Modelado de reacciones de catálisis en micelas bio-inspiradas

Alonso Rueda, Elia (2020). Modelado de reacciones de catálisis en micelas bio-inspiradas. Proyecto Fin de Carrera / Trabajo Fin de Grado, E.T.S. de Ingeniería Agronómica, Alimentaria y de Biosistemas (UPM), Madrid, España.

Description

Title: Modelado de reacciones de catálisis en micelas bio-inspiradas
Author/s:
  • Alonso Rueda, Elia
Contributor/s:
  • Martín Santamaría, Sonsoles
Item Type: Final Project
Degree: Grado en Biotecnología
Date: June 2020
Subjects:
Faculty: E.T.S. de Ingeniería Agronómica, Alimentaria y de Biosistemas (UPM)
Department: Biotecnología - Biología Vegetal
Creative Commons Licenses: Recognition - No derivative works - Non commercial

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Abstract

The direct oxidation of methane (CH4) into methanol (CH3OH) at the industrial level is an important challenge in the green chemistry field since CH4 is a 33 times more potent greenhouse gas than CO2 and, due to its physical properties, its storage involves a high cost. Thus, it is suitable to convert CH4 into CH3OH because its storage is much more economical and energy-efficient, and it is also an important carbon chemical feedstock. It is known that methanotrophic bacteria mediate the selective oxidation of CH4 into CH3OH employing methane monooxygenases (MMO) with high efficiency under ambient conditions, so understanding the molecular mechanism of these metalloenzymes is interesting in order to mimic and optimize the reaction at the industrial level in non-biological systems. Based on the work reported by Gava et al. (2019), where they accomplished methane C-H bond functionalization by carbene insertion from ethyl diazoacetate (EDA) catalyzed by a silver-based complex by bio-inspired micellar catalysis, we have performed the computational studies of five water-solvated systems in order to understand the molecular interactions among the reagents and the surfactants and to explain the different yields obtained. Molecular dynamics simulations were performed with the aim to study the self-assembly process of the different surfactant micelles (SDS, PFOS, DTAC and Triton) and their interaction with the silver-based catalyst and EDA. Our results show that the reaction does not occur in water, so it is necessary the hydrophobic environment provided by micelles core. PFOS micelles are the best system for the reaction to take place because the catalyst is totally inserted into the core, where is able to interact with EDA and start the reaction successfully (yield = 14%). The reaction also occurs in SDS micelles, but the yield is lower (10%) because the catalyst is oriented to the surface, so the environment is not as hydrophobic as it was in PFOS micelles. In DTAC micelles, the catalyst is oriented in a similar way as it was in SDS micelles; however, it is more exposed to water in the micellar surface and the reaction does not occur (yield = 0%). Finally, triton molecules have a structure that does not allow the successful interaction between the catalyst and EDA for the reaction to take place, although the catalyst is located in a hydrophobic environment.

More information

Item ID: 66665
DC Identifier: https://oa.upm.es/66665/
OAI Identifier: oai:oa.upm.es:66665
Deposited by: Biblioteca ETSI Agrónomos
Deposited on: 09 Apr 2021 08:52
Last Modified: 09 Jun 2021 22:30
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