CO Capture and Release in Amine Solutions: To What Extent Can Molecular Simulations Help Understand the Trends?

Absorption in amine solutions is a well-established advanced technology for CO capture. However, the fundamental aspects of the chemical reactions occurring in solution still appear to be unclear. Our previous investigation of aqueous monoethanolamine (MEA) and 2-amino-2-methyl-1,3-propanediol (AMPD), based on ab initio molecular dynamics simulations aided with metadynamics, provided new insights into the reaction mechanisms leading to CO capture and release with carbamate formation and dissociation.

A Combined Experimental-Theoretical Study on Diels-Alder Reaction with Bio-Based Furfural: Towards Renewable Aromatics.

The synthesis of relevant renewable aromatics from bio-based furfural derivatives and cheap alkenes is carried out by using a Diels-Alder/aromatization sequence. The prediction and the control of the ortho/meta selectivity in the Diels-Alder step is an important issue to pave the way to a wide range of renewable aromatics, but it remains a challenging task. A combined experimental-theoretical approach reveals that, as a general trend, ortho and meta cycloadducts are the kinetic and thermodynamic products, respectively.

Direct Catalytic Conversion of Furfural to Furan-derived Amines in the Presence of Ru-based Catalyst.

The production of amine intermediates from biomass is capturing increasing attention. Herein, a simple and efficient preparation of l furan-derived amines was developed [e.g.

Alkyl coupling in tertiary amines as analog of Guerbet condensation reaction.

We report here that C-C coupling in tertiary amines for the synthesis of long chain and hindered amines might be efficiently performed over Pt and Pd catalysts. The mechanism study confirms similarity with the Guerbet reaction through dehydrogenation of the alkyl group and subsequent attack of the α-carbon atom by an alkyl group of another molecule. Finally, secondary amines and tertiary amines with longer alkyl chains are formed.

Capture and Release of CO₂ in Monoethanolamine Aqueous Solutions: New Insights from First-Principles Reaction Dynamics.

Aqueous monoethanolamine (MEA) solution is commonly used for post-combustion carbon capture via chemical absorption. Extensive research has been carried out to characterize both uptake and release of carbon dioxide (CO2), with the aim of improving process performance. However, an intensive research is still needed on fundamental aspects of the key chemical reactions, to achieve a comprehensive understanding of the cyclic process at the microscopic level and a quantitative assessment.

Rigid- and polarizable-ion potentials for modeling Ru-polyoxometalate catalysts for water oxidation.

This work assesses the predictive power and capabilities of classical interatomic potentials for describing the atomistic structure of a fully inorganic water-oxidation catalyst in the gas phase and in solution. We address a Ru-polyoxometalate molecule (Ru-POM) that is presently one of the most promising catalysts for water oxidation due to its efficiency and stability under reaction conditions. The Ru-POM molecule is modeled with two interatomic potentials, the rigid ion model and the shell model potentials, which are used to perform molecular dynamics simulations.

Capturing CO2 in Monoethanolamine (MEA) Aqueous Solutions: Fingerprints of Carbamate Formation Assessed with First-Principles Simulations.

Chemical absorption in amine aqueous solutions is a widespread technology for postcombustion carbon capture, and a large effort is ongoing to improve their performance. Characterization of the "reactant" and "product" solutions at the microscopic level is highly desirable for process optimization. Recently X-ray scattering experiments and "in situ" infrared spectroscopy have been applied to this aim, but a complete and convincing interpretation is missing.

Interface structure and reactivity of water-oxidation Ru-polyoxometalate catalysts on functionalized graphene electrodes.

We combine classical empirical potentials and density functional theory (DFT) calculations to characterize the catalyst/electrode interface of a promising device for artificial photosynthesis. This system consists of inorganic Ru-polyoxometalate (Ru-POM) molecules that are supported by a graphitic substrate functionalized with organic dendrimers. The experimental atomic-scale characterization of the active interface under working conditions is hampered by the complexity of its structure, composition, as well as by the presence of the electrolyte or solvent.