Efficient operation of autothermal microchannel reactors for the production of hydrogen by steam methane reforming

Efficient conversion of methane to hydrogen has emerged as a significant challenge to realizing fuel cell-based energy systems. Autothermal microchannel reactors, coupling of exothermic and endothermic reactions in parallel channels, have become one of the most promising technologies in the field of hydrogen production. Such reactors were utilized as an intensified design for conducting the endothermic steam methane reforming reaction. The energy required by the endothermic process is supplied directly through the separating plates of the reactor structure from the exothermic process occurring on the opposing side. Optimal design problems associated with transport phenomena in such an autothermal system were analyzed. Various methods for designing and operating autothermal reactors employed in steam methane reforming were discussed. Computational fluid dynamics simulations were performed to identify the underlying principles of process intensification, and to delineate several design and operational features of the intensified reforming process. The results indicated that the autothermal reactor is preferable to be thermally conductive to ensure its structural integrity and maximum operating regime. However, the thermal properties of the reactor structure are not essential due to efficient heat transfer existing between endothermic and exothermic process streams. A reactor design which minimizes the mass transfer resistance is highly required, and the channel dimension is of critical importance. Furthermore, the challenges presented by the efficient operation of the autothermal system were identified, along with demonstrating the implementation of transport management in order to improve overall reactor performance and to mitigate extreme temperature excursions.     

Comparisons between methane and methanol steam reforming in thermally integrated microchannel reactors for hydrogen production: A computational fluid dynamics study

This paper addresses the issues related to the design and operation of steam reforming combined with catalytic combustion in thermally integrated microchannel reactors for hydrogen production. Comparisons were made between methanol and methane steam reforming, representing a low and a high temperature process respectively, under the same operating conditions to determine whether methanol-based thermally integrated systems can be more energy-efficient than methane-based ones. Computational fluid dynamics simulations were performed to gain insight into the reactor performance and thermal behavior. The effect of various design parameters was investigated to identify suitable ranges of operating conditions, and an analysis of heat and mass transfer was performed to design a highly efficient system. It was shown that steam reforming of both fuels is feasible in millisecond reactors under a variety of conditions, but very careful design is necessary. Methanol reforming can be more efficient, offering a better solution not only to simplify design but also to improve power and efficiency. The wall thermal conductivity is essential to the design and optimization of these systems, as it can significantly affect the overall energy balance. There is no significant difference in reactor performance between different channel heights at the same flow rate. The ratio of the flow rates on opposite sides of the reactor is an important design parameter and must be carefully adjusted to improve efficiency and eliminate hot spots. Finally, a simple operating strategy was proposed to achieve variable power output, and design recommendations were made.     

Autothermal reforming of n‐hexadecane over Rh catalyst to produce syngas in microchannel reactor using finite element method

Numerical study on the autothermal reforming of n‐hexadecane, which can be used in proton exchange membrane fuel cell for automotive applications, in microchannels is necessary. A 2D computational fluid dynamics (CFD) model, with combustion and reforming channels thermally coupled and separated by a metal medium wall, is developed and studied in terms of hydrogen production and catalyst activity. Rh supported on CeO₂ is used as a catalyst and applied to the inner surface of the channels, where the catalytic endothermic and exothermic reactions occur. CFD analysis shows considerable results in terms of reactor performance. Along the reactor channel length, the mole percentage of hydrogen is 86% after over 2 hours of catalyst activity. The corresponding fuel conversion in respective channels is 85% on the catalytic surface of the reactor. The predicted hydrogen production from the CFD model is 59% higher than that as equilibrium conditions. Heat conduction through the medium solid wall depends on the thermal conductivity of a material. In this model, a metal solid wall with thermal conductivity of 40 W/m K, which transfers heat from the combustion channel within milliseconds, is used. The calculated model operating temperature in the reforming channel ranges from 660 to 850 K.     

Mass transport limitations in microchannel methanol-reforming reactors for hydrogen production

The potential of methanol reforming systems to greatly improve productivity in chemical reactors has been limited, due in part, to the effect of mass transfer limitations on the production of hydrogen. There is a need to determine whether or not a microchannel reforming reactor system is operated in a mass transfer-controlled regime, and provide the necessary criteria so that mass transfer limitations can be effectively eliminated in the reactor. Three-dimensional numerical simulations were carried out using computational fluid dynamics to investigate the essential characteristics of mass transport processes in a microchannel reforming reactor and to develop criteria for determining mass transfer limitations. The reactor was designed for thermochemically producing hydrogen from methanol by steam reforming. The mass transfer effects involved in the reforming process were evaluated, and the role of various design parameters was determined for the thermally integrated reactor. In order to simplify the mathematics of mass transport phenomena, use was made of dimensionless numbers or ratios of parameters that numerically describe the physical properties in the reactor without units. The results indicated that the performance of the reactor can be greatly improved by means of proper design of catalyst layer thickness and through adjusting feed composition to minimize or reduce mass transfer limitations in the reactor. There is not an effective method to reduce channel dimensions if the flow rate remains constant, or to reduce fluid velocities if the residence time is kept constant. The rate of the reforming reaction is limited by mass transfer near the entrance of the reactor and by kinetics further downstream, when the heat transfer in the autothermal system is efficient. Finally, the criteria that can be used to distinguish between different mass transport and kinetics regimes in the reactor with a first-order reforming reaction were presented.     

Millisecond methane steam reforming for hydrogen production: A computational fluid dynamics study

The potential of methane steam reforming to produce hydrogen in thermally integrated micro-chemical systems at short contact times was theoretically explored. Methane steam reforming coupled with methane catalytic combustion in microchannel reactors for hydrogen production was studied numerically. A two-dimensional computational fluid dynamics model with detailed chemistry and transport was developed. To provide guidelines for optimal design, reactor behavior was studied, and the effect of design parameters such as catalyst loading, channel height, and flow arrangement was evaluated. To understand how steam reforming can happen at millisecond contact times, the relevant process time scales were analyzed, and a heat and mass transfer analysis was performed. The importance of energy management was also discussed in order to obtain a better understanding of the mechanism responsible for efficient heat exchange between highly exothermic and endothermic reactions. The results demonstrated the feasibility of the design of millisecond reforming systems, but only under certain conditions. To achieve this goal, process intensification through miniaturization and the improvement in catalyst performance is very important, but not sufficient; very careful design and implementation of the system is also necessary to enable high thermal integration. The channel height plays an important role in determining the efficiency of heat exchange. A proper balance of the flow rates of the combustible and reforming streams is an important design criterion. Reactor performance is significantly affected by flow arrangement, and co-current operation is recommended to achieve a good energy balance within the system. The catalyst loading must be carefully designed to avoid insufficient reactant conversion or hot spots. Finally, operating windows were identified, and engineering maps for designing devices with desired power were constructed.     

Transient numerical modeling and model predictive control of an industrial-scale steam methane reforming reactor

A steam methane reforming reactor is a key equipment in hydrogen production, and numerical analysis and process control can provide a critical insight into its reforming mechanisms and flexible operation in real engineering applications. The present paper firstly studies the transport phenomena in an industrial-scale steam methane reforming reactor by transient numerical simulations. Wall effect and local non thermal equilibrium is considered in the simulations. A temperature profile of the tube outer wall is given by user defined functions integrated into the ANSYS FLUENT software. Dynamic simulations show that the species distribution is closely related to the temperature distribution which makes the temperature of the reactor tube wall an important factor for the hydrogen production of the reformer and the thermal conductivity of the catalyst network is crucial in the heat transfer in the reactor. Besides, there exists a delay of the reformer's hydrogen production when the temperature profile of the tube wall changes. Among inlet temperature, inlet mass flow rate and inlet steam-to-carbon (S/C) ratio, the mass flow rate is the most influencing factor for the hydrogen production. The dynamic matrix control (DMC) scheme is subsequently designed to manipulate the mole fraction of hydrogen of the outlet to the target value by setting the temperature profile trajectory of the reforming tube with time. The proportional-integral control strategy is also studied for comparison. The closed-loop simulation results show that the proposed DMC control strategy can reduce the overshoot and have a small change of the input variable. In addition, the disturbances of feed disturbance can also be well rejected to assure the tracking performance, indicating the superiority of the DMC controller. All the results give insight to the theoretical analysis and controller design of a steam methane reformer and demonstrate the potential of the CFD modeling in study the transport mechanism and the idea of combining CFD modeling with controller design for the real application.     

Constructal Parallel-Flow and Counterflow Microchannel Heat Sinks with Bifurcations

Based on the Constructal Theory, parallel-flow and counterflow microchannels heat sinks with bifurcations are put forward to manage the temperature nonuniformity and further reduce the temperature of microchannel heat sinks bottom plates. Several models with different lengths of bifurcations are designed, and the corresponding laminar fluid flow and heat transfer of all models have been investigated through numerical simulations. The pressure, velocity, temperature distributions, and averaged Nusselt numbers are analyzed in details, and then the overall thermal resistances and overall thermal performance are compared. The results show that the thermal performance of counterflow microchannel heat sinks is better than that of parallel-flow heat sinks for the same geometry, and bifurcation can improve the thermal performance for all cases. It is suggested that a proper design of the length of bifurcation counterflow microchannel can be employed to improve the overall thermal performance of microchannel heat sinks. The study complements and extends previous works.     

Characteristics of intraphase transport processes in methanol reforming microchannel reactors: A computational fluid dynamics study

Ignoring possible effects due to intraphase diffusion within catalyst layers is a common feature of computational fluid dynamics models developed for reforming microchannel reactors. Resistance to diffusion within the catalyst layers applied to such a reactor is often ignored on the grounds that the catalyst layers are sufficiently thin to allow reactants unrestricted access to all available reaction sites. However, this assumption is not necessarily correct, and intraphase diffusion effects could be important. Three-dimensional numerical simulations were carried out using computational fluid dynamics to investigate the characteristics of intraphase transport processes within the catalyst layers arranged in a thermally integrated methanol reforming microchannel reactor. The heat and mass transfer effects involved in the reforming process were evaluated, and the optimum thickness of catalyst layers was determined for the reactor. Particular focus was placed on how to optimize the thickness of catalyst layers in order to operate the reactor more efficiently. The results indicated that the performance of the reactor can be greatly improved by means of proper design of catalyst layer thickness to enhance heat and mass transfer into the catalyst layers. The thickness of the catalyst layers can be optimized to minimize diffusional resistance while maximizing methanol conversion and hydrogen yield. Thick catalyst layers offer higher reactor performance, whereas thin catalyst layers improve catalyst utilization and thermal uniformity. The thickness scale at which intraphase diffusion effects become noticeable was finally determined on the basis of reactor performance. The critical thickness was found to be about 0.10 mm, and catalyst layers should be designed beyond this dimension to achieve the desired level of conversion. The critical thickness will vary depending upon layer properties and operating conditions.     

Numerical simulation of heat-pipe and folded reformers for efficient hydrogen production through methane autothermal reforming

In order to intensify the methane autothermal reforming (ATR) process for efficient hydrogen production, novel heat-pipe and the folded reactors were designed and studied by numerical simulations. The reactor performance, such as methane conversion rate, hydrogen yield, and temperature difference between the reactor inlet and outlet, was computed and compared for both traditional tubular reactors and the novel reactors. Under the optimum operating parameters, compared with the tubular reactor, the heat pipe reactor and the folded reactor can help to increase methane conversion rate from 34% to 45% and 50%, while hydrogen productivity from 22.2% to 28.6% and 31.4%, respectively. The performance of the heat pipe reactor depends on the length and position of the heat pipe, while for the folded reactor, thicker intermediate plate with higher thermal conductivity material is more beneficial. Results were compared with previous experiments and could be used as a reference to guide new experimental and theoretical works toward the ultimate goal of designing and optimizing the ATR reactors for hydrogen production in the future.     

Modeling of double-layer triangular microchannel heat sink based on thermal resistance network and multivariate structural optimization using firefly algorithm

Abstract

The micro-channel heat dissipation system has minor specifications and good thermal conductivity per unit, which is the best choice for heat dissipation of micro-chips. By optimizing the cross section of microchannel, the heat exchange efficiency and temperature uniformity can be effectively improved. In this article, a double-layer triangular microchannel heat sink is proposed, which uniquely combines triangular cross section and double-layer structure to obtain a better heat dissipation performance. A new thermal resistance network model is established. At the same time, the model of pressure drop in microchannel heat sink is obtained by use of fluid theory. Taking thermal resistance and pressure drop as optimization objectives, the thermal resistance of double-layer triangular microchannel heat sink is 0.284?K/W and the pressure drop is 1386.89?Pa by using the firefly algorithm based on the Pareto optimal solution set, obtaining the optimal structural parameters. The thermal-flow-solid coupling simulation analysis shows that the thermal resistance and theoretical analysis error is 5.19%, and the pressure drop and theoretical analysis error is 9.49%, which can verify the accuracy of the thermal resistance network model. This article has a guiding significance for the thermal resistance analysis and heat dissipation improvement of non-rectangular cross section microchannel heat sinks.     

Constructal design and thermal analysis of microchannel heat sinks with multistage bifurcations in single-phase liquid flow

Based on constructal theory, five different cases with multistage bifurcations are designed as well as one case without bifurcations, and the corresponding laminar fluid flow and thermal performance have been investigated numerically. All laminar fluid flow and heat transfer results are obtained using computation fluid dynamics, and a uniform wall heat flux thermal boundary condition is applied all heated surfaces. The inlet velocity ranges from 0.66 m/s to 1.6 m/s with the corresponding Reynolds number ranging from 230 to 560. The pressure, velocity, temperature distributions and averaged Nusselt number are presented. The overall thermal resistances versus inlet Reynolds number or pumping power are evaluated and compared for the six microchannel heat sinks. Numerical results show that the thermal performance of the microchannel heat sink with multistage bifurcation flow is better than that of the corresponding straight microchannel heat sink. The heat sink with a long bifurcation length in the first stage (Case 1A) is superior. The usage of multistage bifurcated plates in microchannel heat sink can reduce the overall thermal resistance and make the temperature of the heated surface more uniform (Case 3). It is suggested that proper design of the multistage bifurcations could be employed to improve the overall thermal performance of microchannel heat sinks and the maximum number of stages of bifurcations is recommended to be two. The study complements and extends previous works.     

Three-dimensional numerical optimization of a manifold microchannel heat sink

A three-dimensional analysis procedure for the thermal performance of a manifold microchannel heat sink has been developed and applied to optimize the heat-sink design. The system of fully elliptic equations, that govern the flow and thermal fields, are solved by a SIMPLE-type finite volume method, while the optimal geometric shape is traced by a steepest descent technique. For a given pumping power, the optimal design variables that minimize the thermal resistance are obtained iteratively. The procedure is robust and the optimal state is reached within six global iterations. Comparing with the comparable traditional microchannel heat sink, the thermal resistance is reduced by more than a half while the temperature uniformity on the heated wall is improved by tenfold. The sensitivity of the thermal performance on each design variable is also examined and presented in the paper. Among various design variables, the channel width and depth are more crucial than others to the heat-sink performance. The optimal dimensions and corresponding thermal resistance have a power-law dependence on the pumping power.     

Comparison of steam and autothermal reforming of methanol using a packed-bed low-cost copper catalyst

Small-scale reformers for hydrogen production via steam and autothermal reforming of hydrocarbon feedstocks can be a solution to the lack of hydrogen distribution infrastructure. A packed-bed reactor is one possible design for such purpose. However, the two reforming processes of steam and autothermal methods have different characteristics, thus they have different and often opposite design requirements. In implementing control strategy for small-scale reformers, understanding the overall chemical reactions and the reactor physical properties becomes essential. This paper presents some inherent features of a packed-bed reactor that can both improve and/or degrade the performance of a packed-bed reactor with both reforming modes.The high thermal resistance of the packed bed is disadvantageous to steam reforming (SR), but it is beneficial to the autothermal reforming (ATR) mode with appropriate reactor geometry. The low catalyst utilization in steam reforming can help to prevent the unconverted fuel leaving the reactor during transient by allowing briefly for higher reactant fuel flow rates. In this study, experiments were performed using three reactor geometries to illustrate these properties and a discussion is presented on how to take advantages of these properties in reactor design.     

Autothermal hydrogen generation from methanol in a ceramic microchannel network

In this paper, the authors present the first demonstration of a new class of integrated ceramic microchannel reactors for all-in-one reforming of hydrocarbon fuels. The reactor concept employs precision-machined metal distributors capable of realizing complex flow distribution patterns with extruded ceramic microchannel networks for cost-effective thermal integration of multiple chemical processes. The presently reported reactor is comprised of five methanol steam reforming channels packed with CuO/γ-Al₂O₃, interspersed with four methanol combustion channels washcoated with Pt/γ-Al₂O₃, for autothermal hydrogen production (i.e., without external heating). Results demonstrate the capability of this new device for integrating combustion and steam reforming of methanol for autothermal production of hydrogen, owing to the axially self-insulating nature of distributor-packaged ceramic microchannels. In the absence of any external insulation, stable reforming of methanol to hydrogen at conversions >90% and hydrogen yields >70% was achieved at a maximum reactor temperature of 400 °C, while simultaneously maintaining a packaging temperature <50 °C.     

Numerical analysis of methanol steam reforming reactor heated by catalytic combustion for hydrogen production

Thermal coupling of endothermic and exothermic reactions is an important pathway for integrated thermal management within a methanol steam reforming reactor heated by methanol catalytic combustion. In this study, a numerical model is developed for heat and mass transfer calculations, methanol steam reforming and catalytic combustion reactions, which is used to explore the effects of design parameters on compact parallel channel reactor performance. Efficiency of the integrated reactor is optimized by the coupling of endothermic and exothermic reactions using conventional wall material. Temperature uniformity is improved by the adjustment of the flow arrangement and the catalyst distribution. This work provides an effective energy management strategy and tool which can be adopted in the design of portable hydrogen generation systems.     

System performance of a combined heat and mass recovery adsorption cooling cycle: A parametric study

Based on the previous work of the authors [K.C. Leong, Y. Liu, Numerical study of a combined heat and mass recovery adsorption cooling cycle, Int. J. Heat Mass Transfer 47 (2004) 4761–4770], a numerical study of the effects of system design and operation parameters on the performance of a combined heat and mass recovery adsorption cycle is presented in this paper. The effects of bed dimensions, bed thermal conductivity, heat exchange fluid velocity, driven temperature and the degree of the heat recovery on the system performance are investigated. It is found that an increase in the driven temperature results in the increase of both the coefficient of performance (COP) and specific cooling power (SCP) of the adsorption cycle. On the other hand, the system performance can be severely deteriorated for velocities of the heat exchange fluid smaller than a critical value. An increase in the bed thickness will result in an increase in COP and a decrease in the SCP. The results of our simulations will provide useful guidelines for the design of this type of advanced adsorption cooling cycle.     

Performance analysis of a high-temperature magnesium hydride reactor tank with a helical coil heat exchanger for thermal storage

Metal hydrides are regarded as one of the most attractive options for thermal energy storage (TES) materials for concentrated solar thermal applications. Improved thermal performance of such systems is vitally determined by the effectiveness of heat exchange between the metal hydride and the heat transfer fluid (HTF). This paper presents a numerical study supported by experimental validation on a magnesium hydride reactor fitted with a helical coil heat exchanger for enhanced thermal performance. The model incorporates hydrogen absorption kinetics of ball-milled magnesium hydride, with titanium boride and expanded natural graphite additives obtained by Sievert's apparatus measurements and considers thermal diffusion within the reactor to the heat transfer fluid for a realistic representation of its operation. A detailed parametric analysis is carried out, and the outcomes are discussed, examining the ramifications of hydrogen supply pressure and its flow rate. The study identifies that the enhancement of thermal conductivity in magnesium hydride has an insignificant impact on current reactor performance.     

Cooling performance of a microchannel heat sink with nanofluids

In this paper, the cooling performance of a microchannel heat sink with nanoparticle–fluid suspensions (“nanofluids”) is numerically investigated. By using a theoretical model of thermal conductivity of nanofluids that accounts for the fundamental role of Brownian motion, we investigate the temperature contours and thermal resistance of a microchannel heat sink with nanofluids such as 6 nm copper-in-water and 2 nm diamond-in-water. The results show that the cooling performance of a microchannel heat sink with water-based nanofluids containing diamond (1 vol.%, 2 nm) at the fixed pumping power of 2.25 W is enhanced by about 10% compared with that of a microchannel heat sink with water. Nanofluids reduce both the thermal resistance and the temperature difference between the heated microchannel wall and the coolant. Finally, the potential of deploying a combined microchannel heat sink with nanofluids as the next generation cooling devices for removing ultra-high heat flux is shown.     

Methane steam reforming in a novel ceramic microchannel reactor

Microchannel heat exchangers and reactors can deliver very high performance in small packages. Such heat exchangers are typically fabricated from aluminum, copper, stainless steel, and silicon materials. Ceramic microchannel reactors offer some significant advantages over their metallic counterparts, including very-high-temperature operation, corrosion resistance in harsh chemical environments, low cost of materials and manufacturing, and compatibility with ceramic-supported catalysts. This work describes a ceramic microchannel reactor that achieves process intensification by combining heat-exchanger and catalytic-reactor functions to produce syngas. A complete computational fluid dynamics (CFD) model as well as a geometrically simplified hybrid CFD/chemical kinetics model is used in conjunction with experimentation to examine heat transfer, fluid flow, and chemical kinetics within the ceramic microchannel structure. Heat-exchanger effectiveness of up to 88% is experimentally demonstrated. Reactive heat-exchanger performance for methane-steam reforming reaches 100% methane conversion and high selectivity to syngas at a gas hourly space velocities (GHSV) of 15,000 h⁻¹. Model results agree well with experimental data and provide insight into physical processes underway during reactor operation.     

Analysis of phase change heat transfer with annulus 1 kW class methanol steam reforming reaction under high-pressure operation

A fuel cell air independent propulsion (AIP) system of underwater vehicle requires a hydrogen storage system. The methanol steam reforming system is a candidate of hydrogen storage which can produce hydrogen from chemical reaction. Different from reforming system for station fuel cell system, the methanol steam reformer (MSR) for underwater vehicle requires high-pressure operation.Since the longitudinal temperature uniformity is a core parameter of conversion efficiency of steam reforming system, this study is focused on computational analysis of phase change heat transfer through the annulus for methanol steam reforming reaction. The annulus MSR using phase change material was developed to improve the temperature uniformity. The simulation model is verified with safety and performance analysis code (SPACE). The performance parameters of MSR were flow arrangement, steam to carbon ratio (SCR), and gas hourly space velocity (GHSV). The results were analyzed in terms of the hydrogen yield, heat flux, liquid mass flow rate, and methanol conversion rate. The flow arrangement varied the methanol conversion rate to a minor extent of approximately 0.1% because wall temperature was maintained uniformly. In the case of SCR, the hydrogen yield at SCR 2.5 was 0.637 (dry basis), which was the highest yield rate. Also, if GHSV was increased, hydrogen yield decreased from 0.690 (dry basis) to 0.527 (dry basis). The heat transfer pattern was also analyzed and it was found that steam is interactively condensed along with the progress of the reforming reaction.