Recent advances in the understanding of structural and electronic effects in heterogeneous electrocatalysis are summarized. Typical examples are given illustrating how the knowledge obtained from a detailed theoretical analysis of structural and electronic effects supported by model experiments can be used for the rational design of new electrocatalytic materials. Recent successes and future challenges in designing active, stable, and selective electrocatalysts are discussed. (C) 2013 Elsevier Inc. All rights reserved.