3.1. Agglomeration and Removal Characteristics of SO3
When the flue gas contains only SO3, the cooling process in the heat exchanger induces homogeneous nucleation, leading to the formation of a large number of ultrafine sulfuric acid droplets. As these droplets pass through the turbulent agglomerators, collisions and agglomeration occur, altering their concentration and size distribution, which in turn affects their removal efficiency. Therefore, this section focuses on investigating the agglomeration and removal characteristics of SO3 in the absence of fine fly ash particles.
When the aerosol generator was turned off and the SO
3 generation system was operating normally, ELPI+ was used to measure the change in the number concentration of sulfuric acid droplets formed by SO
3 condensation before and after turbulent agglomeration. The results are shown in
Figure 4. It can be observed that after passing through the heat exchanger, the gaseous SO
3 in the flue gas condensed into a large number of sulfuric acid droplets, with a number concentration of 1.59 × 10
7 1/cm
3. After passing through the turbulent agglomerator, the number concentration decreased to 1.25 × 10
7 1/cm
3, a reduction of approximately 21.4%. This result indicates that sulfuric acid droplets underwent collisions and agglomeration in the turbulent flow field, where multiple droplets adhered to each other to form larger droplets, thereby reducing their number concentration.
Figure 5 shows the change in the size distribution of sulfuric acid droplets before and after turbulent agglomeration. The results indicate that before turbulent agglomeration, most of the sulfuric acid droplets formed by condensation were smaller than 0.1 µm, accounting for 99.2% of the total droplet count. After passing through the turbulent agglomerator, due to collisions and agglomeration, multiple droplets combined to form larger ones, resulting in a significant reduction in the number concentration of droplets below 0.1 µm. The proportion of droplets within this size range decreased to 89.4%, while the number of droplets larger than 0.1 µm increased accordingly.
These findings suggest that turbulent agglomeration also has a certain agglomeration effect on sulfuric acid droplets formed by SO
3 condensation, leading to a reduction in the number concentration and an increase in the droplet size. According to previous studies [
17,
19], smaller particles tend to enter the recirculation zone behind the vortex generators in the turbulent agglomerator, where they undergo agglomeration. In the case of SO
3 alone, most of the sulfuric acid droplets formed by homogeneous nucleation are smaller than 0.1 µm, making them highly responsive to the flue gas flow. Consequently, they can enter the recirculation zone of the turbulent agglomerator, experience agglomeration, and grow into larger droplets, thereby reducing their number concentration.
Figure 6 presents the concentration of SO
3 before and after LLT-ESP and its removal efficiency with and without turbulent agglomeration. When the experimental system was operated without turbulent agglomeration, the SO
3 concentration in the flue gas before the heat exchanger was 82.5 mg/m
3, while the concentration after the ESP was 73.2 mg/m
3, resulting in a removal efficiency of 11.3%. When a turbulent agglomerator was incorporated into the system, the SO
3 concentration before the heat exchanger was 81.6 mg/m
3, while the concentration after the ESP decreased to 68.4 mg/m
3, improving the removal efficiency to 16.2%. These results indicate that in the presence of SO
3 alone, the removal efficiency of SO
3 by LLT-ESP is relatively low. This is because the sulfuric acid droplets formed by homogeneous nucleation of SO
3 are extremely small, making them difficult to acquire sufficient charge within the electric field. As a result, their electrostatic migration rate is low, leading to poor capture efficiency.
When a turbulent agglomerator is introduced into the system, two key effects improve SO3 removal. The first reason is that multiple sulfuric acid droplets collide and merge into larger droplets, reducing the overall droplet number concentration. Another reason is that as droplet size increases, their ability to acquire charge in the electric field improves, leading to a higher charge level and increased migration rate. Consequently, the turbulent agglomeration process enhances the capture efficiency of sulfuric acid droplets in the ESP, thereby promoting the removal of SO3 even when present alone in the flue gas. To further improve the removal efficiency, one can consider regulating the flue gas by adding some vapor inside the flue gas, which can significantly enhance the tendency of the growth of sulfuric acid droplets by homogeneous condensation and thereby improve the overall removal efficiency.
3.2. Agglomeration and Removal Characteristics of Fly Ash Particles
The agglomeration and removal characteristics of fine PM were also tested in the presence of fly ash alone in the flue gas. This serves as a baseline for comparison with the agglomeration and removal characteristics when SO3 and fly ash coexist.
When the SO
3 generation system was turned off and the aerosol generator was operating normally, ELPI
+ was used to measure the change in the fine particulate number concentration before and after turbulent agglomeration, as shown in
Figure 7. The results indicate that before turbulent agglomeration, the number concentration of fine particulates in the flue gas was 5.79 × 10
6 1/cm
3, which decreased to 4.66 × 10
6 1/cm
3 after turbulent agglomeration, achieving an agglomeration efficiency of 19.5% (
Figure 8), illustrates the change in particle size distribution before and after turbulent agglomeration. Before turbulent agglomeration, the particle size distribution exhibited a bimodal pattern, with peak particle sizes at 0.04 µm and 1.25 µm. The number concentrations at these peak sizes were 2.20 × 10
6 1/cm
3 and 2.19 × 10
5 1/cm
3, respectively. After turbulent agglomeration, the particle size distribution remained bimodal, and the peak particle sizes did not change. However, an analysis of the distribution changes reveals that the number concentration of fine particles below 0.13 µm decreased to varying degrees, while that in the range of 0.13–1.25 µm slightly increased. This suggests that turbulent agglomeration facilitated the collision and adhesion of smaller fine particles, leading to the formation of larger particles. Consequently, the number concentration of smaller fine particles decreased, while that of larger particles increased.
The PM
1.0/2.5/10 samplers were used to measure the mass concentration of fine particulates before and after the low-low temperature electrostatic precipitator (ESP) under conditions with and without turbulent agglomeration. The removal efficiency was then calculated, and the results are shown in
Figure 9. Without the turbulent agglomeration, the mass concentration of fine particulates in the flue gas before the heat exchanger was 245 mg/m
3, and it decreased to 33.6 mg/m
3 after passing through the ESP, achieving a removal efficiency of 86.3%. When a turbulent agglomerator was installed after the heat exchanger, the mass concentration of fine particulates before the heat exchanger remained at 245 mg/m
3, but after the ESP, it further decreased to 19.4 mg/m
3, with the removal efficiency increasing to 92.1%. These experimental results indicate that the turbulent agglomerator enhances fine particulate removal efficiency by promoting the agglomeration and growth of particulates in the flue gas.
3.3. Synergistic Agglomeration and Removal of SO3 and Fine Fly Ash Particles
When both SO3 and coal combustion fly ash coexist in the flue gas, SO3 undergoes heterogeneous condensation on fine fly ash particles as condensation nuclei, along with homogeneous condensation during the cooling process in the heat exchanger. Subsequently, sulfuric acid droplets formed via homogeneous condensation interact with fine particulates through collisions and adhesion under the influence of turbulent vortices, thereby enhancing the combined removal efficiency of SO3 and fine fly ash particulates by the ESP. Therefore, this section experimentally investigates the coagulation and removal characteristics of SO3 and fine fly ash particulates in coexistence.
When both the aerosol generator and SO
3 generation system were operating normally, ELPI+ was used to measure the overall particle size distribution in the flue gas before and after turbulent agglomeration. Additionally, a comparison curve was plotted, representing the sum of the size distributions after turbulent agglomeration for cases with only SO
3 and only fly ash. The results are shown in
Figure 10. The measurements indicate that before turbulent agglomeration, the flue gas after cooling in the heat exchanger contained both fine fly ash particles and sulfuric acid droplets. The overall particle size distribution exhibited a bimodal pattern, with peak particle sizes at 0.02 µm and 1.25 µm, and corresponding number concentrations of 5.85 × 10
6 1/cm
3 and 8.25 × 10
5 1/cm
3, respectively. After passing through the turbulent aggregator, the size distribution shifted to a unimodal form, with a peak at 0.02 µm and a number concentration of 3.79 × 10
6 1/cm
3 at the peak. Furthermore, the particle number concentration decreased across all size ranges, with the most significant reduction occurring in the sub-micro range. In this range, the number concentration dropped from 1.67 × 10
7 1/cm
3 before agglomeration to 9.77 × 10⁶ 1/cm
3 after agglomeration, representing a 41.5% decrease. Given that most sulfuric acid droplets formed via homogeneous condensation of SO
3 fall below 0.1 µm and are present in large quantities, it can be inferred that the droplets and fine particles underwent collision and adhesion in the turbulent field, leading to a substantial reduction in the particle concentration within this size range. Moreover, when comparing the sum of the particle size distributions after turbulent agglomeration for the individual SO
3 and fly ash cases with the distribution obtained in their coexistence, it is evident that particle concentrations at all size ranges were significantly lower in the coexistence case. This suggests that not only did fine fly ash particles and sulfuric acid droplets aggregate among themselves respectively, but also that inter-particle agglomeration occurred between the fly ash and sulfuric acid droplets. Consequently, the overall agglomeration effect in the coexistence scenario was superior to the sum of the effects observed in the individual cases.
Additionally, PM
1.0/2.5/10 samplers were used to collect fine particulate samples before and after turbulent agglomeration. The SO
3 mass concentration in fine particles across four particle size ranges was measured, and the results are shown in
Figure 11. It can be observed that after turbulent agglomeration, the SO
3 mass concentration within fine particles increased across all size ranges, with the most significant rise occurring in particles smaller than 1.0 µm. In this range, the SO
3 mass concentration increased from 154.2 μg/mg before agglomeration to 392.4 μg/mg after agglomeration. These results indicate that turbulent agglomeration enhances the adhesion and deposition of sulfuric acid droplets onto fine fly ash particles [
22], with this effect being more pronounced for smaller particles. Particles with lower mass and inertia in a turbulent flow field can follow the gas stream into the recirculation zone behind the turbulence-generating elements, where agglomeration occurs. In the case of fly ash, fine particles smaller than 1.0 µm exhibit better gas-following behavior due to their lower mass, allowing them to accumulate in the recirculation zone. Since most sulfuric acid droplets are smaller than 0.1 µm, they can also fully follow the gas flow into the recirculation zone. Consequently, many submicron fly ash particles collide and aggregate with sulfuric acid droplets within this zone, leading to significant adhesion and a marked increase in the SO
3 mass concentration in particles smaller than 1.0 µm. In contrast, larger fly ash particles tend to maintain their original velocity and movement within the mainstream flow, reducing their probability of collision with sulfuric acid droplets. As a result, the enhancement effect of the turbulent aggregator on sulfuric acid droplet deposition weakens with increasing particle size.
To further investigate the agglomeration characteristics when SO
3 and fine fly ash particles coexist, SEM and EDS analyses were conducted on the morphology and elemental changes of fine particles before and after turbulent agglomeration. The results are shown in
Figure 12. It can be observed that before the turbulent aggregator, only a small amount of agglomeration contact occurred between fine particles, with most particles unconnected (
Figure 12a). However, after passing through the turbulent aggregator, multiple fine particles of different sizes were found to combine, forming larger agglomerates (
Figure 12b). The main mechanism behind the synergistic effect was the heterogeneous condensation of SO
3 on the fly ash particles. Compared with the single pollutant scenario, the condensational growth of SO
3 was greatly enhanced, since the energy barrier of heterogeneous condensation was lower than that of homogeneous nucleation. Moreover, the SO
3 on the fly ash particles could induce surface chemistry modification, which increased the cohesiveness of PM and thus increased the turbulent agglomeration efficiency.
Furthermore, EDS analysis (
Figure 12c) revealed that the surface sulfur content of the agglomerates was significantly higher than that of the fine particles before agglomeration. This indicates that during the turbulent agglomeration process, sulfuric acid droplets collided and aggregated with fine particles, leading to the deposition of sulfuric acid droplets onto the surface of the fine particles. This increased the surface interaction forces of the particles, promoting the adhesion of multiple fine particles to form larger agglomerates. Therefore, the deposition of SO
3 on the surface of fine particles also enhanced the turbulent agglomeration effect.
To investigate the removal characteristics of SO
3 and fine PM, concentrations were measured using an SO
3 sampling system and PM
1.0/2.5/10 samplers before and after the LLT-ESP. As illustrated in
Figure 13, the SO
3 concentration measured 83 mg/m
3 upstream of the heat exchanger. Without turbulent agglomeration, the LLT-ESP outlet concentration decreased to 25.1 mg/m
3 (69.7% removal efficiency). With turbulent agglomeration, this further reduced to 14.2 mg/m
3 (82.9% removal efficiency). For PM
2.5, the initial concentration of 245 mg/m
3 decreased to 24.3 mg/m
3 (90.1% removal efficiency) without turbulent agglomeration and 5.9 mg/m
3 (97.6% removal efficiency) with turbulent agglomeration.
These findings indicate that turbulent agglomeration synergistically enhances LLT-ESP’s removal performance for both SO3 and fine PM. The coexistence of SO3 and fly ash yielded higher removal efficiencies than individual components. Mechanistic analysis reveals two pathways: (1) Sulfuric acid droplets coalesce onto particulates through turbulent collision, enabling their co-removal; (2) Sulfate deposition increases particle surface adhesion and reduces electrical resistivity, thereby improving charge acquisition and capture efficiency in the ESP field. The implementation of turbulent agglomeration technology in the LLT-ESP system demonstrates dual optimization for multi-pollutant control in the flue gas treatment process.