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Endothermic reaction at room temperature enabled by deep-ultraviolet plasmons
Nature Materials ( IF 41.2 ) Pub Date : 2020-11-02 , DOI: 10.1038/s41563-020-00851-x
Canhui Wang 1, 2 , Wei-Chang D Yang 1, 2 , David Raciti 3 , Alina Bruma 1, 2 , Ronald Marx 4 , Amit Agrawal 1, 2 , Renu Sharma 1
Affiliation  

Metallic nanoparticles have been used to harvest energy from a light source and transfer it to adsorbed gas molecules, which results in a reduced chemical reaction temperature. However, most reported reactions, such as ethylene epoxidation, ammonia decomposition and H–D bond formation are exothermic, and only H–D bond formation has been achieved at room temperature. These reactions require low activation energies (<2 eV), which are readily attained using visible-frequency localized surface plasmons (from ~1.75 eV to ~3.1 eV). Here, we show that endothermic reactions that require higher activation energy (>3.1 eV) can be initiated at room temperature by using localized surface plasmons in the deep-UV range. As an example, by leveraging simultaneous excitation of multiple localized surface plasmon modes of Al nanoparticles by using high-energy electrons, we initiate the reduction of CO2 to CO by carbon at room temperature. We employ an environmental transmission electron microscope to excite and characterize Al localized surface plasmon resonances, and simultaneously measure the spatial distribution of carbon gasification near the nanoparticles in a CO2 environment. This approach opens a path towards exploring other industrially relevant chemical processes that are initiated by plasmonic fields at room temperature.



中文翻译:

深紫外等离子体使室温下的吸热反应成为可能

金属纳米粒子已被用于从光源收集能量并将其转移到吸附的气体分子,从而降低化学反应温度。然而,大多数报道的反应,如乙烯环氧化、氨分解和 H-D 键的形成都是放热的,并且在室温下仅实现了 H-D 键的形成。这些反应需要低活化能 (<2 eV),使用可见光频率局部表面等离子体激元 (从 ~1.75 eV 到 ~​​3.1 eV) 很容易实现。在这里,我们展示了需要更高活化能 (>3.1 eV) 的吸热反应可以在室温下通过使用深紫外范围内的局部表面等离子体激元启动。举个例子,2在室温下由碳转化为 CO。我们采用环境透射电子显微镜来激发和表征 Al 局部表面等离子体共振,同时测量 CO 2环境中纳米颗粒附近碳气化的空间分布。这种方法为探索在室温下由等离子体场引发的其他工业相关化学过程开辟了道路。

更新日期:2020-11-02
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