Electrochemical Hydrogen Peroxide Production Via Oxygen Reduction Reaction

Abstract

Hydrogen peroxide (H2O2) is a valuable chemical with rapidly growing demand in a variety of applications. At present, industrial production of H2O2 is through an energy-intensive anthraquinone process with high production costs and environmental hazards. Recently, the reported noble-metal based catalysts such as Pd-Au alloy, using renewable electricity to generate H2O2 via two-electron transferred oxygen reduction reaction (2e–-ORR), has received much attention. However, the cost and abundance of noble metals limit such catalysts for large-scale applications. To reduce the high overpotential requirement and improve the low yield of such noble metal catalysts, developing cost-efficient catalysts with high H2O2 selectivity and activity is a challenge that must be addressed immediately. Therefore, it is of great importance to design and synthesize electrocatalysts with abundant high-performance active sites for electrochemical H2O2 synthesis. In this thesis, by using a combination of theoretical calculation and experiments, I have demonstrated some effective approaches to tune the H2O2 generation performance on a series of structure-defined systems, including columbites (MNb2O6, M = Mn, Fe, Co, Ni and Cu), a porphyrin-based covalent organic framework (COF-366-M, M = Mn, Fe, Co, Ni, Cu and Zn) and a heterogeneous molecular catalyst system (HMC). In acid, neutral or alkaline conditions, I showcase the tunable H2O2 synthesis performance and identify the optimal composition and atomistic structure for these catalytic systems, paving the foundation for practical electrochemical H2O2 synthesis.