1. Introduction
The internal-loop airlift reactor (ILAR) is a type of multiphase reactor developed from the bubble column reactor (BCR), which combines the advantages of BCRs and stirred tank reactors and has characteristics such as a simple structure, no rotating parts, low energy consumption, low and uniform shear force, large liquid holding capacity, and excellent mass transfer and mixing performance [
1,
2,
3]. Since the development of ILARs in the last century, it has been intensively used in chemical engineering, bioengineering and environmental protection [
4], Fischer–Tropsch synthesis [
5], coal liquefaction [
6], fermentation [
7], cell culture [
3], desulfurization [
8], wastewater treatment [
9], and volatile organic compound removal [
10].
Despite their unique advantages, ILARs also have some drawbacks that need to be addressed, such as poor mixing efficiency in high-viscosity systems and low gas holdup in the downcomer region, which can lead to a decrease in overall reactor efficiency. This poses certain challenges to the design, development, and scale-up of ILARs. To improve the low gas holdup in the descending zone of the single-stage internal-loop airlift reactor (SSALR) and further enhance mass transfer and mixing, the draft tube can be segmented to form a multistage ILAR [
11].
Compared with the SSALR, the multistage ILAR has many advantages, such as higher gas holdup and mass transfer coefficient, and it has received extensive attention in recent years [
12,
13]. Ramonet et al. [
14] used CFD to simulate the fluid flow of ILARs with different geometric structures, including single- and two-stage draft tubes. It was found that, among the three geometric structures (squared, cylindrical, and cylindrical with coned bottom), the squared structure had higher liquid velocity, higher turbulent kinetic energy, and shorter loop circulation time. In terms of the single- and two-stage structures, the upper turbulent kinetic energy of the two-stage structure was higher. Additionally, Ramonet et al. [
13] also used CFD simulation to optimize the structure of a two-stage ILAR, studying the effects of ten different geometric structures (including draft tube placement, liquid height, interstage height, and draft tube diameters) on hydrodynamic performance. It was found that the placement of the draft tube had a significant effect on the hydrodynamic behavior. For the two-stage ILAR with a coned bottom, the liquid velocity increased with the decrease in the interstage height. The fluid flow in the reactor was simulated using CFD to correctly predict the hydrodynamic characteristics, which is a trend in reactor design and development. This study provided valuable insights for optimizing the structure of two-stage ILAR through CFD simulation, which is helpful in developing more efficient bioreactors. To inhibit liquid back mixing between the stages of a two-stage ILAR, Shi et al. [
15] proposed a contraction–expansion guide vane. CFD simulation and experimental results showed that the internals generated local circulation flows at each stage rather than overall circulation flow, which increased the overall gas holdup by 1.98 times. Tao et al. [
11] investigated gas–liquid–solid three-phase hydrodynamics and mass transfer in a pilot-scale multistage ILAR. It was found that increasing the superficial gas velocity can improve the gas holdup, liquid circulating velocity, and mass transfer coefficient, and shorten the mixing time in the gas–liquid flow, while the addition of solid particles has the opposite effect. Li et al. [
12] investigated the local hydrodynamics and bubble characteristics of gas–liquid–solid three-phase in a two-stage ILAR. The results showed that increasing solid holdup and superficial gas velocity can promote the transition of the bubble circulation regime in the second stage (upper), and the gas holdup in the second stage is higher. In view of the relatively few studies on the local hydrodynamic characteristics of multistage ILAR in three-phase systems, this work is helpful for obtaining a deeper understanding of multistage ILAR. Zhang et al. [
16] experimentally studied the influence of screen internals on hydrodynamics and mass transfer of a two-stage ILAR. The results indicated that the screen can effectively break bubbles up and make the radial bubble velocity distribution more uniform. Appropriate screens can improve the gas holdup and mass transfer coefficient. Li et al. [
17] measured the radial distribution of bubble characteristics in each stage of the three-stage ILAR using dual electrical resistivity probes. The results showed that the bubble frequency, bubble size, gas holdup, and bubble velocity in each stage increased, and the distributions became wider with increasing the superficial gas velocity. Moreover, the bubble size and gas holdup in the second and third stages were almost radially uniform at low superficial gas velocity. Li et al. [
18] also measured the local hydrodynamics in a three-stage ILAR using dual electrical resistivity probes and conductivity cells. The Zuber and Findlay drift flux model [
19] was used to express the correlation of slip velocity with the total gas–liquid velocity, and it fitted the experimental data very well. Compared with the SSALR, the fluid flow in the multistage ILAR is more complex. A detailed study of the local hydrodynamic characteristics in each stage, such as bubble size and liquid circulating velocity, can help us better understand the multistage ILAR. The work of Li et al. [
17,
18] provided valuable insight for related research. Behin [
20] investigated the mixing performance of a modified airlift loop reactor with a double-draft tube using the classical tracer response technique. The experimental results showed that, compared with a conventional concentric-tube airlift reactor, the mixing time and circulation time of the reactor were reduced by 48.3% and 35.5% in the homogeneous flow regime, respectively.
Yu et al. [
21] proposed a novel interstage internal, which can inhibit the liquid back mixing and provide for a homogeneous suspension of solid particles in the multistage ILAR. In a related research study, the effect of two types of interstage internals (perforated plate and perforated plate with three long tubes) on liquid back-mixing was investigated, and the results suggested that the perforated plate with tubes could provide a more uniform distribution of solid particles in different stages [
21]. Other studies investigated three bubble circulation regimes [
22], the influences of the opening ratio of the internal on the gas and liquid channels and the effect of superficial gas velocity on the height of the gas layer below the internal [
23], and the experimental and theoretical analyses of the different types of operations (concurrent, countercurrent, and batch) [
24]. Mohanty et al. [
25,
26] proposed a novel multistage external-loop airlift reactor. It was found that the gas holdup of the multistage structure was 45% higher than that of the single-stage structure, and the mass transfer performance was better. Sarkar et al. [
27] established a mathematical model that can predict the hydrodynamics of the three-stage external-loop airlift reactor, and the predicted values agreed well with the experimental data. Liu et al. [
28] used a bubble column reactor and a two-stage ILAR to culture aerobic granules. It found that the two-stage ILAR had the characteristic of long-term stable operation compared with the bubble column reactor.
Until now, there have been relatively few research reports on the fluid flow behavior in multistage ILARs, and most of them only investigate a single reactor structure. Therefore, in order to better explore the substantive effect of multistage structure, comparative analysis and further research should be conducted on different reactor configurations, such as multistage, single-stage, and bubble columns. Additionally, some internals were designed and developed to enhance the performance of multistage ILARs [
15,
24]. However, their more complex geometric structures may lead to energy consumption, as well as installation and operational difficulties in industrial applications. In this case, the simple multistage structure has much broader application. Finally, most experimental setups reported in the literature only involve bench-scale testing, using reactors with diameters less than 0.2 m.. However, the experimental data from bench-scale reactors can hardly satisfy the demands of the scale-up design of industrial reactors due to insufficient consideration of scale-up effects. Therefore, there is an urgent need for a systematic investigation of the hydrodynamics, mass transfer, and mixing performance of pilot-scale multistage ILARs.
In this work, the effects of three reactor structures, namely a BCR, an SSALR, and a four-stage internal-loop airlift reactor (FSALR), on mass transfer and mixing performance were systematically investigated in a pilot-scale transparent cylindrical column. The aim of this study was to provide a quantitative basis and theoretical support for the development and design of multistage ILARs. The axial liquid velocity was measured using a modified Pavlov tube technique, the volumetric mass transfer coefficient was calculated based on dynamic dissolved oxygen curve measurements, and the mixing time was determined using tracer response techniques.
2. Experimental Work
The experimental apparatus is shown in
Figure 1. The structures of the three reactors are displayed in
Figure 2. The ILAR was constructed from transparent Plexiglas, with an inner diameter of 0.484 m and a height of 5.5 m. The outer diameter of the draft tube of the SSALR was 0.35 m, with a wall thickness of 5 mm and a length of 4 m. An FSALR was built by dividing the draft tube into four equal parts, with each segment length of 1 m and segment spacing of 6 cm. The same ladder distributor with an opening diameter of 1 mm was employed for all three reactor structures. Air and tap water were used as experimental media, and all experiments were carried out in a semi-batch operation, with continuous gas phase and intermittent liquid phase. Before each experiment, tap water in a water tank was injected into the reactor through a centrifugal pump, with the liquid level controlled at a height of 4.5 m. The air was compressed using a screw air compressor, and the flow rate was regulated with a rotameter. It was redistributed through the sparger at the bottom of the reactor and then entered the draft tube. All experiments were conducted at room temperature and atmospheric pressure. The superficial gas velocity is defined as the ratio of gas flow to the cross-sectional area of the reactor, that is, the linear velocity of gas. In order to comprehensively investigate the hydrodynamic characteristics in different flow regimes, the superficial gas velocity range was from 0.9 to 9.1 cm/s.
The overall gas holdup was measured using the differential pressure method. Ignoring the pressure difference caused by gas density, the overall gas holdup has the following relationship with the pressure difference between the two ends of the measuring point [
29]:
where
ε, Δ
P,
ρL,
g, and
H are the gas holdup, the pressure difference between two measuring points, the liquid density, the gravitational acceleration, and the height difference between the two measurement points, respectively.
The pressure difference was measured using high-precision pressure sensors and collected online through supporting software. The data collection frequency was 13 Hz, and the collection time was 2 min.
Local liquid velocity was measured using a modified Pavlov tube [
30]. The measured pressure difference can be transformed into local liquid velocity according to the Bernoulli equation:
where
UL,
n, and
n1 represent local liquid velocity, the total number of data, and the number of positive values, respectively.
The volumetric mass transfer coefficient (
kLa) was determined using the dissolved oxygen dynamic response curve method. In order to comprehensively investigate the mass transfer situation inside the reactor, two equally dissolved oxygen electrodes were used to measure
kLa at different positions, with axial positions of 1.5 m and 3.5 m, respectively, i.e., H/D = 3.1 and H/D = 7.2. The radial positions were at the center and sidewall inside the reactor. The detailed experimental steps can be obtained from our previous research work [
31]. Since temperature also has a significant impact on
kLa, when the ambient temperature changes, correction can be performed using the following equation [
32,
33,
34]:
The mixing performance in ILARs is usually determined by mixing time. The mixing time is defined as the time required to reach a specific degree of homogeneity after a small amount of tracer is injected into the reactor. The definition of the degree of homogeneity (
η) is as follows [
35]:
where
C0,
C∞, and
Ct represent the initial concentration of the tracer, the concentration after being completely mixed, and the instantaneous concentration, respectively.
The
η parameter was 95% in this study. The mixing time was measured using the conductivity method. Considering the fact that the mixing time may change significantly with the detection position, four conductivity probes were arranged at different axial heights (H/D = 1.9, 4.5, 6.8, and 8.9) on the inner sidewall of the reactor to detect liquid conductivity.
Figure 3 shows the results after the calibration of the four conductivity electrodes. It can be seen that there is a good linear relationship between conductivity and electrolyte concentration within the range of the experimental conditions, so it can indirectly represent the concentration of the tracer. When the two-phase gas–liquid flow reached a steady state in the reactor, a KCl solution was instantly injected into the top of the reactor, and the conductivity curve of the mixing process was recorded using the conductivity meters. The typical tracer concentration variation curve is depicted in
Figure 4. Then, the mixing time was obtained using Equation (4).
4. Conclusions
In order to investigate the impact of draft tube structures on mass transfer and mixing performance in a pilot-scale ILAR, the gas holdup, liquid circulating velocity, kLa, and mixing time of three reactor structures (BCR, SSALR, and FSALR) were systematically studied in experiments. Experimental results demonstrated that the BCR had higher gas holdup and kLa values. The gas holdup and kLa decreased due to the rapid escape of bubbles caused by the introduction of the draft tube. The single-stage draft tube was axially segmented to build an FSALR, which increased the gas holdup in the reactor, particularly in the downcomer by 9%. Furthermore, compared with the SSALR, the kLa in the riser of the FSALR increased by 10.2% on average, while that in the downcomer increased by 9.3% on average. The FSALR had the fastest liquid circulating velocity due to its lower circulating resistance. The liquid circulating velocity of the FSALR was 134.1% higher than that of the BCR and 15.8% higher than that of the SSALR. The mixing effect of the FSALR was the best because of its faster liquid circulating velocity and more effective axial and radial mixing, which is close to the CSTR. Specifically, the mixing time experiment illustrated that the mixing time in the BCR was seriously affected by the measurement position, while it was the least affected in the FSALR. In the heterogenous regime, the mixing time of the FSALR was reduced by 70.2% on average compared with the BCR and 51.3% compared with the SSALR. The empirical correlations were developed for gas holdup, liquid circulating velocity, kLa, and mixing time with respect to the superficial gas velocity, which fit the experimental data well.