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利用铝铱天线-反应器纳米颗粒将一氧化二氮等离子体光催化转化为氮和氧

Plasmonic Photocatalysis of Nitrous Oxide into N and O Using Aluminum-Iridium Antenna-Reactor Nanoparticles.

作者信息

Swearer Dayne F, Robatjazi Hossein, Martirez John Mark P, Zhang Ming, Zhou Linan, Carter Emily A, Nordlander Peter, Halas Naomi J

出版信息

ACS Nano. 2019 Jul 23;13(7):8076-8086. doi: 10.1021/acsnano.9b02924. Epub 2019 Jun 24.

Abstract

Photocatalysis with optically active "plasmonic" nanoparticles is a growing field in heterogeneous catalysis, with the potential for substantially increasing efficiencies and selectivities of chemical reactions. Here, the decomposition of nitrous oxide (NO), a potent anthropogenic greenhouse gas, on illuminated aluminum-iridium (Al-Ir) antenna-reactor plasmonic photocatalysts is reported. Under resonant illumination conditions, N and O are the only observable decomposition products, avoiding the problematic generation of NO species observed using other approaches. Because no appreciable change to the apparent activation energy was observed under illumination, the primary reaction enhancement mechanism for Al-Ir is likely due to photothermal heating rather than plasmon-induced hot-carrier contributions. This light-based approach can induce autocatalysis for rapid NO conversion, a process with highly promising potential for applications in NO abatement technologies, satellite propulsion, or emergency life-support systems in space stations and submarines.

摘要

利用具有光学活性的“等离子体”纳米颗粒进行光催化是多相催化中一个不断发展的领域,具有大幅提高化学反应效率和选择性的潜力。在此,报道了在光照下的铝铱(Al-Ir)天线-反应器等离子体光催化剂上,强效人为温室气体一氧化二氮(N₂O)的分解情况。在共振光照条件下,氮(N)和氧(O)是仅可观察到的分解产物,避免了使用其他方法时出现的有问题的氮氧化物生成。由于在光照下未观察到表观活化能有明显变化,Al-Ir的主要反应增强机制可能是由于光热加热而非等离子体诱导的热载流子贡献。这种基于光的方法可诱导自催化以实现快速的N₂O转化,该过程在N₂O减排技术、卫星推进或空间站及潜艇的应急生命支持系统中的应用具有极具前景的潜力。

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