For a sustainable future we need energy- and resource-efficient catalytic processes that can be controlled externally and use catalysts made of earth-abundant elements. Binary inorganic materials, such as transition metal phosphides and chalcogenides, have shown great promise to replace noble metal catalysts in some areas, but catalysis has not been broadly explored. The goal is to develop customizable catalysis by abundant inorganic materials for complex chemistry and added-value chemical products through a fundamental understanding of their interfacial chemistry. Electric fields could provide an external control on catalysis that is complementary to the more common temperature and pressure controls used in chemical industry. Electrostatic effects, such as electric fields are thought to be a major contributor to enzymatic catalysis, but have not been broadly explored in chemical synthesis. Herein, we will probe electric fields as external controls on catalysis of reductive and oxidative transformations by abundant materials using electrochemical methods and in-situ surface-enhanced infrared absorption spectroscopy. These studies will be supported by elucidation of the structure, thermochemistry, and elementary reactivity of the operative surfaces and the fine-tuning of their catalytic properties by chemical tailoring. Together, these strategies could open up great opportunities for the technological application of binary materials in sustainable chemical processes and for chemical synthesis.