期刊
SCIENCE
卷 371, 期 6526, 页码 280-+出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.abd2847
关键词
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资金
- SLAC National Accelerator Laboratory
- National Science Foundation's Alan T. Waterman Award
- U.S. Department of Energy, Office of Science, Division of Materials Science and Engineering [DE-AC02-76SF00515]
- National Science Foundation [ECCS-1542152]
- Gabilan Stanford Graduate Fellowship
- National Science Foundation Graduate Research Fellowship [DGE-1656518]
- TomKat Center for Sustainable Energy at Stanford University
- Diversifying Academia, Recruiting Excellence (DARE) Doctoral Fellowship Program by Stanford University
- Department of Energy Photonics at Thermodynamic Limits Energy Frontier Research Center [DE-SC0019140]
The study demonstrates how optical excitation of plasmons enables spatially modified phase transformations, activating energetically unfavorable sites and forming new catalytic sites on nanorod faces.
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-PdHx antenna-reactor system that localizes electromagnetic enhancement away from the innately reactive PdHx 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.
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