The first part of this thesis is concerned with the synthesis, characterisation and applications of surface functionalised carbon nanoparticles. Synthetic techniques are used to modify the existing surface architecture of carbon nanoparticles towards high surface area modified electrodes and pH sensing applications. Electrochemical and synthetic techniques have been used to study triple phase boundaries and enhance their properties towards a bulk synthetic technique, in which an electrolyte phase and redox probe phase are held separate. A salt matrix, ultrasound, high shear force and a carbon fibre membrane have all been used to form unique triple phase boundary environments in which electron and ion transfer processes can be studied and enhanced towards analytical and electrosynthetic applications. A number of electro-reduction reactions have been shown to be feasible using the triple phase boundary methodology. Alkenes, aldehydes and imines have all been successfully electro-reduced, analysed and optimised to elucidate the synthetic triple phase boundary mechanism.