Abstract：
Plasmonic nanostructures have attracted increasing interest in the fields of photochemistry and photocatalysis for their ability to enhance reactivity and tune reaction selectivity, a benefit of their strong interactions with light and their multiple energy decay mechanisms. Here we introduce the use of earth-abundant plasmonic aluminum nanoparticles as a promising renewable detoxifier of the sulfur mustard simulant 2-chloroethylethylsulfide through gas phase photodecomposition. Analysis of the decomposition products indicates that C-S bond breaking is facilitated under illumination, while C-Cl breaking and HCl elimination are favored under thermocatalytic (dark) conditions. This difference in reaction pathways illuminates the potential of plasmonic nanoparticles to tailor reaction selectivity toward less hazardous products in the detoxification of chemical warfare agents. Moreover, the photocatalytic activity of the Al nanoparticles can be regenerated almost completely after the reaction concludes through a simple surface treatment.
摘要：
等离子体纳米结构因其增强反应性和调节反应选择性的能力而在光化学和光催化领域引起了越来越多的兴趣。它们与光的强烈相互作用以及它们的多种能量衰减机制的好处。在这里，我们介绍了通过气相光分解将地球丰富的等离子体铝纳米粒子用作硫芥子气模拟物2-氯乙基乙基硫化物的有前途的可再生解毒剂。对分解产物的分析表明，在光照下促进了C-S键的断裂，而C-Cl破坏和HCl消除在热催化（黑暗）条件下是有利的。反应途径的这种差异阐明了等离子体纳米颗粒在化学战剂解毒中对危害较小的产品定制反应选择性的潜力。此外，Al纳米颗粒的光催化活性可以在反应结束后通过简单的表面处理几乎完全再生。
