CFD Modeling of a Carbonation Reactor with a K‐Based Dry Sorbent for CO2 Capture

A 2D CFD simulation of the carbonation reactor is carried out to evaluate the performance of potassium‐based dry sorbent during the CO₂ capture process. A multiscale drag coefficient model is incorporated into the two‐fluid model to take the effects of clusters into account. The influence of several parameters on CO₂ removal is investigated. The results indicate that increasing the reactor height and reducing the gas velocity can lengthen the residence time of particles and enhance the CO₂ removal. The operating pressure has a significant influence on the performance of solid sorbents. A higher pressure will decrease the CO₂ removal efficiency.     

Tap Reactor for Temporally and Spatially Resolved Analysis of the CO2 Methanation Reaction

Chemical energy carriers produced according to power-to-X concepts will play a crucial role in the future energy system. Here, CO₂ methanation is described as one promising route. However, transient operating conditions and the resulting effects on catalyst stability are to be considered. In this contribution, a tap reactor for spatially and temporally resolved analysis of the methanation reaction is presented. The Ni catalyst investigated was implemented as coating. Reaction data as a function of time and reactor coordinate under various operating conditions are presented and discussed. A comparison with simulation data validates the presented tap reactor concept.     

Design and Analysis of a Submerged Membrane Reactor by CFD Simulation

CFD was applied to demonstrate the effect of reactor configurations on the fluid flow pattern in submerged membrane reactors. A mixture model, a realizable k‐? model, and the multiple reference frame (MRF) technique were employed to simulate the solid‐liquid turbulent flow. Influences of the introduction of a ceramic membrane, the relative position between ceramic membrane and impeller, and the types of impeller on velocity profiles and concentration distributions were systematically discussed. These simulation results were validated qualitatively with experimental data for various reactor configurations.     

Entwicklung des Katalysatorbetts in einem Flachbettreaktor zur CO2-Methanisierung

This work presents a development step for a novel flatbed reactor for CO₂ methanation as well as a CFD-based method that can be used for the development and optimization of reactors. The development step comprises the construction of the catalyst bed in the flat bed reactor into which a pure stoichiometric reactive gas is fed. The results show that a high CO₂ conversion (92.9 %) and a small rise in temperature in the catalyst bed (12.4 °C) can be achieved with an arrangement of the catalyst bed. The heat flow reaches 1924 W m⁻² in the hot spot zone.     

LiH合成反应器的CFD模拟与过程强化

为了强化釜式氢化锂(LiH)合成反应器,采用计算流体力学(CFD)方法模拟了该坩埚反应器在静态操作、机械搅拌和气体鼓泡三种情况下的物质传递、化学反应和流体运动规律。模拟结果表明:自然对流对反应有较大的促进作用,其使LiH脱离反应界面,保证界面处"新鲜"金属Li与氢气的有效接触;另外,自然对流也促使反应器内物料良好混合;机械搅拌虽提高了反应物料的混合状况,但并不显著增加反应界面,过程强化程度有限;气体鼓泡可大幅度增加气液接触面积,反应时间大幅度缩减,是一种优选的LiH合成反应器构型。     

Numerical Simulation of Interfacial Closures for 3D Bubble Column Flows

Numerical investigation of flow hydrodynamics in a square cross‐sectioned bubble column was conducted in a transient Euler‐Euler environment by applying the simulation tool Ansys CFX 14.0. The influence of the drag coefficient (C_D) was investigated and the results were also compared with drag force models. Furthermore, three different lift force models and a defined lift coefficient were studied. All results were compared with the available experimental data. All simulations were carried out for a single‐hole sparger with given aspect ratio (H/D) and superficial gas velocity.     

Systematic mesh development for 3D CFD simulation of fixed beds: Single sphere study

To develop and validate meshes for computational fluid dynamics (CFD) simulations of transport in fixed beds, a single particle is often used as a test case. We present results for drag coefficient (C_D) and heat transfer Nusselt number (Nu) for flow past a sphere, focusing on high flow rates typical of industrial steam reformers (400 < Re < 20,000). Over this range, good predictions of C_D were obtained using large eddy simulation (LES) to capture vortex shedding and wake dynamics, with a mesh refined downstream from the sphere. The small time-steps and high cell count required make this too expensive for fixed beds. Nu can be accurately calculated using a Reynolds-averaged Navier-Stokes (RANS) method with shear-stress transport (SST) k-ω closure provided the mesh at the particle surface is fine enough and covers most of the boundary layer. Single sphere simulations of heat transfer are more useful for fixed bed mesh development than drag coefficient calculations.     

Heat Transfer Characteristics of CO2 Desorption from N‐Methyldiethanolamine Solution in a Microchannel Reactor

The heat transfer performance and energy consumption of CO₂ desorption from rich N‐methyldiethanolamine (MDEA) solution were determined experimentally in a straight microchannel reactor. Nucleate boiling was found to be the dominant heat transfer mechanism in this experiment. The heat transfer coefficients were strongly dependent on the heat flux. The solution flow rate was the most influential factor on the heat flux, followed by desorption temperature, MDEA concentration, and CO₂ loading. In addition, an empirical correlation was proposed to predict the experimental heat transfer coefficients.     

Convection Heat Transfer of CO2 at Supercritical Pressures in Microtubes

Convection heat transfer of supercritical pressure CO₂ in microtubes as well as characteristics of fluid flow and heat transfer were investigated. Alterations of physical properties of supercritical CO₂ and the impact of buoyancy on the heat transfer were analyzed when the inlet Reynolds (Re) number of CO₂, diameter of heat exchanger, and inlet Re of cooling water were changed. The temperatures of hot fluid in numerical simulations from several classical turbulence calculation models were compared with experimental results from the literature. The physical properties of CO₂ changed significantly around the critical point, causing a distinct decline of buoyancy and strengthening of heat transfer.     

用多孔金属—SiO2复合膜反应器进行CO水蒸汽变换反应

用自制的多孔金属－ＳｉＯ２复合膜组装成一种新颖的膜反应器,利用ＣＯ变换反应考察该膜反应器的性能实验系统地考察了反应温度,空速、水／气比和只发气流量对ＣＯ转化率的影响。结果表明,在相同的反应条件下,膜反应器的转化率比固定床反应器的转化率提高４－１１％左右,最高可达２０％。     

低高径比气升式环流反应器数值模拟分析

气升式反应器因其结构简单，有良好的混合传热性能，便于操作等优点已广泛用于化工、生物化工等行业。利用商用计算流体力学软件Fluent，利用Euler—Euler双流体模型，重点针对好氧反应的特点，对一种具有低高径比（H/D=1．67）的环流气升式反应器内的气液两相流动及混合性能进行研究，描述出反应器内气含率和环流液速等参数的详细分布，分析模拟结果，气液速度分布和气含率分布等与实际情况基本吻合，从而证实了计算结果的有效性，为工业实际应用提供一定参考。     

Performance evaluation of fixed‐bed,millistructured, and metallic foam reactor channels for CO2 methanation

Power‐to‐gas technologies, combining hydrogen produced by water electrolysis with carbon dioxide to produce substitute natural gas (SNG), can support the increased penetration of renewable electricity sources. However, the technical and economic feasibility of these technologies requires the conversion efficiency of the whole process, including the methanation step. This paper provides an experimental performance comparison of three catalytic methanation reactor concepts, a fixed‐bed reactor, a millistructured reactor, and a metallic foam reactor with the same nickel‐alumina catalyst. The response of each reactor was analyzed in light of five performance criteria, representing the methane yield, the reactor compactness, and the maximum temperature elevation. The millistructured reactor channel showed a higher methane space‐time yield and volumetric productivity than the other reactors, but a significant catalyst temperature elevation. The metallic foam reactor showed a much lower space‐time yield and volumetric productivity, but very good thermal management.

     

Process intensification of CO2 absorption using a 3D printed intensified packing device

This study presents a first of its kind demonstration of successful enhancement of CO₂ chemical absorption, under selected conditions, using a process intensification approach. A multifunctional device that integrates contact of phases and heat exchange has been developed, characterized, and tested. Heat transfer analysis has demonstrated the efficacy of the device as a heat exchanger, and mass transfer results have shown substantial improvement in the uptake of CO₂ under a range of operating conditions.     

Co负载量对Co/TiO2催化CO2甲烷化性能影响

采用沉淀-沉积法制备出w(Co)=10%、15%、20%和25%的Co/TiO_2催化剂,并用于催化CO_2甲烷化反应。通过XRD、TEM、N_2吸附-脱附、H_2程序升温还原(H_2-TPR)和CO_2程序升温脱附(CO_2-TPD)对催化剂进行了表征与测试。结果表明,Co的负载影响了催化剂中Co3O4晶粒尺寸、比表面积、孔径以及催化剂的还原性能,且Co物种与TiO_2载体发生了强相互作用。其中,w(Co)=20%的Co/TiO_2催化剂中Co颗粒平均尺寸约为8nm,比表面积及孔径分别为40.9 m2/g和6.96 nm,且Co分散度达10.1%,从而更有利于CO_2甲烷化反应。此外,w(Co)=20%的Co/TiO_2催化剂表面具有最大的中强碱位量(28μmol/g),从而可活化更多的CO_2。活性测试结果表明,当反应温度为400℃、压力0.5 MPa、原料气空速3 600 m L/(g·h)、V(H_2)/V(CO_2)=4时,w(Co)=20%的Co/TiO_2催化剂的活性最好,其CO_2转化率和CH_4选择性可分别达到69.9%和98.3%,且在20 h内保持稳定。     

ZrO2-Al2O3复合氧化物对负载Ni基催化剂合成甲烷的性能影响

采用并流沉淀法制备了不同配比的ZrO2-Al2O3复合氧化物,并通过浸渍法制备了10% Ni/ZrO2-Al2O3催化剂,考察了复合氧化物载体的水热稳定性及ZrO2与Al2O3的配比对合成气制甲烷Ni基催化剂性能的影响。研究结果表明：ZrO2的添加能在一定程度上抑制Al2O3的水解反应,这可能是ZrO2与Al2O3形成固溶体所致。随着ZrO2含量增加,复合氧化物载体的水热稳定性先降低后升高,当ZrO2与Al2O3质量比为0.24时,载体的水热稳定性最好。不同配比的ZrO2-Al2O3复合氧化物负载Ni基催化剂的稳定性与载体的水热稳定性变化是一致的,说明载体的抗水热能力增强,催化剂结构更稳定,催化剂的活性稳定性相应增加。     

On the temperature control in a microstructured packed bed reactor for methanation of CO/CO2 mixtures

Microreactor technology is widely used for process intensification and is essential for fast and strongly exothermic reactions exhibiting mass and heat transfer limitations. In the scope of the MINERVE Power‐to‐Gas project, sponsored by KIC InnoEnergy from 2012 to 2015, a micro packed bed reactor was developed for conversion of syngas containing CO₂ into methane. This work focuses on heat removal and temperature control in a manufactured device using syngas throughputs less than 1.4 Nm³/h (10% CO, 7% CO₂, H₂/C = 4) while examining the cooling potential of different cooling fluids, e.g., air, steam and water. © 2016 American Institute of Chemical Engineers AIChE J, 63: 120–129, 2017     

负载型K2CO3/Al2O3吸收剂吸收CO2反应机理

利用热重分析仪、扫描电镜和氮吸附仪对不同粒径的K₂CO₃颗粒和负载型K₂CO₃/Al₂O₃二氧化碳吸收剂的碳酸化特性进行研究。负载后的吸收剂比表面积和孔隙结构得到较大改善,使得碳酸化反应速率和转化率均提高,吸收剂碳酸化特性得到改善。纯K₂CO₃颗粒吸收剂的反应速率和转化率随着粒径的增加而减小,负载型吸收剂的反应速率和转化率随着粒径的增加略增大。研究了不同粒径和反应时间对K₂CO₃/Al₂O₃颗粒微观结构的影响,结果表明K₂CO₃/Al₂O₃颗粒具有较稳定的微观结构。采用负载型粒子模型对K₂CO₃/Al₂O₃吸收剂吸收CO₂碳酸化过程进行研究,所建立的粒子模型计算结果与试验值吻合较好。利用建立的模型对不同CO₂浓度下K₂CO₃/Al₂O₃吸收剂碳酸化反应特性进行模拟计算,模拟结果具备一定的合理性和准确性,为开展进一步研究提供了基础。     

Development of a 3D Hybrid Intelligent‐Mechanistic Model for Simulation of Multiphase Chemical Reactors

A novel intelligent‐mechanistic model was developed to understand the behavior of multiphase chemical reactors. Computational fluid dynamics (CFD) and an intelligent algorithm were combined to predict different levels of 3D cylindrical bubble‐column reactors. An adaptive neuro‐fuzzy inference system (ANFIS) was used as the intelligence algorithm, and different ANFIS parameters were evaluated. With about one third of the training data the method can predict the overall behavior of the gas fraction in the reactor. A number of rules significantly influence the accuracy of the ANFIS method. After finding appropriate parameters, the method is applied for prediction of points which are not simulated with CFD, representing ANFIS mesh refinement. Also, bubble‐column reactors without training of exact values of measured data or numerical results can be predicted. Main advantages are time savings and reduction of computational expenses.     

A Short Review on Ni-Catalyzed Methanation of CO2: Reaction Mechanism,Catalyst Deactivation,Dynamic Operation

Today, the use of renewable energies and recycling of climate-changing gases are increasingly important. In this context, coupling of methanation with small, decentralized CO₂ sources such as biogas plants provides one possibility. However, fluctuating availability of renewables for hydrogen production in combination with small storage volumes result in an enhanced demand for dynamic process operation. This leads to new research challenges with respect to the required catalysts and the overall process design. To draw reliable conclusions about the catalytic performance under dynamic process operation, the mechanism of the methanation reaction as well as typical deactivation procedures of the catalyst applied under steady-state conditions have to be reviewed thoroughly.