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Ce-based three-dimensional (3D) mesoporous microspheres with Mn homogeneous incorporation were synthesized. The CeMn-0.4, characterized by a Ce/Mn molar ratio of 6:4, demonstrated exceptional catalytic activity and stability. The formation of CeMn solid solution strengthened the Ce-Mn interaction, yielding higher concentrations of Ce 3+ and Mn 4+ . Mn 4+ initiated toluene preliminary activation owing to its robust oxidative properties, while Ce 3+ contributed to oxygen vacancy generation, enhancing the activation of gaseous oxygen and lattice oxygen mobility. Integrating experiments and Density Functional Theory (DFT) calculations elucidated the oxygen reaction mechanisms. A portion of oxygen was converted into surface reactive oxygen species (O ads ) that directly oxidized toluene. Additionally, the presence of oxygen vacancies promoted the participation of oxygen in toluene oxidation by converting it into lattice oxygen, which was crucial for the deep oxidation of toluene. Diffuse Reflectance Fourier Transform Infrared Spectroscopy (DRIFTS) indicated the accumulation of benzene-ring intermediates on the catalyst surface hindered continuous toluene oxidation. Thus, the abundant oxygen vacancies in CeMn-0.4 played a pivotal role in sustaining the oxidation process by bolstering the activation of gaseous oxygen and the mobility of lattice oxygen., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Inc. All rights reserved.)

Advancement of the absorbent for CO 2 capture is essential in optimizing the performance and reducing the negative environmental effects associated with this technology. Despite ammonia's promise as an absorbent, the volatility limits its practical application and creates potential environmental pollution. Therein, we assess various additives (amino acids, carbonates, and alkanolamines) for ammonia-based solvents using multi-stage circulation absorber from the viewpoints of aerosol emission, ammonia emission, and CO 2 capture efficiency. Experimental findings reveal that ammonia volatilization can be inhibited by the protonation of free ammonia by carboxyl groups and the formation of hydrogen bonding between amino/hydroxyl groups and ammonia, with ammonia emission reduced by 21.7 %, aerosol emission reduced by 26.5 %, and CO 2 capture efficiency increased to a maximum of 87.8 % under the condition of adding histidine. Moreover, the experiment highlights a positive correlation between total ammonia emission and aerosol concentration/diameter. Additionally, tests combining source abatement with water wash exhibit up to 50.5 % aerosol removal efficiency and up to 76.6 % ammonia removal efficiency. To further mitigate emissions, a comprehensive approach is proposed, achieving an 84.4 % reduction in ammonia emission and a 61.9 % reduction in aerosol emission. Finally, a method for recycling ammonia for desulfurization is suggested., Competing Interests: Declaration of competing interest We declare that we do not have any commercial or associative interest that represents a conflict of interest in connection with the work submitted., (Copyright © 2024. Published by Elsevier B.V.)

A redox co-precipitation method was employed to synthesize CeMn homogeneous solid solutions, utilizing various alcohols as activating agents. Ethanol effectively orchestrated the precipitation of CeO 2 and MnO x , promoting their co-growth. As a result, the CeMn-EA achieved 90 % toluene conversion at 218 ℃ (T 90 =218 ℃) with a weight hourly space velocity (WHSV) of 48000 ml/(g·h). It also demonstrated high adaptability to increased WHSV, suggesting its potential for industrial-scale applications. The uniform dispersion of Ce and Mn accelerated the coupling between Ce 3+ /Ce 4+ and Mn 4+ /Mn 3+ , engineering numerous oxygen vacancies, which enhanced the activation of gas-phase oxygen and the mobility of lattice oxygen. In situ DRIFTS confirmed that toluene oxidation accommodated both Langmuir-Hinshelwood (L-H) and Mars-van Krevelen (MvK) mechanisms, with benzoate identified as a pivotal intermediate. Enhanced oxygen mobility facilitated the cleavage of the benzene ring, which was the rate-determining step. Additionally, the introduction of H 2 O significantly enhanced the dissociation and adsorption of toluene and facilitated the activation of gas-phase oxygen. At higher temperatures, H 2 O could further activate lattice oxygen engaging in toluene oxidation. ENVIRONMENTAL IMPLICATION: Volatile organic compounds (VOCs) have emerged as major air pollutants due to the changes in air pollution patterns. They can act as precursors to near-surface ozone and haze. Toluene, a typical VOC, is primarily released from anthropogenic sources and poses significant risks to human health and the environment. Ce-based catalysts have been demonstrated efficiency in toluene oxidation due to their excellent oxygen storage and release properties. This study synthesized CeMn homogeneous solid solutions utilizing various alcohols as activating agents, which possessed abundant oxygen vacancies and optimum oxygen activation capacity to oxidize toluene in time., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

The mercury oxidation performance of Ce/TiO 2 catalyst can be further enhanced by transition metal modifications. This study employed density functional theory (DFT) calculations to investigate the adsorption and oxidation mechanisms of Hg 0 on Ce/TiO 2 (001) and its transition metal modified surfaces. According to the calculation results, Ru-, Mo-, Nb-, and Mn-doping increased the affinity of the Ce/TiO 2 (001) surface towards Hg 0 and HCl, thereby facilitating the efficient capture and oxidation of Hg 0 . The increased adsorption energy (E ads ) of the intermediate HgCl on the modified surfaces could promote its conversion to the final product HgCl 2 . The modification of transition metals impeded the desorption of the final products HgCl 2 and HgO, but it did not serve as the rate-determining step. The oxidation of Hg 0 by lattice oxygen and HCl followed the Mars-Maessen and Langmuir-Hinshelwood mechanisms, respectively. HCl exhibited higher mercury oxidation ability than lattice oxygen. The reactivity of lattice oxygen could be further improved by doping transition metals, their promotion order was Ru > Nb > Mo > Mn. In a HCl atmosphere, Mn modification could significantly reduce the energy barrier for HCl activation and HgCl 2 formation, providing the optimal enhancement for the mercury oxidation ability of Ce/TiO 2 catalyst. The screening method of transition metal modified components based on surface adsorption reaction and oxidation energy barrier was proposed in this study, which provided theoretical guidance for the development of CeTi based catalysts with high mercury oxidation activity., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)

Aerosols produced in the amine carbon capture process can lead to secondary environmental pollution. This study employs molecular dynamics (MD) simulations to investigate cluster formation, amine behavior, and aerosol growth of amines, essential for reducing amine aerosol emissions. Results showed that the cluster evolution process can be divided into cluster formation and growth in terms of molecular content, and the nucleation rate for the present systems was estimated in the order of 10 28 cm -3 s -1 . CO 2 absorption was observed alongside successful nucleation, with CO 2 predominantly localizing in the cluster's outer layer postabsorption. Monoethanolamine (MEA) exhibited robust electrostatic interactions with other components via hydrogen bonding, leading to its migration toward regions where CO 2 and H 2 O coexisted within the cluster. While MEA presence markedly spurred cluster formation, its concentration had a marginal effect on the final cluster size. Elevating water content can augment the aerosol growth rate. However, altering the gas saturation is possible only within narrow confines by introducing vapor. Contrarily, gas cooling introduced dual, opposing effects on aerosol growth. These findings, including diffusion coefficients and growth rates, enhance theoretical frameworks for predicting aerosol formation in absorbers, aiding in mitigating environmental impacts of amine-based carbon capture.

Aerosol emissions from the CO 2 capture process have a significant impact in terms of solvent loss and environmental pollution. Here, we propose a novel approach with multi-stage circulation for CO 2 capture and synergistic aerosol reduction, which divides the absorption section into three circulation stages and reduces aerosol emissions through decoupled operation of the three absorption sections and the management of solvent CO 2 loadings. Experimental results show that with the decoupled management of the liquid-gas ratio and solvent temperature in absorption sections, the aerosol mass concentration at the outlet of the 3rd absorption section can be reduced by 25.6% to a minimum of 349.7 mg/m 3 at a liquid-gas ratio of 43.2 L/m 3 and a solvent temperature of 303 K. Furthermore, aerosol removal is performed by setting up a water wash section after the absorption section. The aerosol mass concentration at the outlet of the absorber is reduced to 168.6 mg/m 3 with the regulation of the wash water temperature and flow rate. In addition, improvements are proposed for the combination of the utilization of recovered solvents and the co-removal of SO 2 . This study provides innovative insights into the design of the CO 2 capture system and the reduction of aerosol emissions, which are of great significance for the mitigation of global warming and the control of environmental pollution.

Aerosol emission from the CO 2 capture system has raised great concern for causing solvent loss and serious environmental issues. Here, we propose a comprehensive method for reducing aerosol emissions in a CO 2 capture system under the synergy of aerosol formation inhibition and wet electrostatic precipitation. The gas-solvent temperature difference plays a vital role in aerosol formation, with aerosol emissions of 740.80 mg/m 3 at 50 K and 119.36 mg/m 3 at 0 K. Different effects of SO 2 and SO 3 on aerosol formation are also found in this research; the aerosol mass concentration could reach 2341.25 mg/m 3 at 20 ppm SO 3 and 681.01 mg/m 3 at 50 ppm SO 2 with different aerosol size distributions. After the CO 2 capture process, an aerosol removal efficiency of 98% can be realized by electrostatic precipitation under different CO 2 concentrations. Due to the high concentration of aerosols and aerosol space charge generated by SO 2 and SO 3 , the removal performance of the wet electrostatic precipitator decreases, resulting in a high aerosol emission concentration (up to 130.26 mg/m 3 ). Thus, a heat exchanger is installed before the electrostatic precipitation section to enhance aerosol growth and increase aerosol removal efficiency. Under the synergy of aerosol formation inhibition and electrostatic precipitation, an aerosol removal efficiency of 99% and emission concentrations lower than 5 mg/m 3 are achieved, contributing to global warming mitigation and environmental protection.

Pollutant removal and resource recovery from high-humidity flue gas after desulfurization in a thermal power plant are crucial for improving air quality and saving energy. This study developed a flue gas treatment method involving phase transition enhanced by corona discharge based on laboratory research and established a field-scale unit for demonstration. The results indicate that an adequate increase in size will improve the ease of particle capture. A wet electrostatic precipitator is applied before the condensing heat exchangers to enhance the particle growth and capture processes. This results in an increase of 58% in the particle median diameter in the heat exchanger and an emission concentration below 1 mg/m 3 . Other pollutants, such as SO 3 and Hg, can also be removed with emission concentrations of 0.13 mg/m 3 and 1.10 μg/m 3 , respectively. Under the condensation enhancement of the method, it is possible to recover up to 3.26 t/h of water from 200 000 m 3 /h saturated flue gas (323 K), and the quality of the recovered water meets the standards stipulated in China. Additionally, charge-induced condensation is shown to improve heat recovery, resulting in the recovery of more than 43.34 kJ/h·m 3 of heat from the flue gas. This method is expected to save 2628 t of standard coal and reduce carbon dioxide emission by 2% annually, contributing to environmental protection and global-warming mitigation.

CeO 2 /TiO 2 catalyst is a promising material for realizing the integration of denitrification and mercury removal to reduce mercury emissions. Oxidation mechanism of Hg 0 on CeO 2 /TiO 2 (001) surface in the presence of HCl and O 2 was studied by density functional theory (DFT). The results indicated that Hg 0 was physically adsorbed on CeO 2 /TiO 2 (001) surface. As an important intermediate, HgCl was adsorbed on the surface of CeO 2 /TiO 2 (001) utilizing enhanced chemisorption, while the adsorption energy of HgCl 2 was only -57.05 kJ/mol. In the absence of HCl, mercury oxidation followed the Mars-Maessen mechanism with a relatively high energy barrier, and the product (HgO) was difficult to desorb, which hindered the reaction process. When HCl existed, reactive chlorine (Cl*) would be produced by the dissociation of HCl, and the mercury oxidation would follow the Langmuir-Hinshelwood mechanism. The co-existence of HCl and O 2 had no significant effect on the adsorption of Hg 0 , but reduced the reaction energy barrier and the final product (HgCl 2 ) was more easily desorbed from the catalyst surface. In addition, two complete cyclic reaction pathways for catalytic oxidation of Hg 0 on CeO 2 /TiO 2 (001) surface were constructed to clarify the detailed reaction process., (Copyright © 2022 Elsevier B.V. All rights reserved.)

In the steam-assisted-gravity-drainage (SAGD) process, heat energy is transferred from the steam chamber to the farther cold reservoir by conduction and convection mechanisms, so as to reduce the oil viscosity. In previous research works, although it was proved that convection is an indispensable part of the heat-transfer process, there is still a controversy about the formation mechanism of heat convection. In this study, an analytical mathematic model was proposed to explore the convective heat transfer in SAGD operation. Typically, this model integrates three heat convection forms that are generated by pressure difference, gravity, and thermal expansion of connate water,. Subsequently, the simulation results are compared with field data to evaluate the accuracy of the new model, and they are reasonably consistent with UTF field data. The results indicate that convective heat transfer plays a predominant role in the immediate vicinity of the steam chamber interface. Furthermore, this paper derives a mathematic model of oil production to explore the effect of heat convection on oil production under different operation conditions. The results demonstrate that heat convection has an adverse impact on oil production, but it is inevitable. This study also displays that some parameters, such as the lateral spreading rate, the thermal diffusivity, the viscosity coefficient, and the curvature of oil relative permeability curve, can significantly affect the oil production rate. Based on this study, the effect of convection mechanism on the heat-transfer process and oil production will be further clarified, and the parameters in the SAGD process can be optimized, so as to effectively enhance and predict oil production., Competing Interests: The authors declare no competing financial interest., (© 2020 American Chemical Society.)

Condensation fine particles (CFPs) from coal-fired flue gas harm humans and the environment after being emitted into the atmosphere. Given their small size (<0.1 μm), difficulty arises in efficiently removing CFPs by wet electrostatic precipitators and mist eliminators. In this work, a laboratory apparatus was used to study the CFP growth under simulated power plant conditions. Four methods were independently investigated to increase the particle size: addition of ammonia, addition of fly ash, decreasing temperature, and applying an electrical discharge. Results demonstrated that the CFP size distribution possessed a unimodal structure with peak at 0.05 μm. At increased ammonia concentration from 10 to 30 ppm, the peak of growth factor shifted rightward and increased from 1.21 to 1.35 and the range of growth factor >1 was significantly broadened due to joint action of multiple mechanisms. Fly ash acted as the core, and CFPs adhered to the ash surface when forming ash-salt droplets. Cooling flue gas could also enhance the CFP growth due to vapor condensation. At decreased temperature from 45 to 30 °C, the median diameter of CFPs increased by 15%. Finally, the growth and agglomeration of CFPs can be further enhanced when an external electrical field was utilized. The size range of growth factor >1 can be broadened, and the peak growth factor significantly increased at 8 kV applied voltage. The research findings provide valuable guidance for effectively improving the CFP removal efficiency by external regulation for growth enhancement.

Sulfuric acid aerosol (SAA) can considerably deteriorate air visibility, which poses a threat to human health. Pretreatment methods that enlarge SAA sizes are crucial to enhanced emission control from industrials. This study provides an insight into SAA growth in terms of aerosol dynamics simulation and growth experiments under simulated flue gas conditions. Results show that SAA growth dynamics are dominated by coagulation and condensation mechanisms for small and large aerosols, respectively. The two mechanisms are coupled mainly in SAA sizes smaller than 0.05 μm. A large amount of time was allotted for the SAA distribution to grow into an approximately log-normal form without the use of any activation methods. Cooling gas and corona discharge can both enhance SAA growth. Cooling gas is in charge of condensation, whereas corona discharge mainly acts on coagulation. They exhibited 14.3% and 12.3% increases in mean diameter and 12.3% and 69.1% decreases in number concentration. In contrast, adding vapor led to a 1.58% decrease in mean diameter and a 9.4% increase in number concentration. Findings suggest that combining cooling gas and corona discharge to simultaneously promote coagulation and condensation and reduce SAA emission from humid flue gas is possible.

Under the extensive implementation of ultra-low emission (ULE) facilities in coal-fired power plants of China, sulfur trioxide (SO 3 ) has received increasing attention due to its impact on human health and operation safety of power plants. However, systematic research and evaluation for controlling SO 3 emission in various ULE facilities are still lacking. Here, a systematic study was conducted based on 378 in situ performance evaluation tests carried out in 148 coal-fired power plants. The results illustrate that the SO 2 /SO 3 conversion rate of the selective catalytic reduction devices can be controlled within 1% before and after ULE retrofit. Also, the synergistic removal efficiency of SO 3 in the low-low-temperature electrostatic precipitator and the wet electrostatic precipitator can be higher than 70%. The removal efficiency of SO 3 in the wet limestone-gypsum flue gas desulfurization scrubber is 33-64% before ULE and 31-81% after, and the average efficiency of the double scrubbers is 8.7% higher than that of the single scrubber. Due to the different SO 3 removing abilities of various technologies, the overall efficiency of SO 3 removal is in the range between 27 and 95% adopting different ULE technical routes. Average concentration of SO 3 emission can be decreased by 51.8% after ULE application.

During the thermal enhanced oil recovery (EOR) process, the hazardous hydrogen sulfide (H 2 S) gas among the produced gases causes significant difficulty in the exploration and development of petroleum. In this study, the effects of superheat degree on the H 2 S generation by heavy oil aquathermolysis were explored through simulated experiments. The crude and residual oils before and after the reaction were separated into saturate, aromatic, resin and asphaltene fractions (SARA). The oil samples were analyzed from various perspectives by various characterization methods including Fourier transform infrared (FTIR) spectroscopy, elemental analysis, and X-ray photoelectron spectroscopy (XPS). The results showed that H 2 S generation was favored by larger superheat degree at the same temperature, and it increased from 0.178 to 0.345 mL g -1 oil with an increase in the superheat degree from 62.19 to 89.42 °C. The contents of the sulfur-containing substances, which were supposed to be the main sources of H 2 S generation, in the saturate and aromatic fractions decreased significantly with an increase in the superheat degree; the increase in the superheat degree led to a slight reduction in the contents of the methylene, methyl and carboxyl/carbonyl groups. Moreover, the analysis of the main sulfur existing forms before and after the reaction suggests that sulfur in the forms of sulfides, sulfones and sulfates is more likely to generate H 2 S under superheated steam conditions. This study provides an understanding of the mechanism of H 2 S generation during the process of injecting superheated steam for heavy oil recovery., Competing Interests: There are no conflicts of interest to declare., (This journal is © The Royal Society of Chemistry.)

Wastewater from a limestone-gypsum wet desulfurization system cannot be directly reused or discharged due to its high suspended matter content and complex water composition. Desulfurization wastewater evaporation in flue gas is an effective way to dispose wastewater. Multicomponent soluble chlorine salts exist in the desulfurization wastewater. During the evaporation, chlorine enters into the flue gas due to volatilization, which accelerates the enrichment rate of the Cl - concentration in the desulfurization slurry and leads to an increase in wastewater production. This study explored the chlorine migration of various chlorine salt solutions and typical desulfurization wastewater at high temperature during the evaporation process of concentrated wastewater by a laboratory-scale tube furnace and a pilot-scale system. Results showed that when NaCl-evaporated substance was heated, the chlorine ion hardly volatilized. For the evaporated substances of CaCl 2 and MgCl 2 solutions, some of the crystal water was lost, and hydrolysis occurred to generate gaseous HCl. NH 4 Cl was easily sublimed, and the decomposition temperature was lowest. A pilot study on spray evaporation of desulfurization wastewater in flue gas showed that the particle size of the evaporated product increased and the main particle size was within 2.5-10 μm with increasing flue gas temperature. Increasing the mass ratio of gas to liquid significantly reduced the particle size of the atomized particles, thereby reducing the average particle size of the evaporated particles. The HCl concentration increased with increasing flue gas temperature. When the flue gas temperature was 350 °C, the concentration of HCl was 40 ppm, and the escape rate of chlorine in the desulfurization wastewater was approximately 30% using typical wastewater from a limestone-gypsum wet desulfurization system.

Wet electrostatic precipitators (ESPs) demonstrate a robust adaptability for particulate matter control and have been confirmed to be a promising technology for removing particles and sulfuric acid aerosol from flue gas. Recent studies have shown that removing fine particles or sulfuric acid aerosol from wet ESPs requires further development. Among the components of wet ESPs, discharge electrode configurations are crucial for determining the performance of wet ESPs. This paper reports the corona discharge characteristics and removal performance of sulfuric acid aerosol using different discharge electrode configurations in a honeycomb wet ESP experimental system. Two key parameters, namely, V - I characteristics and current density distribution, with different discharge electrode geometries ( e.g. , electrode type, spike spacing, and spike length) and rotation angles, were investigated by using a novel electrical parameter measurement system to evaluate the effects of these parameters on corona discharge. The results showed that triple-spike and sawtooth electrodes exhibit the highest average current density. The average current density of the triple-spike electrode increased with the spike length from 10 mm to 20 mm, and the peak current density distribution on the collection electrode increased by 62.1%, but the current density decreased sharply away from the spike. Moreover, the average peak current density decreased by 30.1% when the spike spacing was 25 mm given the sharp point discharge suppression when spikes were significantly dense. The electrode configuration was optimized on the basis of the current density distribution. The highest removal efficiency of sulfuric acid aerosol was 99.2% at a specific collection area of 23.09 m 2 (m 3 s -1 ) -1 ., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Electrostatic precipitation is considered as an effective technology for fine particle removal. A lab-scale wet electrostatic precipitator (ESP) with wire-to-plate configuration was developed to study particle migration and collection. The performance of the wet ESP was evaluated in terms of the corona discharge characteristics, total removal efficiency and fractional removal efficiency. The corona discharge characteristics and particle removal abilities of the wet ESP were investigated and compared with dry ESP. Particle removal efficiency was influenced by discharge electrode type, SO 2 concentration, specific collection area (SCA) and particle/droplet interaction. Results showed that the particle removal efficiency of wet ESP was elevated to 97.86% from 93.75% of dry ESP. Three types of discharge electrodes were investigated. Higher particle removal efficiency and larger migration velocity could be obtained with fishbone electrode. Particle removal efficiency decreased by 2.87% when SO 2 concentration increased from 0 ppm to 43 ppm as a result of the suppression of corona discharge and particle charging. The removal efficiency increased with higher SCA, but it changed by only 0.71% with the SCA increasing from 25.0 m 2 /(m 3 /s) to 32.5 m 2 /(m 3 /s). Meanwhile, the increasing of particle and droplet concentration was favorable to the particle aggregation and improved particle removal efficiency., Implications: This work tends to study the particle migration and collection under spraying condition. The performance of a wet electrostatic precipitator (ESP) is evaluated in terms of the corona discharge characteristics, total particle removal efficiency, and fractional particle removal efficiency. The effects of water droplets on particle removal, especially on removal of particles with different sizes, is investigated. The optimization work was done to determine appropriate water consumption, discharge electrode type, and specific collection area, which can provide a basis for wet ESP design and application.