PORE-SCALE STUDY OF MULTIPLE COUPLED PHYSICOCHEMICAL PROCESSES IN ENERGY AND ENVIRONMENTAL SCIENCES
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1 Proceedings of the Asian Conference on Thermal Sciences 2017, 1st ACTS March 26-30, 2017, Jeju Island, Korea ACTS-P00449 PORE-SCALE STUDY OF MULTIPLE COUPLED PHYSICOCHEMICAL PROCESSES IN ENERGY AND ENVIRONMENTAL SCIENCES L. Chen 1 *, Y. T. Mu 1, Ting Min 1, Q.J. Kang 2, Y.L. He 1, W.Q. Tao 1 1 Xi an Jiaotong University, 28 Xianning West Rd. Beiling District, Xi an, Shaanxi , China 2 EES-16, Earth and Environmental Science, Los Alamos National Lab, New Mexico, 87544, USA * Presenting and Corresponding Author: lichennht08@mail.xjtu.edu.cn ABSTRACT Multiple physicochemical reactive transport processes in porous media are pervasive in energy and environmental science. Typical examples include fuel cells and batteries, geological storage of carbon dioxide and nuclear waste, exploitation of conventional/unconventional hydrocarbon resources and VOC emissions. In such processes, strongly coupled single or multiphase flow, heat transfer, mass transport and chemical reactions simultaneously take place in complex structures of porous media. A better understanding of these processes is critical to improving efficiency and durability of the electrochemical energy conversion systems, to enhancing the hydrocarbon recovery, to managing safe disposal of energy-related waste, and to controlling the air quality. Such processes, however, is a challenging problem for theoretical analysis, experimental studies and numerical simulations as not only multiple processes are involved but also these processes are strongly coupled. Besides, the complicated morphology of porous media leads to complicated interfacial interactions between reactive transport processes and the porous structures. In this paper, we will introduce our work of developing advanced pore-scale numerical methods which take into account the coupled multiple physicochemical processes and their interactions. Such pore-scale numerical methods have been adopted to investigate at pore-scale several typical physicochemical processes in energy and environmental science, including multiphase flow and electrochemical processes in gas diffusion layer and catalyst layer in proton exchange membrane fuel cell, multicomponent reactive transport with solid dissolution-precipitation during CO2 sequestration, brine thermal migration in crystals during nuclear waste disposal, and VOC emission. Complicated pore-scale phenomena are captured and the coupled mechanisms are revealed by the pore-scale studies. KEYWORDS: Porous media, pore-scale study, reactive transport, multiphase flow, heat and mass transfer, simulation 1. INTRODUCTION In energy and environmental sciences, multiple physicochemical reactive transport processes widely occur, in which multiple processes (single or multiphase flow, heat and mass transfer, chemical reactions) are simultaneously taking place and are closely interacted. Typical examples include fuel cells and batteries, geological storage of carbon dioxide and nuclear waste, exploitation of conventional/unconventional hydrocarbon resources and VOC emissions. Taking CO2 sequestration as an example, supercritical CO2 (sc-co2) is injected into deep brine for storage, during which there are four mechanisms helping CO2 sequestration, namely structural trapping, capillary trapping, dissolution trapping and mineral trapping. Several sub-processes can be identified during CO2 sequestration, including sc-co2 multiphase flow, dissolved ion transport, homogeneous reactions in the bulk brine and heterogeneous reactions at the rock surface, as well as rock dissolution-precipitation[1]. Reactive transport in fuel cell is another typical example, in which more than ten sub-processes are involved, such as gas-water two phase flow, heat transfer, multicomponent mass transport, electron conduction, proton transfer and electrochemical 1
2 reaction at the triple-phase boundary in porous catalyst layer[2]. Another typical example is the transfer and adsorption in microscopic porous structures of suspending particles in the air (such as PM 2.5) [3]. A better understanding of these processes is critical to improving efficiency and durability of the electrochemical energy conversion systems, to enhancing the hydrocarbon recovery, to managing safe disposal of energy-related waste, and to controlling the air quality. Such processes, however, is a challenging problem for theoretical analysis, experimental studies and numerical simulations as not only multiple processes are involved but also these processes are strongly coupled. Besides, the complicated morphology of porous media leads to complicated interfacial interactions between reactive transport processes and the porous structures. Due to the non-linear non-equilibrium characteristics of the multiphase transport processes, the complicated coupled mechanisms, as well as the complex porous structures, it is really hard or impossible to find corresponding analytical solutions[4]. Due to current spatial and temporal limitations of experimental techniques, it is also challenging for experiments to observe in-situ the coupled multiple reactive transport processes inside the porous media[5]. Numerical simulations provide an efficient way to investigate at a much fundamental scale the transport processes and their coupling mechanisms. Pore-scale simulations, in which the complex microscopic structures of porous media are explicitly resolved, have been widely adopted for multiple physicochemical reactive transport processes. Compared with continuum models and simulations in which homogeneous structure assumption is widely adopted, in pore-scale models no assumptions are made [6-11]. Therefore, empirical relationships such as porositypermeability which are highly required in continuum models are not needed in pore-scale models. In fact, such empirical relationships for macroscopic transport properties can be provided by pore-scale studies. For example, after details of velocity field in each void nodes inside a porous medium are predicted by pore-scale simulations, the permeability can be calculated based on the Darcy s law. Another advantage of pore-scale studies compared with continuum models is the ability of providing distribution details of related variables such as pressure, velocity, temperature and concentration within the realistic structures of porous media. With the distribution details, transport processes inside the porous media as well as the interfacial interactions at the fluid-solid surface can be more deeply understood [6-11]. During the past decade, we have been working on developing advanced pore-scale numerical methods which take into account the coupled multiple physicochemical processes and their interactions. Such pore-scale numerical methods have been successfully adopted to investigate at pore-scale several typical physicochemical processes in energy and environmental science, including multiphase flow and electrochemical processes in gas diffusion layer and catalyst layer in proton exchange membrane fuel cell, multicomponent reactive transport with solid dissolutionprecipitation during CO2 sequestration, brine thermal migration in crystals during nuclear waste disposal, and VOC emission. Complicated pore-scale phenomena are captured and the coupled mechanisms are revealed by the porescale studies. In this paper, we will introduce the advanced pore-scale models developed by our group and their applications. 2. ADVANCED PORE-SCALE METHODS FOR REACTIVE TRANSPORT PROCCESS 2.1 STRUCTURAL RECONSTUCTION The first step towards pore-scale studies is to precisely describe the realistic structures of a porous medium including the solid skeletons and pores separated by the skeletons. To this end there are usually two schemes, the experimental techniques and the computational reconstruction, both of which are adopted in our group. Advanced image techniques, such as X-ray computed micro-tomography (XCMT) [12], focused ion beam[13], serial sectioning [14], and laser scanning confocal microscopy [15], allow one to directly obtain sufficient structural information in a nondestructive manner. The applications of these image techniques, however, have not been widespread due to some factors such as their relatively low resolution and high cost [16]. On the other hand, a variety of reconstruction methods have been developed, including Gaussian random filed method, stochastic reconstruction procedure, multipoint reconstruction method, etc. Obviously, the shape, interaction and distribution of different elements in different 2
3 porous media are quite different. Thus, it is impossible (or extremely challenging if possible) to develop a generalized algorithm to describe structural variations of all kinds of porous media. It is required to develop a corresponding customized algorism for a certain kind of porous media. During the past decade, both experimental techniques and numerical reconstruction have been adopted in our group to acquire accurate representation of the structures of porous media. Particularly, we have adopted or developed several unique reconstruction algorisms for several typical kinds of porous media in energy and environmental sciences, such as fibrous porous media, granular porous media, net-like porous media, etc. Showing in Fig. 1 are the typical porous media reconstructed by our group. For the details of the reconstruction processes, one can refer to the corresponding literature [17-22]. Fig. 1 Porous structures reconstructed by our group. (a) granular porous structure[17], (b) vonoroi porous structure[18], (c) random pore sphere[19], (d) shale[20], (e) fibrous structure[21], (f) foam structure, (g) composite material and (h) fracture[22]. 2.2 NUMERICAL METHODS Accurate pore-scale simulation of the multiple multiphase multi-component reactive transport processes, where the shape of the deformable liquid-gas-solid interfaces is part of the required result, is associated with four major essential and fundamental elements. The first one is the capture of deformable liquid-gas interfaces which may stretch, break-up or coalesce. The available models for tracking the moving liquid-gas interface can be roughly classified in two groups: the diffusion interface model and the sharp interface model [23-27] and one can refer to the recent review for more detail [28]. The second one is how to track the moving fluid-solid interfaces due to dissolution-precipitation (or melting-solidification). Actually, the models developed for predicting the liquid-gas interfaces can be directly used for this purpose. The common features of the problems with the evolutions of the solid phases is that there is no fluid flow and mass transport in the solid phase, and flow at the solid-fluid interfaces is subject to a no-slip condition as the dissolution-precipitation (or melting-solidification) is very low in the practical systems [29-36]. The third one is mass transfer in the multiphase systems. The mass transfer processes in different phases, which is very important for understanding the reactive transport, processes poses a great challenge. In addition to the mass transfer itself, the accompanying deformation of the liquid-gas-solid interface, make the interphase mass transfer more complicated [28, 37]. The last one is the incorporation of the homogeneous and heterogeneous reactions into the simulations[38]. The spatial heterogeneity due to complex porous structures and the moving liquid-gas-solid interfaces lead to a strong coupling between heat transfer, mass transport and chemical reactions. Among the various numerical methods adopted for pore-scale studies, the lattice Boltzmann method, to the best of our knowledge, is one of the most widely adopted. The LBM considers flow as a collective behavior of pseudo-particles residing on a mesoscopic level, and solves Boltzmann equation using a small number of velocities adapted to a regular grid in space[39]. Compared with conventional CFD (computational fluid dynamics) methods 3
4 based on a direct discretization of the NS equations, the LBM shows appealing features such as programming simplicity and intrinsic parallelism. Due to its kinetic origin, the most distinct feature of the LBM is its powerful ability to deal with complex solid boundaries, as well as incorporate molecular interactions. Therefore, the LBM has gained popularity for simulating fluid flow in porous media [40, 41] and multiphase flow problem [42-44]. Therefore in our pore-scale numerical strategy, the LBM is adopted as the fundamental method for solving transport process in porous media. The strategy is called pore-scale lattice Boltzmann model for multiphase multicomponent reactive transport (PS-LBM3RT) [8, 37, 38, 45, 46]. PS-LBM3RT has the ability to solve single or multiphase fluid flow, mass transport, heat transfer, electron and proton conduction, homogeneous and heterogeneous reaction, and solid dissolution-precipitation (melting-solidification) processes. Compared with previous pore-scale models in the literature, the unique feature of PS-LBM3RT is: (a) it takes into account the multiple physicochemical processes and their interactions, (b) it is, the to the best of our knowledge, the first pore-scale model for coupled multiphase flow and reactive transport in porous media [37, 47], (c) it accounts for solid structure evolution due to chemical dissolution-precipitation (or melting-solidification due to heat transfer), (d) it can treat transport problems with huge changes of transport properties, such as high thermal conductivity ratio within fluid-solid conjugate heat transfer, or high diffusivity ratio within mass transport across phase interface[48]. Fig. 2 shows functions and potential applications of PS-LBM3RT. Fig.2 The function and application of pore-scale lattice Boltzmann model for multiphase multicomponent reactive transport (PS-LBM3RT) developed by the author s group. 3. APPLICATIONS Up to now, PS-LBM3RT has been adopted for a variety of problems in energy and environmental sciences, such as electrochemical energy conversion system[48], micro reactor[45], CO2 sequestration[31], enhanced oil recovery[8, 49], shale gas exploitation[20], nuclear water disposal[37], VOC/SVOC emission[50], etc. Below a few typical applications are introduced briefly. 3.1 REACTIVE TRANSPORT IN CATALYST LAYER OF FUEL CELL Several technical barriers must be overcome before widespread commercialization of proton exchange membrane fuel cell, such as the high cost due to precious metal-based catalysts (Pt) in catalyst layer. Deep understanding of mass transport in catalyst layer will improve the utilization of Pt and can reduce the Pt loading. To this end, pore- 4
5 scale simulations have been conducted in the literature. However, these studies either were based on ideal structures of catalyst or took into account part of the multiple reactive transport processes involved. Our group reconstructed the porous catalyst layer based on specific synthesis process used in fabricating a given CL structure [51], in which the CL is reconstructed step by step based on experimental fabrication processes including carbon seed generation, carbon phase growth, Pt deposition, and ionomer inclusion. This method had a much higher resolution (~2 nm) which allows for a more detailed distribution of Pt particles when compared with previous studies, as shown in Fig. 3a. PS-LBM3RT was adopted to investigate the reactant transport, proton conduction and electrochemical reactions at the triple-phase boundary[48]. Results indicate that the non-uniform distribution of ionomer in CL generates more tortuous pathways for reactant transport, greatly reducing the effective diffusivity. The tortuosity of CLs is much higher than that adopted by the Bruggeman equation. Knudsen diffusion plays a significant role in oxygen diffusion and significantly reduces the effective diffusivity. In addition, reative transport in a novel non-precious metal catalyst (NPMC) CL was also studied. Although the reactive surface area of the NPMC CL is much higher than that of the Pt CL, the oxygen reaction rate is lower in the NPMC CL due to the much lower reaction rate coefficient. Although pores of a few nanometers in size can increase the number of reactive sites in NPMC CLs, they contribute little to enhance the mass transport. Mesopores, which are a few tens of nanometers or larger in size, are shown to be required in order to increase the mass transport rate Fig. 3(c). To the best of our knowledge, our work is the first one for pore-scale investigation of reactive transport in realistic porous CL with Pt and NPMC catalysts. (a) (b) (c) Fig. 3 Pore-scale study of reactive transport in porous catalyst layer. (a) Reconstructed CL, (b) distribution of oxygen concentration, (c) effects of pore size on reaction rate. 3.2 DISSOLUTION OF ROCK DURING CO2 SEQUSTRATION Four mechanisms help the CO2 sequestration in deep brine include structural, capillary, soluble and mineral trapping. sc-co2 dissolves into the brine, causing a lower ph of brine. Therefore, brine will react with surrounding rock. Several pore-scale studies have been performed to explore above processes. However, none of the existing studies consider the effects of un-dissolved minerals in rocks. Natural rocks usually consist of multiple minerals and different minerals present different dissolution rate. For example, in experiment of [52, 53], calcite, clay, quartz, dolomite and pyrite were identified in the argillaceous limestone rock, and the dissolution rate of clay is about 10 6 magnitude lower than that of carbonate minerals. Using PS-LBM3RT, effects of undissolved minerals on the changes of permeability and porosity of porous rocks under different Peclet and Damkohler numbers were investigated [18]. The simulation results show porous layers formed by the undissolved mineral remain behind the 5
6 dissolution reaction front. Due to the large flow resistance in these porous layers, the permeability increases very slowly or even remains at a small value although the porosity increases by a large amount. Besides, due to the heterogeneous characteristic of the dissolution, the chemical, mechanical and hydraulic apertures are very different from each other. Simulations also demonstrate that the existence of the porous layers of the nonreactive mineral suppresses the wormholing phenomena observed in the dissolution of mono-mineralic rocks. t = 2s t = 500s t = 2000s Fig. 4 Pore-scale study of effects of undissolved mineral on the dissolution of porous rocks 3.3. MULTIPHASE REACTIVE TRANSPORT DURING NUCLEAR WATER DISPOSAL As discussed previously, coupled multiphase flow and reactive transport pose new challenging to pore-scale studies due to complicated interfacial phenomena. The pore-scale model is used to simulate the thermally driven migration of a brined inclusion in a salt crystal. The background is that salt deposits have been considered as an attractive disposal medium for heat-generating wastes such as used nuclear fuel [54]. PS-LBM3RT was adopted to investigate the microscopic coupled multiple physicochemical processes including multiphase flow with phase separation, mass transport, surface reaction, and salt dissolution/precipitation (Fig. 5). The mechanism of macro thermal migration of the inclusion in the salt is identified as cold-site precipitation and hot-site dissolution by the pore-scale studies. Effects of initial inclusion size and temperature gradient on the migration process were investigated [37]. Fig. 6 Multiphase reactive transport processes during thermal migration of brine in salt. 6
7 4. CONCLUSION In this paper, a pore-scale model for multiphase multicomponent reactive transport in porous media developed by the author during the past decade is introduced briefly. The numerical method adopted for solving single or multiphase flow, heat transfer, mass transfer, and electron/proton conduction is the lattice Boltzmann method, which is a macroscopic method particularly suitable for porous flow and multiphase flow. The pore-scale model developed is called PS-LBM3RT (pore-scale lattice Boltzmann model for multiphase multicomponent reactive transport). PS- LBM3RT has the ability to solve single or multiphase fluid flow, mass transport, heat transfer, electron and proton conduction, homogeneous and heterogeneous reaction, and solid dissolution-precipitation (melting-solidification) processes. Compared with previous pore-scale models in the literature, the unique feature of PS-LBM3RT is: (a) it takes into account the multiple physicochemical processes and their interactions, particularly the homogeneous and heterogeneous reactions, (b) it is, the to the best of our knowledge, the first pore-scale model for coupled multiphase flow and reactive transport in porous media, (c) it accounts for solid structure evolution due to chemical dissolutionprecipitation (or melting-solidification due to heat transfer), (d) it can treat transport problems with huge changes of transport properties, such as high thermal conductivity ratio within fluid-solid conjugate heat transfer, or high diffusivity ratio within mass transport across phase interface. Up to now, PS-LBM3RT has been successfully applied to investigate a number of reactive transport processes in porous media, such as electrochemical energy conversion system, CO2 sequestration, enhanced oil recovery, micro reactor, contaminant transport under subsurface, voc/svoc emission, etc. In the future, we will further develop PS- LBM3RT, particularly in the aspect of multiphase reactive transport with high density ratio of two phase flow, flow with high Re number, transport with high Pe number and mass transport with high Sc number. ACKNOWLEDGMENT The author thanks support from National Nature Science Foundation of China (NSFC) and the Fundamental Research Funds for the Central Universities. The authors acknowledge the support of LANL s LDRD Program and Institutional Computing Program. REFERENCE [1] R.S. Middleton, G.N. Keating, P.H. Stauffer, A.B. Jordan, H.S. Viswanathan, Q.J. Kang, J.W. Carey, M.L. Mulkey, E.J. Sullivan, S.P. Chu, R. Esposito, T.A. Meckel, The cross-scale science of CO2 capture and storage: from pore scale to regional scale, Energy & Environmental Science, 5(6) (2012) [2] D. Song, Q. Wang, Z. Liu, T. Navessin, M. Eikerling, S. Holdcroft, Numerical optimization study of the catalyst layer of PEM fuel cell cathode, Journal of Power Sources, 126(1 2) (2004) [3] Y. Xu, J.C. Little, Predicting Emissions of SVOCs from Polymeric Materials and Their Interaction with Airborne Particles, Environmental Science & Technology, 40(2) (2006) [4] P. Meakin, A.M. Tartakovsky, Modeling and simulation of pore-scale multiphase fluid flow and reactive transport in fractured and porous media, Reviews of Geophysics, 47(3) (2009) n/a-n/a. [5] A. Bazylak, Liquid water visualization in PEM fuel cells: A review, International Journal of Hydrogen Energy, 34(9) (2009) [6] L. Hao, P. Cheng, Lattice Boltzmann simulations of liquid droplet dynamic behavior on a hydrophobic surface of a gas flow channel, Journal of Power Sources, 190(2) (2009) [7] Q. Kang, P.C. Lichtner, H.S. Viswanathan, A.I. Abdel-Fattah, Pore Scale Modeling of Reactive Transport Involved in Geologic CO2 Sequestration Transport in porous media, 82(1) (2010) [8] Q. Kang, D. Zhang, S. Chen, X. He, Lattice Boltzmann simulation of chemical dissolution in porous media, Physical Review E, 65(3) (2002) [9] K.-J. Lee, J.H. Nam, C.-J. Kim, Pore-network analysis of two-phase water transport in gas diffusion layers of polymer electrolyte membrane fuel cells, Electrochimica Acta, 54(4) (2009) [10] T. Zeiser, P. Lammers, E. Klemm, Y. W. Li, J. Bernsdorf, G. Brenner, CFD-calculation of flow, dispersion and reaction in a catalyst filled tube by the lattice Boltzmann method, Chemical Engineering Science, 56(4) (2001) [11] Yaling He, Yong Wang, Qing Li, Theory and appication of the lattice Boltzmann method, Science Press, Beijing,
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