Monolithic reactors catalyst incorporation

Tronconi et al. [46] developed a fully transient two-phase 1D + 1D mathematical model of an SCR honeycomb monolith reactor, where the intrinsic kinetics determined over the powdered SCR catalyst were incorporated, and which also accounts for intra-porous diffusion within the catalyst substrate. Accordingly, the model is able to simulate both coated and bulk extruded catalysts. The model was validated successfully against laboratory data obtained over SCR monolith catalyst samples during transients associated with start-up (ammonia injection), shut-down (ammonia... 

In this chapter, modeling of monolith reactors will be considered from a first-principles point of view, preceded by a discussion of the typical phenomena in monoliths that should be taken into account. General model equations will be presented and subsequently simplified, depending on the subprocesses that should be described by a model. A main lead will be the time scales at which these subprocesses occur. If they are all small, the process operates in the steady state, and all time-dependent behavior can be discarded. Unsteady-state behavior is to be considered if the model should include the time scale of reactor startup or if deactivation of the catalyst versus time-on-stream has to be addressed. A description of fully dynamic reactor operation, as met when cycling of the feed is applied, requires that all elementary steps of a kinetic model with their corresponding time scales are incorporated in the reactor model. 

The U.S. Department of Energy is also investigating the performance of monolithic reactors using the same cell configuration as General Motors. The catalyst used was Selectra PROX I (BASF Catalysts, LLC), which was used to generate a data set that was incorporated into a correlation that enable them to model different staged reactors. They developed an empirical correlation for selectivity toward CO... 

Firstly, there are technical reasons concerning catalyst and reactor requirements. In the chemical industry, catalyst performance is critical. Compared to conventional catalysts, they are relatively expensive and catalyst production and standardization lag behind. In practice, a robust, proven catalyst is needed. For a specific application, an extended catalyst and washcoat development program is unavoidable, and in particular, for the fine chemistry in-house development is a burden. For coated systems, catalyst loading is low, making them unsuited for reactions occurring in the kinetic regime, which is particularly important for bulk chemistry and refineries. In that case, incorporated monolithic catalysts are the logical choice. Catalyst stability is crucial. It determines the amount of catalyst required for a batch process, the number of times the catalyst can be reused, and for a continuous process, the run time. 

The cleaning of flue gases from stationary sources is another field in which the application of monolithic catalysts will certainly rise. There will be no versatile catalyst for cleaning all off-gases. Therefore tailor-made catalysts with zeoliths of various types for specific applications will be developed. Incorporated-type monolithic catalysts are likely to prevail in this field. Since cleaning usually requires a set of equipment items in series (e.g., converter, heat exchangers), multifunctional reactors (reverse-flow reactors, rotating monoliths) will become more common. 

Along with the inclusion of heterogeneous metal catalysts in continuous flow reactors, numerous authors have evaluated the advantages associated with the incorporation of acid and base catalysts in these reaction systems, using a range of packed beds, monoliths, and wall-coated reactors. 

Depending on the application, different kinds of support geometries such as pellets, monolithic honeycomb stmctures and fibers are used. Pressure drop induction becomes of importance when incorporating a catalyst to the reactor system. Pellets can contribute to relatively higher pressure drops. The monolithic honeycomb stmctures are technologically advanced and can offer low pressure drop induction. They are predominantly applied for environmental catalysis applications and hydrogen peroxide production. In order to lower the pressure drop in... 

A microstructured monolith for autothermal reforming of isooctane was fabricated by Kolb et cd. from stainless steel metal foils, which were sealed to a monohthic stack of plates by laser welding [73]. A rhodium catalyst developed for this specific application was coated by a sol-gel technique onto the metal foils prior to the sealing procedure. The reactor carried a perforated plate in the inlet section to ensure flow equi-partition. At a weight hourly space velocity of 316 L (h gcat). S/C 3.3 and O/C 0.52 ratios, more than 99% conversion of the fuel was achieved. The temperature profile in the reactor was relatively flat. It decreased from 730 °C at the inlet section to 680 °C at the outlet. This was attributed to the higher wall thickness of the plate monolith compared with conventional metallic monolith technology. The reactor was later incorporated into a breadboard fuel processor (see Section 9.5). 

Unfortunately, the widely used flow reactors (for example, microreactors, multi-cell flow reactors, and disk reactors) do not tolerate solid particulates and precipitates, which would clog the miniaturized flow devices. Therefore, immobilization of the reagents/catalysts by a solid support is of significant importance in this field. Hence, a broad range of solid supports have been employed to incorporate the reagent/ catalyst into the reactors, including packed-beds, monoliths, and other systems that exploit the high surface-to-volume areas obtained in microchannel devices. 

Structured reactors such as monoliths have several obvious advantages over the traditional reactor randomly filled with catalyst particles [1]. They have lower pressure drop, uniform flow distributions, less hot-spot formation and uniform residence times. However, these catalytic systems have low surface areas, making it necessary to incorporate some phase like alumina or silica, which increases the surface area. 

---