Major Successes of Theory-and-Experiment-Combined Studies in Surface Chemistry and Heterogeneous Catalysis

Abstract

Experimental discoveries followed by theoretical interpretations that pave the way of further advances by experimentalists is a developing pattern in modern surface chemistry and catalysis. The revolution of modern surface science started with the development of surfacesensitive techniques such as LEED, XPS, AES, ISS and SIMS, in which the close collaboration between experimentalists and theorists led to the quantitative determination of surface structure and composition. The experimental discovery of the chemical activity of surface defects and the trends in the reactivity of transitional metals followed by the explanations from the theoretical studies led to the molecular level understanding of active sites in catalysis. The molecular level knowledge, in turn, provided a guide for experiments to search for new generation of catalysts. These and many other examples of successes in experiment-and-theory-combined studies demonstrate the importance of the collaboration between experimentalists and theorists in the development of modern surface science.

Impact of surface chemistry

“…A recent trend in surface chemistry is to study surface reactions at the molecular level under conditions close to those of the real applications by using experimental techniques combined with theoretical simulations (134). This type of research highlights the importance of developing new in situ techniques and is expected to directly aid in the rational design of surface properties for technological applications (135).…”

Crossing the divide between homogeneous and heterogeneous catalysis in water oxidation

“…Phosphonate-derivatized catalysts and molecular assemblies provide a basis for sustained water oxidation on these surfaces in acidic solution but are unstable toward hydrolysis and loss from surfaces as the pH is increased. Here, we report enhanced surface binding stability of a phosphonate-derivatized water oxidation catalyst over a wide pH range (1)(2)(3)(4)(5)(6)(7)(8)(9)(10)(11)(12) by atomic layer deposition of an overlayer of TiO 2 . Increased stability of surface binding, and the reactivity of the bound catalyst, provides a hybrid approach to heterogeneous catalysis combining the advantages of systematic modifications possible by chemical synthesis with heterogeneous reactivity.…”

“…Examples include the Haber-Bosch process, steam reforming, Ziegler-Natta polymerization, and hydrocarbon cracking (1)(2)(3)(4)(5)(6)(7)(8). Research in heterogeneous catalysis continues to flourish (9-15) but iterative design and modification are restricted by limitations in materials preparation and experimental access to surface mechanisms.…”

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.…”