Advanced catalysts for the electrocatalytic hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are required in the future to further develop an efficient and up-scalable water splitting process. Among all the potential candidates, carbon-supported transition metal-based nanomaterials are of great interest due to their low cost, high durability, and promising functional performance.
This dissertation presents an innovative and cost-effective approach to synthesize carbon shell-encapsulated transition metal alloys or phosphide nanoparticles supported on in-situ formed defective N-doped carbon/carbon nanotube hybrids, which are derived from novel single-source-precursors (SSPs). The precursor is synthesized by a facile one-pot reaction using cheap and environmentally friendly carbon and phosphorus sources. The obtained core-shell structured hybrids perform as highly active and durable electrocatalysts for HER and/or OER, benefiting from the following common features: (1) A synergistic electronic effect among transition metal compounds, heteroatom-doped carbon, and entangled carbon nanotubes. (2) Promotion of electrolyte penetration towards the active sites through the porous structure of the formed mesoporous carbon clusters. (3) The unique core-shell nanostructure of the hybrid material effectively curbs the degradation of the electrocatalyst by protecting the active nanoparticles from harsh electrolyte.
The present studies propose various strategies to enhance the electrocatalytic properties, utilizing both morphology-controlled and composition-controlled methods. Additionally, the studies also focus on the relationship between structure and property, which ultimately determines the electrocatalytic activity for the HER and OER. These findings may offer valuable insights for future applications in the field of electrochemical water splitting. Furthermore, the thesis aims to provide a cost-effective and straightforward approach for synthesizing hybrid materials comprised of transition metal compounds and carbon, with the goal of facilitating their potential utilization in energy storage and conversion applications
