When will fossil fuel reserves be diminished

Catalytic partial oxidation of methane has been reviewed with an emphasis on the reaction mechanisms over transition metal catalysts. The thermodynamics and aspects related to heat and mass transport is also evaluated, and an extensive table on research contributions to methane partial oxidation over transition metal catalysts in the literature is provided. Presented are both theoretical and experimental evidence pointing to inherent differences in the reaction mechanism over transition metals. These differences are related to methane dissociation, binding site preferences, the stability of OH surface species, surface residence times of active species and contributions from lattice oxygen atoms and support species. Methane dissociation requires a reduced metal surface, but at elevated temperatures oxides of active species may be reduced by direct interaction with methane or from the reaction with H, H2, C or CO. The comparison of elementary reaction steps on Pt and Rh illustrates that a key factor to produce hydrogen as a primary product is a high activation energy barrier to the formation of OH. Another essential property for the formation of H2 and CO as primary products is a low surface coverage of intermediates, such that the probability of O–H, OH–H and CO–O interactions are reduced. The local concentrations of reactants and products change rapidly through the catalyst bed. This influences the reaction mechanisms, but the product composition is typically close to equilibrated at the bed exit temperature.

A review of catalytic partial oxidation of methane to synthesis gas with emphasis on reaction mechanisms over transition metal catalysts

Microscale combustion: Technology development and fundamental research

The microscopic spatial kinetic Monte Carlo (KMC) method has been employed extensively in materials modeling. In this review paper, we focus on different traditional and multiscale KMC algorithms, challenges associated with their implementation, and methods developed to overcome these challenges. In the first part of the paper, we compare the implementation and computational cost of the null-event and rejection-free microscopic KMC algorithms. A firmer and more general foundation of the null-event KMC algorithm is presented. Statistical equivalence between the null-event and rejection-free KMC algorithms is also demonstrated. Implementation and efficiency of various search and update algorithms, which are at the heart of all spatial KMC simulations, are outlined and compared via numerical examples. In the second half of the paper, we review various spatial and temporal multiscale KMC methods, namely, the coarse-grained Monte Carlo (CGMC), the stochastic singular perturbation approximation, and the τ-leap methods, introduced recently to overcome the disparity of length and time scales and the one-at-a time execution of events. The concepts of the CGMC and the τ-leap methods, stochastic closures, multigrid methods, error associated with coarse-graining, a posteriori error estimates for generating spatially adaptive coarse-grained lattices, and computational speed-up upon coarse-graining are illustrated through simple examples from crystal growth, defect dynamics, adsorption–desorption, surface diffusion, and phase transitions.

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An overview of spatial microscopic and accelerated kinetic Monte Carlo methods

Combustion characteristics and flame stability at the microscale: a CFD study of premixed methane/air mixtures

Underground Coal Gasification (UCG) is the process of in-situ conversion of coal into combustible products (syngas) which can be used either as fuel or as a chemical feedstock. In this study, the gasification channel is viewed as a one-dimensional packed bed reactor. The packed bed reactor model is solved incorporating chemical reactions and mass transfer effects. A pseudo-transient model is simulated for temperature and composition profiles of the gas and solid phases. The movements of the pyrolysis and the reaction front are obtained. The model results are in qualitative agreement with literature. The effects of various operating parameters are studied in detail. Steam/O2 ratio, inlet O2 and total pressure determine the solid temperature profile and hence the outlet gas composition. The simulations are performed for two sets of kinetics parameters. The solid temperature profile and outlet gas compositions change significantly with a change in kinetics parameters. The main motivation behind this study is to provide a theoretical base for understanding the critical aspects of UCG and to provide a tool which coupled with experiments will help in determining the commercial feasibility of the UCG process.

Reactor Model for the Underground Coal Gasification (UCG) Channel

Detailed surface reaction mechanism for reduction of NO by CO

A detailed surface reaction mechanism for oxidation of CO on polycrystalline Pt surfaces, capable of predicting various available experimental features, has been developed using a multistep methodology. First, thermodynamically consistent, coverage-dependent activation energies and heats of reactions were derived from the application of the unity bond index-quadratic exponential potential formulation. Next, initial estimates of pre-exponentials were obtained from transition state theory or available experiments. Important feature identification analysis was performed to determine key reaction parameters for each experiment. Model responses were then parameterized in terms of these important parameters by simple polynomials and factorial design techniques and subsequently used in simultaneous optimization through simulated annealing against different sets of literature and new experimental data from our laboratory. Model validation with independent experiments shows that the proposed surface reaction mechanism performs very well. The potential of our approach for developing surface reaction mechanisms for catalytic combustion of more complex fuels is also discussed.

A detailed surface reaction mechanism for CO oxidation on Pt

Simulation of hydrogen mitigation in catalytic recombiner: Part-I: Surface chemistry modelling

During underground coal gasification (UCG), a cavity is formed in the coal seam when coal is converted to gaseous products This cavity grows three dimensionally in a nonlinear fashion as gasification proceeds The cavity shape is determined by the flow field, which is a strong function of various parameters such as the position and orientation of the inlet nozzle and the temperature distribution and coal properties such as thermal conductivity In addition to the complex flow patterns in the UCG cavity, several phenomena occur simultaneously They include chemical reactions (both homogeneous and heterogeneous), water influx, thermomechanical failure of the coal, heat and mass transfer, and so on Thus, enormous computational efforts are required to simulate the performance of UCG through a mathematical model It is therefore necessary to simplify the modeling approach for relatively quick but reliable predictions for application in process design and optimization The primary objective of this work is to

Preeti Aghalayam

Papers

Reactor Model for the Underground Coal Gasification (UCG) Channel

Detailed surface reaction mechanism for reduction of NO by CO

A detailed surface reaction mechanism for CO oxidation on Pt

Simulation of hydrogen mitigation in catalytic recombiner: Part-I: Surface chemistry modelling

Compartment Modeling for Flow Characterization of Underground Coal Gasification Cavity