Driving energetically unfavorable dehydrogenation dynamics with plasmonics

doi:10.1126/science.abd2847

GSTDTAP > 气候变化

DOI	10.1126/science.abd2847
	Driving energetically unfavorable dehydrogenation dynamics with plasmonics
	Katherine Sytwu; Michal Vadai; Fariah Hayee; Daniel K. Angell; Alan Dai; Jefferson Dixon; Jennifer A. Dionne
	2021-01-15
发表期刊	Science
出版年	2021
英文摘要	Optical excitation of localized surface plasmon resonances can confine light and create electromagnetic (EM) “hotspots” that can increase catalytic reaction rates. Sytwu et al. show how optical excited plasmons can also control the location of the active site. A crossed-bar gold-palladium hydride (Au-PdH x ) plasmonic antenna-reactor system localized EM radiation away from the more reactive PdH x tips. Using in situ environmental transmission electron microscopy, the authors show that changing the illumination wavelength and intensity, along with the surrounding hydrogen gas pressure, could shift dehydrogenation away from the sharp PdH x nanorod tips to the flat middle faces. Science , this issue p. [280][1] Nanoparticle surface structure and geometry generally dictate where chemical transformations occur, with higher chemical activity at sites with lower activation energies. Here, we show how optical excitation of plasmons enables spatially modified phase transformations, activating otherwise energetically unfavorable sites. We have designed a crossed-bar Au-PdH x antenna-reactor system that localizes electromagnetic enhancement away from the innately reactive PdH x nanorod tips. Using optically coupled in situ environmental transmission electron microscopy, we track the dehydrogenation of individual antenna-reactor pairs with varying optical illumination intensity, wavelength, and hydrogen pressure. Our in situ experiments show that plasmons enable new catalytic sites, including dehydrogenation at the nanorod faces. Molecular dynamics simulations confirm that these new nucleation sites are energetically unfavorable in equilibrium and only accessible through tailored plasmonic excitation. [1]: /lookup/doi/10.1126/science.abd2847
领域	气候变化 ; 资源环境
URL	查看原文
引用统计
文献类型	期刊论文
条目标识符	http://119.78.100.173/C666/handle/2XK7JSWQ/311504
专题	气候变化资源环境科学
推荐引用方式 GB/T 7714	Katherine Sytwu,Michal Vadai,Fariah Hayee,et al. Driving energetically unfavorable dehydrogenation dynamics with plasmonics[J]. Science,2021.
APA	Katherine Sytwu.,Michal Vadai.,Fariah Hayee.,Daniel K. Angell.,Alan Dai.,...&Jennifer A. Dionne.(2021).Driving energetically unfavorable dehydrogenation dynamics with plasmonics.Science.
MLA	Katherine Sytwu,et al."Driving energetically unfavorable dehydrogenation dynamics with plasmonics".Science (2021).