Banca de DEFESA: GUSTAVO FELIX BITENCOURT

Uma banca de DEFESA de DOUTORADO foi cadastrada pelo programa.
STUDENT : GUSTAVO FELIX BITENCOURT
Date: 03/11/2026
TIME: 09:00
LOCAL: Auditório 801 no 8º andar do Bloco B do Campus Santo André da Universidade Federal do ABC
TITLE:

MOFs and COFs for the Sustainable Hydrogen Peroxide Production and Methane Partial Oxidation

PAGES: 276
BIG AREA: Ciências Exatas e da Terra
AREA: Química
SUBÁREA: Físico-Química
SPECIALTY: Cinética Química e Catálise
SUMMARY:

Methane, the main component of natural gas, is one of the most abundant carbon resources on Earth and, at the same time, a potent greenhouse gas. Its selective conversion into oxygenated products such as methanol under mild conditions is an attractive route for both valorization and emission mitigation, yet it remains a major challenge owing to the high stability of the C-H bond and the tendency toward overoxidation to CO2. Hydrogen peroxide (H2O2) is among the greenest oxidants available for this transformation, but its conventional industrial synthesis through the anthraquinone process is energy-intensive and centralized, which compromises the sustainability of the overall route. This thesis therefore addresses two coupled halves of a single problem: designing a robust porous catalyst able to activate methane using H2O2, and developing a sustainable, on-site route to generate the H2O2 itself. Metalorganic frameworks (MOFs) were exploited for the catalytic step and covalent organic frameworks (COFs) for the oxidant-supply step, so that the oxidant consumed by one platform is the product delivered by the other. For the catalytic step, novel FeGa-based MOFs were designed, synthesized, characterized, and applied to the partial oxidation of methane under mild conditions, with emphasis on Fe-MIL-88B derivatives. As catalyst stability in oxidative, H2O2-rich environments is a critical limitation, framework robustness was systematically assessed through H2O2 decomposition and metal-leaching studies, relating framework composition and synthesis methodology to catalytic behavior. The incorporation of Ga3⁺ as a redox-inert secondary metal center in bimetallic FeₓGaᵧ-MOFs significantly influenced both catalytic activity and structural stability, and photo-assisted methane oxidation was further investigated to probe the role of metal-node composition and linker functionalization under solar simulated irradiation. For the oxidant-supply step, metal-free COFs were investigated as photocatalysts for the solar-driven synthesis of H2O2 from water and O2, establishing structure-activity relationships across pyridinedicarbaldehyde-based (PDA) COF family. Overall, this work advances the rational design of robust porous catalysts for selective C-H oxidation and, by uniting MOF-based methane activation with COF-based photocatalytic H2O2 generation, outlines an integrated, solar-driven pathway toward more sustainable methane-to-oxygenates conversion.

COMMITTEE MEMBERS:
Membro Titular - Examinador(a) Interno ao Programa - 1762430 - DALMO MANDELLI
Membro Titular - Examinador(a) Externo à Instituição - MOHAMAD EL-ROZ
Membro Titular - Examinador(a) Externo à Instituição - PEDRO HENRIQUE MORAIS ANDRADE - UFMG
Membro Titular - Examinador(a) Externo à Instituição - MARCO ANDRÉ FRAGA - INT
Presidente - Externo à Instituição - LIANE MÁRCIA ROSSI - USP
Membro Suplente - Examinador(a) Interno ao Programa - 2351974 - JULIANA DOS SANTOS DE SOUZA SILVA
Membro Suplente - Examinador(a) Externo à Instituição - PEDRO BATALHA NETO - UFF
Membro Suplente - Examinador(a) Externo à Instituição - THIAGO DE MELO LIMA