Impact of flow velocity on the heterogeneous reaction of SO2 over Fe2O3

Liu, Yangyang; Wang, Tao; Ge, Qingjie; Shi, Zhuocheng; Li, Kejian; Gong, Kedong; Xie, Lifang; Wang, Wei; Wang, Qianlong; Han, Jin; Fu, Hongbo; Chen, Jianmin; Zhang, Liwu

doi:10.1016/j.atmosenv.2022.119491

Cited by 3 publications

(15 citation statements)

References 94 publications

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“…One is ascertained that CO 2 concentration strongly promotes the uptake coefficients regardless of TiO 2 and authentic particles. Among ferric oxide, manganese oxide, Al 2 O 3, and SiO 2 , ferric oxide shows the largest contribution to the SO 2 uptake capability even if its lower abundance of 5% more or less (Agnihotri et al., 2015; Y. Liu et al., 2023c; Myriokefalitakis et al., 2015; Usher et al., 2003) relative to Al 2 O 3 (10%–15%) and SiO 2 (∼60%) (George et al., 2007). This may potentially correlate to the underlying photochemical activity of ferric oxide that enables the proposed scheme to occur.…”

Section: Resultsmentioning

confidence: 99%

“…In dry and low RH conditions, the SO 2 oxidation process is mainly mediated by surface active oxygen (O − ) and OH groups (Y. Chen et al., 2021; T. Wang et al., 2018c). On the contrary, an aqueous‐like medium appears on the dust surface and radical ions will significantly dominate the reactions at moderate and high RH levels (Y. Liu et al., 2022, 2023c). Therefore, we examined the role of CO 2 in SO 2 oxidation on dust surfaces at three typical RH conditions, corresponding to low case (30%), moderate case (50%), and high case (70%).…”

Section: Resultsmentioning

confidence: 99%

“…On the contrary, an aqueous-like medium appears on the dust surface and radical ions will significantly dominate the reactions at moderate and high RH levels (Y. Liu et al, , 2023c. Therefore, we examined the role of CO 2 in SO 2 oxidation on dust surfaces at three typical RH conditions, corresponding to low case (30%), moderate case (50%), and high case (70%).…”

Section: The Influence Of Rh and Light Intensity On So 2 Oxidation Ov...mentioning

confidence: 99%

“…The heterogeneous reaction pathway dominates the SO 2 oxidation process over dust surface at low RH conditions (10%) (Y. Liu et al, 2023c), while radical ions regulate the process when RH was further increased to 30%(Y. because dust surfaces are prone to possess several water layers through a thermodynamic equilibrium process (L. X. D.…”

Section: Reaction Mechanismmentioning

confidence: 99%

“…Carbonate radical ions also show distinct effects on SO 2 oxidation rates and reaction channels in dark and light control experiments in specific meteorological conditions (e.g., low RH and weak light intensity). Nevertheless, diverse RH, light intensity, and dust constituents can largely change the SO 2 uptake capability and synergetic mechanism (Y. Liu et al., 2023c; Ram et al., 2012), and rare information is now currently available into what changes would be involved in SO 2 oxidation in the presence of CO 2 on MD_ACP surfaces by adjusting these factors. This motivates us to give more comprehensive investigations of CO 2 in different meteorological conditions, in which light intensity and RH, the two most important parameters in triggering SO 2 oxidation on dust surfaces, were thus explored.…”

Section: Introductionmentioning

confidence: 99%

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Unveiling the Role of Carbonate Radical Anions in Dust‐Driven SO₂ Oxidation

Liu,

Wang,

et al. 2024

JGR Atmospheres

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Carbonate radical anion () is generally overlooked in atmospheric chemistry. Our recent work emphasizes the important role of carbonate radicals produced on mineral dust surfaces in fast sulfate production under solar irradiation in the presence of CO2 at specifically low RH and light intensity. Yet so far how involves and affects secondary sulfate production under diverse RH, light intensity, and complex constituent matrix remains unknown, which essentially limits our comprehensive knowledge of initiated SO2 oxidation scheme in the atmosphere. Herein, we explored the heterogeneous SO2 oxidation over both model and authentic dust and clays in the presence of CO2 at atmospheric relevant RHs and light intensities. Interestingly, we observe that CO2 promotes sulfate yield over authentic dust and clays at atmospheric‐relevant RH and light intensity. This observation relates to the favorable kinetic between SO2 oxidation and while auto‐quenching of these radical ions is largely minimized due to the sufficient sites of crustal constituents. Furthermore, employing a suite of authentic dust and machine learning strategies, we evaluated the relative importance of each constituent within airborne minerals or clays as well as environmental conditions including relative humidity, light intensity, and CO2 concentration in affecting SO2 uptake capability. On this basis, sulfate formation mediated by dust‐driven pathway, accounting for nearly ∼20.9% of overall contribution by the end of this century during some pollution episodes, even higher than gas‐phase (∼16.9%), will be increased by 163% if CO2‐initiated SO2 oxidation scheme is incorporated.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: The Influence Of Rh and Light Intensity On So 2 Oxidation Ov...mentioning

confidence: 99%

Section: Reaction Mechanismmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Unveiling the Role of Carbonate Radical Anions in Dust‐Driven SO₂ Oxidation

Liu,

Wang,

et al. 2024

JGR Atmospheres

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Investigating the impact of pretreatment strategies on photocatalyst for accurate CO2RR productivity quantification: A machine learning approach

Liu

Wang

et al. 2023

Chemical Engineering Journal

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Insights into the Formation Mechanism of Reactive Oxygen Species in the Interface Reaction of SO₂ on Hematite

Jia,

Ma,

Liu

et al. 2024

Environ. Sci. Technol.

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The interplay between sulfur and iron holds significant importance in their atmospheric cycle, yet a complete understanding of their coupling mechanism remains elusive. This investigation delves comprehensively into the evolution of reactive oxygen species (ROS) during the interfacial reactions involving sulfur dioxide (SO2) and iron oxides under varying relative humidity conditions. Notably, the direct activation of water by iron oxide was observed to generate a surface hydroxyl radical (•OH). In comparison, the aging of SO2 was found to markedly augment the production of •OH radicals on the surface of α-Fe2O3 under humid conditions. This augmentation was ascribed to the generation of superoxide radicals (•O2 –) stemming from the activation of O2 through the Fe(II)/Fe(III) cycle and its combination with the H+ ion to produce hydrogen peroxide (H2O2) on the acidic surface. Moreover, the identification of moderate relative humidity as a pivotal factor in sustaining the surface acidity of iron oxide during SO2 aging underscores its crucial role in the coupling of iron dissolution, ROS production, and SO2 oxidation. Consequently, the interfacial reactions between SO2 and iron oxides under humid conditions are elucidated as atmospheric processes that enhance oxidation capacity rather than deplete ROS. These revelations offer novel insights into the mechanisms underlying •OH radical generation and oxidative potential within atmospheric interfacial chemistry.

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Impact of flow velocity on the heterogeneous reaction of SO2 over Fe2O3

Cited by 3 publications

References 94 publications

Unveiling the Role of Carbonate Radical Anions in Dust‐Driven SO₂ Oxidation

Unveiling the Role of Carbonate Radical Anions in Dust‐Driven SO₂ Oxidation

Investigating the impact of pretreatment strategies on photocatalyst for accurate CO2RR productivity quantification: A machine learning approach

Insights into the Formation Mechanism of Reactive Oxygen Species in the Interface Reaction of SO₂ on Hematite

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Impact of flow velocity on the heterogeneous reaction of SO2 over Fe2O3

Cited by 3 publications

References 94 publications

Unveiling the Role of Carbonate Radical Anions in Dust‐Driven SO2 Oxidation

Unveiling the Role of Carbonate Radical Anions in Dust‐Driven SO2 Oxidation

Investigating the impact of pretreatment strategies on photocatalyst for accurate CO2RR productivity quantification: A machine learning approach

Insights into the Formation Mechanism of Reactive Oxygen Species in the Interface Reaction of SO2 on Hematite

Contact Info

Product

Resources

About

Unveiling the Role of Carbonate Radical Anions in Dust‐Driven SO₂ Oxidation

Unveiling the Role of Carbonate Radical Anions in Dust‐Driven SO₂ Oxidation

Insights into the Formation Mechanism of Reactive Oxygen Species in the Interface Reaction of SO₂ on Hematite