Following the microscopic pathway to adsorption through chemisorption and physisorption wells

doi:10.1126/science.abc9581

GSTDTAP > 气候变化

DOI	10.1126/science.abc9581
	Following the microscopic pathway to adsorption through chemisorption and physisorption wells
	Dmitriy Borodin; Igor Rahinov; Pranav R. Shirhatti; Meng Huang; Alexander Kandratsenka; Daniel J. Auerbach; Tianli Zhong; Hua Guo; Dirk Schwarzer; Theofanis N. Kitsopoulos; Alec M. Wodtke
	2020-09-18
发表期刊	Science
出版年	2020
英文摘要	Adsorption is an important initial step in all heterogeneous chemical processes. However, detailed adsorption dynamics are complex and challenging to follow experimentally. Using the fact that vibrationally excited carbon monoxide molecules can be trapped on the Au(111) surface with all degrees of freedom being equilibrated except the vibrational ones, Borodin et al. show that the vibrational relaxation time can serve as an internal clock to follow the microscopic pathways of adsorption and equilibration on the surface. On the basis of molecular beam experiments and theoretical modeling of this prototypical system, the authors reveal the intricate interplay between physisorption and chemisorption states. These observed characteristics are relevant to many other heterogeneous systems. Science , this issue p. [1461][1] Adsorption involves molecules colliding at the surface of a solid and losing their incidence energy by traversing a dynamical pathway to equilibrium. The interactions responsible for energy loss generally include both chemical bond formation (chemisorption) and nonbonding interactions (physisorption). In this work, we present experiments that revealed a quantitative energy landscape and the microscopic pathways underlying a molecule’s equilibration with a surface in a prototypical system: CO adsorption on Au(111). Although the minimum energy state was physisorbed, initial capture of the gas-phase molecule, dosed with an energetic molecular beam, was into a metastable chemisorption state. Subsequent thermal decay of the chemisorbed state led molecules to the physisorption minimum. We found, through detailed balance, that thermal adsorption into both binding states was important at all temperatures. [1]: /lookup/doi/10.1126/science.abc9581
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/295423
专题	气候变化资源环境科学
推荐引用方式 GB/T 7714	Dmitriy Borodin,Igor Rahinov,Pranav R. Shirhatti,et al. Following the microscopic pathway to adsorption through chemisorption and physisorption wells[J]. Science,2020.
APA	Dmitriy Borodin.,Igor Rahinov.,Pranav R. Shirhatti.,Meng Huang.,Alexander Kandratsenka.,...&Alec M. Wodtke.(2020).Following the microscopic pathway to adsorption through chemisorption and physisorption wells.Science.
MLA	Dmitriy Borodin,et al."Following the microscopic pathway to adsorption through chemisorption and physisorption wells".Science (2020).