Research Article |
Corresponding author: Alexandr V. Avdeenkov ( avdeyenkov@mail.ru ) Academic editor: Georgy Tikhomirov
© 2022 Alexandr V. Avdeenkov, Sergey G. Kalyakin, Sergey L. Soloviev, Huong Duong Quang.
This is an open access article distributed under the terms of the CC0 Public Domain Dedication.
Citation:
Avdeenkov AV, Kalyakin SG, Soloviev SL, Duong Quang H (2022) On the scalability of the operating capacity of hydrogen recombiners. Nuclear Energy and Technology 8(2): 143-152. https://doi.org/10.3897/nucet.8.83223
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One of the main factors in the capacity of passive autocatalytic recombiners (PARs) is its productivity or the hydrogen removal rate. In this work it was demonstrated that regardless of the type of a recombiner, the hydrogen removal rate is mostly determined by the catalytic surface area and the molar density of hydrogen at the inlet. It means that the performance of a recombiner should obey geometric and physical scalability.
Geometric scalability is characterized by the retention of the specific (per unit area of the catalytic surface) hydrogen removal rate with increasing the size of the recombiner by increasing the inlet section while maintaining the height and design of the catalytic unit.
Physical scalability is characterized by maintaining the hydrogen removal rate of the recombiner at a constant input molar density of hydrogen in an air-hydrogen environment while simultaneously changing the input temperature and pressure.
For a numerical demonstration of scalability, several calculations were performed with different initial hydrogen concentrations, external conditions and amounts of catalytic elements. It was shown that, regardless of the number of catalytic plates in the recombiner, the specific removal rate of hydrogen will remain unchanged and that under different external conditions (temperature, pressure), in case they correspond to the same inlet hydrogen density, the hydrogen removal rate does not change.
recombiner, scalability, chemical kinetics, hydrogen removal rate
The most common practice of removing hydrogen from the enclosure vessel (EV) of a nuclear plant is based on the principle of passive catalytic hydrogen recombination using catalytic elements containing some catalysts (
The passive autocatalytic recombiner (PAR) has a standard design with a catalytic unit placed at the bottom of a rectangular steel tube (as a rule) with an open outlet. The exit part is blind from above, one or several side parts at the exit are covered with a metal mesh (lattice). When hydrogen appears in the internal volume of the recombiner, an exothermic reaction of hydrogen and oxygen recombination into water begins on the catalytic surface, which ensures the onset of natural convection. PAR does not require external power supply or any control.
Recombiners of the RVK line (
The full-scale validation of large recombiners is usually very difficult. Therefore, most experimental studies are carried out on recombiners such as RVK-500, RVK-1000, or on separate modules of large recombiners. The largest PAR of this line, RVK-4, consists of four identical modules. RVK-3 consists of two of the same modules (
One of the basic characteristics of a recombiner is its productivity (or hydrogen removal rate). The estimates show that the release of hydrogen during a severe accident at NPPs (like VVER-1000 and similar) can range up to several hundred kilograms per hour depending on the scenario of the accident, the type and size of the reactor. The productivity of recombiners is sometimes given in terms of the inlet area. PARs on the average show a hydrogen removal rate (at 4 vol% and a pressure of 1 bar) in the region of 3–7 kg per hour and per 1m2 inlet section (
It should be noted that the performance characteristics of the recombiners declared by the manufacturers were frequently obtained for quite specific external conditions, namely in a quiescent environment in which the recombiner is self-starting in the natural circulation mode.
Under real conditions of a possible severe accident, the characteristics derived for such experimental conditions are hardly justified in being used for numerical simulation of the accident, since the characteristics of the recombiner essentially depend on the rate of hydrogen-air flow into the recombiner (
For the RVK line of recombiners, the hydrogen removal rate was measured at an initial hydrogen concentration of less than 1% to over 11vol.%. Based on the experimental data, empirical correlations for hydrogen removal rate have been derived in (
G(g/s)=n×C×[a0 +a1×(C-2)+a2×(C-2)2], (1)
а0=1.43+0.24×(Р-1)+0,005×(Т-20),
а1=0.12+0.0031×(Р-1)+0,0003×(Т-20),
а2=0.009×(Р-1)+1,08×10-4×(Т-20)-1,54×10-5× (Т-20)×(Р-1),
n=0.0077 for RVK-500,
n=0.0183 for RVK-1000,
n= 0,16 for RVK-4,
where C (vol.%)- the volume concentration of H2, Р (bar)- pressure, Т (°C) – temperature.
The resulting dependencies are purely empirical and we do not know if there are any verification calculations to justify the recombiner performance outside the experimental conditions.
The similar experimental approach to investigating the global behaviour of a recombiner in a larger environment has been performed for the AREVA type of recombiners. The derived empirical correlations (
The empirical correlations (1) make it possible to determine the specific hydrogen removal rate of the catalytic elements (hydrogen removal rate per unit surface area of the catalyst). Fig.
The last statement can be justified as follows. At a low concentration the recombination takes place at catalyst surfaces and the area of those surfaces mostly determines the hydrogen removal rate while the geometry of catalytic elements (plates or rods and their relative positions) plays a minor role. At a higher concentration the recombination takes place both at catalyst surfaces and in gas phases in a recombiner volume and thus the geometry of a catalyst unit may define “the concentration of the ignition” of the air- hydrogen mixture.
It is reasonable to suggest that in case of severe accidents with a significant release of hydrogen, the environmental conditions around recombiners are not necessarily those for which the above correlations (Fig.
Regardless of the type of a recombiner, the hydrogen removal rate is mostly determined by the catalytic surface area and the mass density of hydrogen at the inlet. It means that the performance of a recombiner should obey geometrical and physical scalability.
To demonstrate such scalabilities for hydrogen removal rates, several calculations were performed with different initial hydrogen concentrations, external conditions and amounts of catalytic elements.
Here two types of a scalability are determined and considered that can be used to construct a realistic numerical model of the performance of recombiners.
Geometric scalability is characterized by the retention of the specific (per unit area of the catalytic surface) hydrogen removal rate while increasing the size of the recombiner by increasing the inlet section while maintaining the height and design of the catalytic unit. In this case, also, the hydrogen removal rate increases in proportion to the increase of the inlet section.
Physical scalability is characterized by the same hydrogen removal rate of the recombiner at the same inlet molar density of hydrogen with a simultaneous change in the inlet temperature and pressure. Here and below, we assume that the oxygen is in excess in the gas mixture for the hydrogen oxidation. In general, the “air” may contain water vapor and other gases.
Geometric scalability was rather closely investigated even in experimental works at Sandia National Laboratories on the Surtsey experimental setup (
Three samples were used in the experiment: ½, ¼, 1/8 of the full-scale prototype (size of the inlet section 1mx1m), consisting of two rows of 44 cartridges (1/2 – 44 (one row), ¼ – 22 , 1/8 – 11). Each cartridge is 0.45mx0.2mx0.01m in size. The scaling effect (proportional to the number of cartridges) was investigated in a mixture of 0.107Mpa of air and 0.107Mpa of steam. In the study, it was noted that “simple” forward scaling was only observed at low hydrogen concentrations; at high concentrations, a normalization factor was introduced to consider the incomplete mixing in the lower part of the setup and to take into account this heterogeneity in the model when processing the results.
Experimental scaling studies of this kind were carried out with recombiners of the KPAR line (
Fig.
Fig.
The physical scalability is a direct consequence of the fact that we can treat our system as the mixture of ideal gases. Using the equation of state it is easy to derive that the inlet hydrogen molar density CM=PC/(RT), where P is the pressure, T is the temperature, R is the gas constant and C is the volumetric hydrogen concentration at inlet. It means that CM is defined by the (P/T) ratio at fixed C.
Fig.
Moreover, we found that the physical scalability may work even in a broader way. If some sets of data for P (in bar), T(in °C) and C (in%) provide rather similar values of CM then it is expected to have a very similar hydrogen removal rate as well. For example, sets of (P, T, C) with (3, 70, 4) and (4, 100, 3.32) provide the removal rate 0.13g/s and 0.121g/s consequently; sets with (2, 140, 4.88) and (4, 100, 2.22) provide the removal rate 0.087g/s and 0.079g/s consequently. Using the data presented on Fig.
The considered examples of geometrical and physical scalabilities are based on the available and presented here experimental data (
In this study, chemical kinetics of the catalytic recombination of hydrogen was analyzed with the use of the CHEMKIN format (
Here we have used a detailed chemical reaction mechanism (the multistep reaction model) for the hydrogen oxidation on the catalyst surface. The surface kinetic model and associated rate expressions are largely based on previous work on oxidation reactions over Pt (
The catalyst sheets (stainless steel coated with washcoat/platinum catalyst material) are arranged in parallel forming vertical rectangular flow channels. Such a set-up represents a box-type recombiner section of AREVA,
The experimental setup of the REKO-3 facility contains only 4 catalyst sheets. Here we used a 2D approach in a way it was done in
In order to verify our approach on the RVK type catalyst we use some experimental data reported in
In order to calculate the hydrogen concentration, sensors were fixed in two places (Fig.
In this work, to verify our approach, we have used the data when the hydrogen concentration at the inlet is 4%, and the total mass flow rate of the gas mixture is 35 grams per minute. The rest of the experimental data can be found in
Fig.
All temperature profiles shown in Fig.
The experimental value of the hydrogen concentration at the point where the sensor is located above the rods is 1.82 vol.%, The calculated value is 1.58 vol.%, which can also be noted as quite acceptable accuracy.
Thus, we have checked the applicability of the multistep hydrogen recombination mechanism on the available experimental data for both the AREVA plate recombiner and the RVK-type rod recombiner, and in the future, this approach can be used to construct a CFD model of the recombiner and test the scalability.
Since the catalytic unit of the recombiner consists of a large number of geometrically identical objects, in most cases there is no need to calculate its characteristics with all tens of catalytic plates or hundreds of rods. It is enough to do it and verify it for the minimal possible geometry – the selected unit cell, as, for example, it was done for the verification of the REKO-3 experiments
We have done some demo calculations to test geometric scalability. The calculations were performed for flow regimes with an initial temperature of 300 K, an initial hydrogen concentration of 4vol.%, an initial velocity of a hydrogen-air mixture of 0.8 m/s, and an initial hydrogen concentration of 8%, an initial velocity of 3 m/s. A square packing of rods was considered. The radius of the catalyst rod is R = 0.0025 m, height = 64 mm, the distance between the centers of the rods is d = 12.5 mm, the distance between the centers of the rods and the walls is d = 12.5 mm (for the variant where the effect of the wall of the recombiner box is taken into account). The simplest cell of a square packing, a symmetric cell, contains four quarters of rods (Fig.
Figs
Another interesting feature of scaling is the scaling, which we call physical. Namely, for a given volumetric hydrogen concentration and the same inlet temperature to pressure ratios, which corresponds to the same initial hydrogen density, the density distribution is maintained throughout the cell (Fig.
In this study it was shown that regardless of the type of geometry of the catalytic elements in a recombiner, and to the main extent, the hydrogen removal rate is determined by the area of the catalytic surface and the molar density of hydrogen at the inlet. Here we only considered the cases with oxygen excess conditions. We presume that oxygen deficiency cases as well as the presence of carbon monoxide and steam should not change the effects of scalability. But it will be studied elsewhere.
We analyzed the existing empirical dependencies for hydrogen removal rates of two types of recombiners and fulfilled a number of CFD calculations using the STAR CCM + code.
An essential part of the approach is the use of a detailed chemical reaction mechanism (the multistep reaction model) for the hydrogen oxidation on the catalysts surface. This approach possesses more universality for determining the hydrogen removal rate both under natural circulation conditions and under conditions of forced circulation in the area of the location of recombiners, which is clearly necessary for the numerical justification of severe accidents with hydrogen release.
Numerical examples were used to demonstrate the geometric and physical scalability of the functioning of the catalytic elements, which can be and will be used to construct an advanced CFD model of the recombiner and its more numerically realizable interaction with the hydrogen-air environment in emergency modes.