的时间演化，气态NO3自由基在N2O5形成之后产生，但会在N2O5淬灭之前分解。通过解耦气态NO3、N2O5和O3在水活化中的作用，结果表明，由气态NO3自由基诱导的短寿命水相物种在PAW灭菌中发挥最关键的作用，而N2O5诱导的酸性环境同样必不可少。此外，SEM照片和生物大分子泄漏实验证明，PAW通过破坏细菌的细胞膜来实现灭活。在实际应用中，开发了一种用于异位PAW生产的集成装置，产量为2 L/h，杀菌效率>99.9%。使用该装置在3分钟内产生的50 mL PAW在相同细菌接触时间下，其消毒效果优于0.5% NaClO和3% H2O2。这项工作为高效PAW生产提供了新途径，并加深了对PAW灭菌中控制活性化学基本过程的理解。
英文摘要：
Efficient sterilization of pathogens with cleaner methods is a critical concern for environmental disinfection and clinical anti-infective treatment. Plasma-activated water (PAW) is a promising alternative to chemical disinfectants and antibiotics for its strong sterilization ability and not inducing any acute toxicity, and only water and air are consumed during production. For more efficient water activation, plasma sources are commonly placed near or fully in contact with water as possible, but the risks of electrode corrosion and metal contamination of water threaten the safety and stability of PAW production. Herein, plasma-activated gas rich in high-valence NOx is generated by a hybrid plasma configuration and introduced into water for off-site PAW production. Plasma-generated O3 is found to dominate the gas-phase reactions for the formation of high-valence NOx. With the time-evolution of O3 concentration, gaseous NO3 radicals are produced behind N2O5 formation, but will be decomposed before N2O5 quenching. By decoupling the roles of gaseous NO3, N2O5, and O3 in the water activation, results show that short-lived aqueous species induced by gaseous NO3 radicals play the most crucial role in PAW sterilization, and the acidic environment induced by N2O5 is also essential. Moreover, SEM photographs and biomacromolecule leakage assays demonstrate that PAW disrupts the cell membranes of bacteria to achieve inactivation. In real-life applications, an integrated device for off-site PAW production with a yield of 2 L/h and a bactericidal efficiency of >99.9% is developed. The PAW of 50mL produced in 3 minutes using this device is more effective in disinfection than 0.5% NaClO and 3% H2O2 with the same bacterial contact time. This work provides new avenues for efficient PAW production and deepens insights into the fundamental processes that govern the reactive chemistry in PAW sterilization.
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