Electrocatalysis density functional theory

Electrocatalysis and Catalyst Screening from Density Functional Theory Calculations... 

Rossmeisl J, Greeley J, Karlberg GS. Electrocatalysis and Catalyst Screening from Density Functional Theory Calculations. In Koper M, editor. Fuel cell catalysis a surface science approach. Hoboken, NJ Wiley-VCH 2009. Chapter 3. 

Fundamentals of ab initio calculations, including density functional theory (DFT) methods, help to understand several key aspects of fuel cell electrocatalysis at the molecular level. 

The recent impressive advances in the use of rigorous ab initio quantum chemical calculations in electrochemistry are described in a remarkable chapter by Marc Koper, one of the leading protagonists in this fascinating area. This lucid chapter is addressed to all electrochemists, including those with very little prior exposure to quantum chemistry, and demonstrates the usefulness of ab initio calculations, including density functional theory (DPI) methods, to understand several key aspects of fuel cell electrocatalysis at the molecular level. 

Figure 4.4 Trends in electrocatalysis relationships between experimentally measured specific activities for the ORR on PtsM surfaces in 0.1 M HCIO4 at 0.9 V and 333 K vs the d-band center position for (A) the Pt-skin and Pt-skeleton surfaces. Results for each alloy were collected from five independent RDE measurements and error range is expressed by the size of circles. (B) Activities and values for d-band center position predicted from (Density functional theory) calculations for (111) oriented skin surfaces. Reprinted from Science, 315,493 (2007), Vojislav R. Stamenkovic., Improved oxygen reduction activity on Pt3Ni(lll) via increased surface site availability, 493—497, 2007, with permission from Sciencemag.

Much effort has been made to enhance the performance of Pd—M (where M = second metal) for alcohol electrooxidation. These efforts were persuaded by the bifunctional mechanism and the electronic/Ugand effect, which can be explained by either the electron density, electronegativity, density functional theory, or d-band theory [6-17]. For example, according to the bifunctional theory of electrocatalysis, the oxidation of a primary alcohol to CO2 and R-COOH (or and R-COO in... 

Chapters 7-12 focus on the electrocatalysis of carbon-based non-precious metal catalysts. The unique properties and fuel cell applications of various carbon based catalysts are intensively discussed in these chapters. Chapter 7 summarizes the fundamental studies on the electrocatalytic properties of metallomacrocyclic and other non-macrocyclic complexes. Chapter 8 and 9 review the progress made in the past 5 years of pyrolyzed carbon-supported nitrogen-coordinated transition metal complexes. Chapter 10 gives a comprehensive discussion on the role of transitional metals in the ORR electrocatalysts in acidic medium. Chapter 11 introduces modeling tools such as density functional theory (DPT) and ah initio molecular dynamics (AIMD) simulation for chemical reaction studies. It also presents a theoretical point of view of the ORR mechanisms on Pt-based catalysts, non-Pt metal catalysts, and non-precious metal catalysts. Chapter 12 presents an overview on recent progresses in the development of carbon-based metal-free ORR electrocatalysts, as well as the correlation between catalyst structure and their activities. 

Density Functional Theory Methods for Electrocatalysis Table 3.1... 

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