Andrea Montessori

Mapping reactive flow patterns in monolithic nanoporous catalysts

Abstract The development of high-efficiency porous catalyst membranes critically depends on our understanding of where the majority of the chemical conversions occur within the porous structure. This requires mapping of chemical reactions and mass transport inside the complex nanoscale architecture of porous catalyst membranes which is a multiscale problem in both the temporal and spatial domains. To address this problem, we developed a multiscale mass transport computational framework based on the lattice Boltzmann method that allows us to account for catalytic reactions at the gas–solid interface by introducing a new boundary condition. In good agreement with experiments, the simulations reveal that most catalytic reactions occur near the gas-flow facing side of the catalyst membrane if chemical reactions are fast compared to mass transport within the porous catalyst membrane.

Lattice Boltzmann approach for complex nonequilibrium flows

We present a lattice Boltzmann realization of Grads extended hydrodynamic approach to nonequilibrium flows. This is achieved by using higher-order isotropic lattices coupled with a higher-order regularization procedure. The method is assessed for flow across parallel plates and three-dimensional flows in porous media, showing excellent agreement of the mass flow with analytical and numerical solutions of the Boltzmann equation across the full range of Knudsen numbers, from the hydrodynamic regime to ballistic motion.

Reassessing the single relaxation time Lattice Boltzmann method for the simulation of Darcy’s flows

It is shown that the single relaxation time (SRT) version of the Lattice Boltzmann (LB) equation permits to compute the permeability of Darcy’s flows in porous media within a few percent accuracy. This stands in contrast with previous claims of inaccuracy, which we relate to the lack of recognition of the physical dependence of the permeability on the Knudsen number.

Extended friction elucidates the breakdown of fast water transport in graphene oxide membranes

The understanding of water transport in graphene oxide (GO) membranes stands out as a major theoretical problem in graphene research. Notwithstanding the intense efforts devoted to the subject in the recent years, a consolidated picture of water transport in GO membranes is yet to emerge. By performing mesoscale simulations of water transport in ultrathin GO membranes, we show that even small amounts of oxygen functionalities can lead to a dramatic drop of the GO permeability, in line with experimental findings. The coexistence of bulk viscous dissipation and spatially extended molecular friction results in a major decrease of both slip and bulk flow, thereby suppressing the fast water transport regime observed in pristine graphene nanochannels. Inspection of the flow structure reveals an inverted curvature in the near-wall region, which connects smoothly with a parabolic profile in the bulk region. Such inverted curvature is a distinctive signature of the coexistence between single-particle Langevin friction and collective hydrodynamics. The present mesoscopic model with spatially extended friction may offer a computationally efficient tool for future simulations of water transport in nanomaterials.

Role of Oxygen Functionalities in Graphene Oxide Architectural Laminate Subnanometer Spacing and Water Transport

Active research in nanotechnology contemplates the use of nanomaterials for environmental engineering applications. However, a primary challenge is understanding the effects of nanomaterial properties on industrial device performance and translating unique nanoscale properties to the macroscale. One emerging example consists of graphene oxide (GO) membranes for separation processes. Thus, here we investigate how individual GO properties can impact GO membrane characteristics and water permeability. GO chemistry and morphology were controlled with easy-to-implement photoreduction and sonication techniques and were quantitatively correlated, offering a valuable tool for accelerating characterization. Chemical GO modification allows for fine control of GO oxidation state, allowing control of GO architectural laminate (GOAL) spacing and permeability. Water permeability was measured for eight GOALs characterized by different GOAL chemistry and morphology and indicates that GOAL nanochannel height dictates water transport. The experimental outputs were corroborated with mesoscale water transport simulations of relatively large domains (thousands of square nanometers) and indicate a no-slip Darcy-like behavior inside the GOAL nanochannels. The experimental and simulation evidence presented in this study helps create a clearer picture of water transport in GOAL and can be used to rationally design more effective and efficient GO membranes.

Regularized lattice BGK versus highly accurate spectral methods for cavity flow simulations

The regularized lattice BGK (RLBGK) is validated against high-accuracy spectral Chebyshev methods for lid-driven cavity flows. RLBGK is shown to provide a viable alternative to standard lattice BGK schemes, with significant enhancement of numerical stability at a very moderate computational extra-cost.

Effect of nanoscale flows on the surface structure of nanoporous catalysts

The surface structure and composition of a multi-component catalyst are critical factors in determining its catalytic performance. The surface composition can depend on the local pressure of the reacting species, leading to the possibility that the flow through a nanoporous catalyst can affect its structure and reactivity. Here, we explore this possibility for oxidation reactions on nanoporous gold, an AgAu bimetallic catalyst. We use microscopy and digital reconstruction to obtain the morphology of a two-dimensional slice of a nanoporous gold sample. Using lattice Boltzmann fluid dynamics simulations along with thermodynamic models based on first-principles total-energy calculations, we show that some sections of this sample have low local O2 partial pressures when exposed to reaction conditions, which leads to a pure Au surface in these regions, instead of the active bimetallic AgAu phase. We also explore the effect of temperature on the surface structure and find that moderate temperatures (≈300-450 K) should result in the highest intrinsic catalytic performance, in apparent agreement with experimental results.

Entropic lattice pseudo-potentials for multiphase flow simulations at high Weber and Reynolds numbers

We present an entropic version of the lattice Boltzmann pseudo-potential approach for the simulation of multiphase flows. The method is shown to correctly simulate the dynamics of impinging droplets on hydrophobic surfaces and head-on and grazing collisions between droplets, at Weber and Reynolds number regimes not accessible to previous pseudo-potential methods at comparable resolution.

A gas-kinetic model for 2D transcritical shallow water flows propagating over dry bed

Abstract The solution of fluid dynamics problems has recently witnessed a remarkable increase in the formulation of Boltzmann-based approaches, mainly triggered by the numerous advantages stemming from the concrete possibility of employing a low number of allowed velocities, which is the basis of the Lattice-Boltzmann (LB) methods. The field of Shallow Water (SW) modeling also took advantage of these techniques, but there are still open problems related to the practical impossibility to simulate transcritical flows while retaining the intrinsic simplicity of the LB approaches. This problem is even more crucial if one considers that transcritical flows always develop whenever a transition over dry bed occurs. Since such vertically integrated models are currently the mostly employed ones for simulating technically interesting flows, and since these flows often require the flooding of an initially dry bed, the application of LB methods seems to be facing its limits. The Gas Kinetic Method (GKM) overcomes this issue, integrating the Boltzmann equations in continuous velocity space. In this work, we formulate and extensively test a GKM-based model for solving the SW equations, which is able to manage the propagation over uneven dry bed. The benchmarking, carried out against analytical, experimental and previously proposed numerical reference solutions, shows promising results of the proposed approach.

Lattice kinetic approach to non-equilibrium flows

We present a Lattice Boltzmann method for the simulation of a wide range of Knudsen regimes. The method is assessed in terms of normalised discharge for flow across parallel plates and three-dimensional flows in porous media. Available analytical solutions are well reproduced, supporting the the method as an appealing candidate to bridge the gap between the hydrodynamic regime and free molecular motion.