Liu, Longxiang; (2024) Design of Carbon-Based Electrocatalysts for Electrochemical Hydrogen Peroxide Production. Doctoral thesis (Ph.D), UCL (University College London).

Text Design of Carbon-Based Electrocatalysts for Electrochemical Hydrogen Peroxide Production.pdf - Other Access restricted to UCL open access staff until 1 February 2025. Download (13MB)

Abstract

The electrochemical conversion of small molecules, bridging renewable energy utilization and value-added chemical synthesis, offers eco-friendly alternatives to traditional thermal processes. Within this realm, electrochemical hydrogen peroxide (H2O2) production (EHPP) via the two-electron oxygen reduction reaction (2e- ORR) emerges as a compelling avenue. In contrast to conventional energy-intensive anthraquinone oxidation/reduction process, EHPP offers a direct and environmentally benign approach for the on-site and on-demand generation of H2O2 solutions. The advancement of EHPP critically depends on the development of efficient electrocatalysts, with carbon-based materials standing out due to exceptional conductivity, tunable properties, and abundant availability. This thesis commenced with a comprehensive introduction to EHPP in the first chapter including its significance, challenges, evaluation methods, characterization techniques, and recent advancements, thus laying the foundation for subsequent investigations. Chapter 2 demonstrated the efficient quinone-doped porous carbon catalysts for EHPP. A direct correlation between quinone content and EHPP performance was established by comprehensive electrochemical evaluation and synchrotron radiation-based near edge X-ray absorption fine structure (NEXAFS) analysis. Subsequently, chapter 3 investigated the crucial role of different oxygen functional groups (OFGs) in tailoring EHPP performance, with a particular emphasis on the superior EHPP performance of quinone groups. Additionally, the role played by the position of quinone groups was further demonstrated using the Density Function Theory (DFT) study. In chapter 4, cobalt-nitrogen-doped carbon (Co-N-C) material with exceptional EHPP performance was synthesized using a surface engineering strategy. Comprehensive characterization techniques involving electron microscopy and X-ray absorption spectroscopy shed light on the isolated dispersion and possible electronic configurations of Co-C/N/O species. Furthermore, chapter 4 uncovered the positive correlation between the asymmetricity of Co-C/N/O species and the adsorption energy of the OOH* intermediate, corroborated by DFT studies. In conclusion, this thesis advances our understanding of EHPP, underscoring the pivotal role of methodologies and characterization techniques in carbon-based materials research, offering sustainable and environmentally friendly approaches to chemical production.

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