Concepts, instruments, and model systems that enabled the rapid evolution of surface science

Abstract

Over the past forty years, surface science has evolved to become both an atomic scale and a molecular scale science. Gerhard Ertl's group has made major contributions in the field of molecular scale surface science, focusing on vacuum studies of adsorption chemistry on single crystal surfaces. In this review, we outline three important aspects that led to the recent advances of surface chemistry: the development of concepts, in situ instruments for molecular scale surface studies at buried interfaces (solid-gas and solidliquid), and new model nanoparticle surface systems in addition to single crystals.Combined molecular beam surface scattering and low energy electron diffraction (LEED)-surface structure studies on metal single crystal surfaces revealed new concepts, including adsorbate-induced surface restructuring and the unique activity of defects, atomic steps and kinks on metal surfaces. We have combined high pressure catalytic reaction studies with ultrahigh vacuum (UHV) surface characterization techniques using the UHV chamber equipped with a high-pressure reaction cell. New instruments, such as high pressure sum frequency generation (SFG) vibrational spectroscopy and scanning tunneling microscopy (STM) have been built that permit molecular-level surface studies performed at pressures. Tools that can access broad ranges of pressures can be used for both the in situ characterization of buried interfaces of solid-gas and solid-liquid and the study of catalytic reaction intermediates. The model systems for the study of molecular 2 surface chemistry have evolved from single crystals to nanoparticles in the 1-10 nm size range, which are the preferred media in catalytic reaction studies.

Understanding Trends in Catalytic Activity: The Effect of Adsorbate–Adsorbate Interactions for CO Oxidation Over Transition Metals

“…In the present case we obtained all energies from periodic density functional theory (DFT) calculations [53][54][55][56][57]. 1 The integral binding energy E int and the differential binding energy E diff can be obtained from E avg as given by Eqs. 2 and 3.…”

“…Surface science experiments have provided a beautiful set of data on very well characterized systems [1][2][3] for these calculations to benchmark against. By combining theory and experiment it is now possible to describe elementary reactions on metal surfaces at the molecular level [4][5][6][7][8][9][10][11][12][13][14].…”

Impact of surface chemistry

“…It took almost 50 y for surface chemistry to develop into a molecular-level science, which is now capable of in situ characterization of a variety of surface properties and providing fundamental understanding to aid in the design and engineering of large-scale chemical processes in technological applications (90,91).…”

Exploring Zeolite Chemistry with the Tools of Surface Science: Challenges, Opportunities, and Limitations

“…The surface science community, in work pioneered by the groups of Somorjai and Ertl, [1][2][3][4] has successfully used simplified versions of industrial catalysts to provide insights on structure-reactivity relationships. By using so called "model" catalysts, the complexity of the catalyst can be reduced in order to disentangle structural, chemical and electronic effects in the reactions and elucidate reaction mechanisms.…”