The development of new catalysts for oxidation reactions is of central importance for many industrial processes. Plasmonic catalysis involves photoexcitation of templates/chips to drive and enhance oxidation of target molecules. Raman-based sensing of target molecules can also be enhanced by these templates. This provides motivation for the rational design, characterization, and experimental demonstration of effective template nanostructures. In this paper, we report on a template comprising silver nanoparticles on aligned peptide nanotubes, contacted with a microfabricated chip in a dry environment. Efficient plasmonic catalysis for oxidation of molecules such as p-aminothiophenol results from facile trans-template charge transfer, activated and controlled by application of an electric field. Raman detection of biomolecules such as glucose and nucleobases are also dramatically enhanced by the template. A reduced quantum mechanical model is formulated, comprising a minimum description of key components. Calculated nanotube-metal-molecule charge transfer is used to understand the catalytic mechanism and shows this system is well-optimized.