The reaction mechanisms of heme catalases: An atomistic view by ab initio molecular dynamics

2012 ◽  
Vol 525 (2) ◽  
pp. 121-130 ◽  
Author(s):  
Mercedes Alfonso-Prieto ◽  
Pietro Vidossich ◽  
Carme Rovira
Keyword(s):  
Molecular Dynamics ◽  
Ab Initio ◽  
Reaction Mechanisms ◽  
Ab Initio Molecular Dynamics

scholarly journals Carbonation Reaction Mechanisms of Portlandite Predicted from Enhanced Ab Initio Molecular Dynamics Simulations

Minerals ◽  
2021 ◽  
Vol 11 (5) ◽  
pp. 509
Author(s):  
Sylvia M. Mutisya ◽  
Andrey G. Kalinichev
Keyword(s):  
Molecular Dynamics ◽  
Ab Initio ◽  
Reaction Mechanisms ◽  
Co2 Storage ◽  
Direct Interaction ◽  
Ab Initio Molecular Dynamics ◽  
Hydroxyl Groups ◽  
Hydrated Cement ◽  
Carbonation Reaction ◽  
Surface Hydroxyl

Geological carbon capture and sequestration (CCS) is a promising technology for curbing the global warming crisis by reduction of the overall carbon footprint. Degradation of cement wellbore casings due to carbonation reactions in the underground CO2 storage environment is one of the central issues in assessing the long-term success of the CCS operations. However, the complexity of hydrated cement coupled with extreme subsurface environmental conditions makes it difficult to understand the carbonation reaction mechanisms leading to the loss of well integrity. In this work, we use biased ab initio molecular dynamics (AIMD) simulations to explore the reactivity of supercritical CO2 with the basal and edge surfaces of a model hydrated cement phase—portlandite—in dry scCO2 and water-rich conditions. Our simulations show that in dry scCO2 conditions, the undercoordinated edge surfaces of portlandite experience a fast barrierless reaction with CO2, while the fully hydroxylated basal surfaces suppress the formation of carbonate ions, resulting in a higher reactivity barrier. We deduce that the rate-limiting step in scCO2 conditions is the formation of the surface carbonate barrier which controls the diffusion of CO2 through the layer. The presence of water hinders direct interaction of CO2 with portlandite as H2O molecules form well-structured surface layers. In the water-rich environment, CO2 undergoes a concerted reaction with H2O and surface hydroxyl groups to form bicarbonate complexes. We relate the variation of the free-energy barriers in the formation of the bicarbonate complexes to the structure of the water layer at the interface which is, in turn, dictated by the surface chemistry and the degree of nanoconfinement.

Combustion Driven by Fragment-based Ab Initio Molecular Dynamics Simulation

2019 ◽  
Author(s):  
Liqun Cao ◽  
Jinzhe Zeng ◽  
Mingyuan Xu ◽  
Chih-Hao Chin ◽  
Tong Zhu ◽  
...  
Keyword(s):  
Molecular Dynamics ◽  
Ab Initio ◽  
Large Scale ◽  
Methane Combustion ◽  
Combustion Method ◽  
Dynamics Simulation ◽  
Ab Initio Molecular Dynamics ◽  
Computational Time ◽  
Combustion Mechanism ◽  
Daily Lives

Combustion is a kind of important reaction that affects people's daily lives and the development of aerospace. Exploring the reaction mechanism contributes to the understanding of combustion and the more efficient use of fuels. Ab initio quantum mechanical (QM) calculation is precise but limited by its computational time for large-scale systems. In order to carry out reactive molecular dynamics (MD) simulation for combustion accurately and quickly, we develop the MFCC-combustion method in this study, which calculates the interaction between atoms using QM method at the level of MN15/6-31G(d). Each molecule in systems is treated as a fragment, and when the distance between any two atoms in different molecules is greater than 3.5 Å, a new fragment involved two molecules is produced in order to consider the two-body interaction. The deviations of MFCC-combustion from full system calculations are within a few kcal/mol, and the result clearly shows that the calculated energies of the different systems using MFCC-combustion are close to converging after the distance thresholds are larger than 3.5 Å for the two-body QM interactions. The methane combustion was studied with the MFCC-combustion method to explore the combustion mechanism of the methane-oxygen system.

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