Resolving multifrequential oscillations and nanoscale interfacet communication in single-particle catalysis

doi:10.1126/science.abf8107

GSTDTAP > 气候变化

DOI	10.1126/science.abf8107
	Resolving multifrequential oscillations and nanoscale interfacet communication in single-particle catalysis
	Y. Suchorski; J. Zeininger; S. Buhr; M. Raab; M. Stöger-Pollach; J. Bernardi; H. Grönbeck; G. Rupprechter
	2021-06-18
发表期刊	Science
出版年	2021
英文摘要	Metal nanoparticles used in heterogeneous catalysis can bear different facets with different reaction kinetics. Suchorski et al. used field electron microscopy with high spatial (∼2 nanometers) and time (∼2 milliseconds) resolution to study hydrogen oxidation on a curved rhodium crystal that displayed individual nanofacets. They also performed field ion microscopy of the water products. Periodic formation and depletion of subsurface oxygen blocked or allowed hydrogen adsorption, respectively, and led to oscillatory kinetics that could frequency lock between facets but at different frequencies. Surface reconstructions could also induce collapse of spatial coupling of oscillations. Science , abf8107, this issue p. [1314][1] In heterogeneous catalysis research, the reactivity of individual nanofacets of single particles is typically not resolved. We applied in situ field electron microscopy to the apex of a curved rhodium crystal (radius of 650 nanometers), providing high spatial (~2 nanometers) and time resolution (~2 milliseconds) of oscillatory catalytic hydrogen oxidation, to image adsorbed species and reaction fronts on the individual facets. Using ionized water as the imaging species, the active sites were directly imaged with field ion microscopy. The catalytic behavior of differently structured nanofacets and the extent of coupling between them were monitored individually. We observed limited interfacet coupling, entrainment, frequency locking, and reconstruction-induced collapse of spatial coupling. The experimental results are backed up by microkinetic modeling of time-dependent oxygen species coverages and oscillation frequencies. [1]: /lookup/doi/10.1126/science.abf8107
领域	气候变化 ; 资源环境
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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/330808
专题	气候变化资源环境科学
推荐引用方式 GB/T 7714	Y. Suchorski,J. Zeininger,S. Buhr,et al. Resolving multifrequential oscillations and nanoscale interfacet communication in single-particle catalysis[J]. Science,2021.
APA	Y. Suchorski.,J. Zeininger.,S. Buhr.,M. Raab.,M. Stöger-Pollach.,...&G. Rupprechter.(2021).Resolving multifrequential oscillations and nanoscale interfacet communication in single-particle catalysis.Science.
MLA	Y. Suchorski,et al."Resolving multifrequential oscillations and nanoscale interfacet communication in single-particle catalysis".Science (2021).