Kedong Gong

University of California, San Diego

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Liwu Zhang

Fudan University

Kejian Li

Chongqing University of Science and Technology

Yangyang Liu

Fudan University

Qiuyue Ge

Fudan University

Tao Wang

Hong Kong Polytechnic University

Aziz-Ur-Rahim Bacha

Harbin Institute of Technology

C. George

Université Claude Bernard Lyon 1

Iqra Nabi

Fudan University

Xiuhui Zhang

Beijing Institute of Technology

Xiaozhong Fang

Fudan University

Cooperative Institutions

Fudan University

Shanghai Institute of Pollution Control and Ecological Security

Chinese Academy of Sciences

Shandong University

State Key Laboratory of Pollution Control and Resource Reuse

Tsinghua University

State Council of the People's Republic of China

Harbin Institute of Technology

Beijing Institute of Technology

Centre National de la Recherche Scientifique

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A Novel Pathway of Atmospheric Sulfate Formation Through Carbonate Radical

Yangyang Liu Yue Deng Jiarong Liu Xiaozhong Fang Tao Wang

Abstract. Carbon dioxide is considered an inert gas that rarely participates in atmospheric chemical reactions. However, we show here that CO2 is involved in some important photo-oxidation reactions in the atmosphere through the formation of carbonate radicals (CO3∙-). This potentially active intermediate CO3∙- is routinely overlooked in atmospheric chemistry regarding its effect on sulfate formation. Present work demonstrates that SO2 uptake coefficient is enhanced by 17 times on mineral dust particles driven by CO3∙-. It can be produced through two routes over mineral dust surfaces: i) hydroxyl radical + CO32-; ii) holes (h+) + CO32-. Employing a suite of laboratory investigations of sulfate formation in the presence of carbonate radical on the model and authentic dust particles, field measurements of sulfate and (bi)carbonate ions within ambient PM, together with density functional theory (DFT) calculations for single electron transfer processes in terms of CO3∙--initiated S(IV) oxidation, a new role of carbonate radical in atmospheric chemistry is elucidated.

Carbonate Ion

Inert gas

Mineral dust

Atmospheric chemistry

Hydroxyl radical

10.5194/acp-2021-564

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Highly efficient photocatalytic H₂O₂production in microdroplets: accelerated charge separation and transfer at interfaces

Energy & Environmental Science (2023)

Kejian Li Qiuyue Ge Yangyang Liu Longqian Wang Kedong Gong

Photocatalytic H 2 O 2 production is significantly accelerated in microdroplets, benefiting from O 2 availability improvement, interfacial electric field, and reaction energy decrease.

10.1039/d2ee03774b

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Citations (50)

Atmospheric fates of SO₂ at the gas–solid interface of iron oxyhydroxide (FeOOH) minerals: effects of crystal structure, oxalate coating and light irradiance

Environmental Science Nano (2022)

Wei Wang Kejian Li Yangyang Liu Kedong Gong Qiuyue Ge

Heterogeneous SO 2 conversion over FeOOH minerals leads to the considerable formation of atmospheric sulfate aerosols, influenced by crystal structure, light irradiance and oxalate coating.

Crystal (programming language)

10.1039/d2en00874b

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New insights into the role of sulfite in BiOX photocatalytic pollutants elimination: In-operando generation of plasmonic Bi metal and oxygen vacancies

Journal of Hazardous Materials (2021)

Kejian Li Kedong Gong Juan Liu Yang Yang Iqra Nabi

Visible spectrum

10.1016/j.jhazmat.2021.126207

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Citations (37)

A novel pathway of atmospheric sulfate formation through carbonate radicals

Atmospheric chemistry and physics (2022)

Yangyang Liu Yue Deng Jiarong Liu Xiaozhong Fang Tao Wang

Abstract. Carbon dioxide is considered an inert gas that rarely participates in atmospheric chemical reactions. Nonetheless, we show here that CO2 is involved in some important photo-oxidation reactions in the atmosphere through the formation of carbonate radicals (CO3⚫-). This potentially active intermediate CO3⚫- is routinely overlooked in atmospheric chemistry concerning its effect on sulfate formation. The present work demonstrates that the SO2 uptake coefficient is enhanced by 17 times on mineral dust particles driven by CO3⚫-. Importantly, upon irradiation, mineral dust particles are speculated to produce gas-phase carbonate radical ions when the atmospherically relevant concentration of CO2 presents, thereby potentially promoting external sulfate aerosol formation and oxidative potential in the atmosphere. Employing a suite of laboratory investigations of sulfate formation in the presence of carbonate radicals on the model and authentic dust particles, ground-based field measurements of sulfate and (bi)carbonate ions within ambient PM, together with density functional theory (DFT) calculations for single electron transfer processes in terms of CO3⚫--initiated S(IV) oxidation, a novel role of carbonate radical in atmospheric chemistry is elucidated.

Carbonate Ion

Atmospheric chemistry

Inert gas

Mineral dust

10.5194/acp-22-9175-2022

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Citations (13)

Imaging of pH distribution inside individual microdroplet by stimulated Raman microscopy

Proceedings of the National Academy of Sciences (2023)

Kedong Gong Jianpeng Ao Kejian Li Le Liu Yangyang Liu

Aerosol microdroplets as microreactors for many important atmospheric reactions are ubiquitous in the atmosphere. pH largely regulates the chemical processes within them; however, how pH and chemical species spatially distribute within an atmospheric microdroplet is still under intense debate. The challenge is to measure pH distribution within a tiny volume without affecting the chemical species distribution. We demonstrate a method based on stimulated Raman scattering microscopy to visualize the three-dimensional pH distribution inside single microdroplets of varying sizes. We find that the surface of all microdroplets is more acidic, and a monotonic trend of pH decreasing is observed in the 2.9-μm aerosol microdroplet from center to edge, which is well supported by molecular dynamics simulation. However, bigger cloud microdroplet differs from small aerosol for pH distribution. This size-dependent pH distribution in microdroplets can be related to the surface-to-volume ratio. This work presents noncontact measurement and chemical imaging of pH distribution in microdroplets, filling the gap in our understanding of spatial pH in atmospheric aerosol.

10.1073/pnas.2219588120

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Citations (34)

Significantly Accelerated Hydroxyl Radical Generation by Fe(III)–Oxalate Photochemistry in Aerosol Droplets

The Journal of Physical Chemistry A (2023)

Longqian Wang Kejian Li Yangyang Liu Kedong Gong Juan Liu

Fe(III)-oxalate complexes are ubiquitous in atmospheric environments, which can release reactive oxygen species (ROS) such as H2O2, O•2-, and OH• under light irradiation. Although Fe(III)-oxalate photochemistry has been investigated extensively, the understanding of its involvement in authentic atmospheric environments such as aerosol droplets is far from enough, since the current available knowledge has mainly been obtained in bulk-phase studies. Here, we find that the production of OH• by Fe(III)-oxalate in aerosol microdroplets is about 10-fold greater than that of its bulk-phase counterpart. In addition, in the presence of Fe(III)-oxalate complexes, the rate of photo-oxidation from SO2 to sulfate in microdroplets was about 19-fold faster than that in the bulk phase. The availability of efficient reactants and mass transfer due to droplet effects made dominant contributions to the accelerated OH• and SO42- formation. This work highlights the necessary consideration of droplet effects in atmospheric laboratory studies and model simulations.

Hydroxyl radical

Atmospheric oxygen

10.1021/acs.jpca.2c05919

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Citations (5)

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

Atmospheric Environment (2022)

Yangyang Liu Tao Wang Qiuyue Ge Zhuocheng Shi Kejian Li

Deposition

10.1016/j.atmosenv.2022.119491

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Citations (5)

Comment on acp-2021-564

Yangyang Liu Yue Deng Jiarong Liu Xiaozhong Fang Tao Wang

Carbon dioxide is considered an inert gas that rarely participates in atmospheric chemical reactions. However, we show here that CO2 is involved in some important photo-oxidation reactions in the atmosphere through the formation of carbonate radicals (CO3â-). This potentially active intermediate CO3â- is routinely overlooked in atmospheric chemistry regarding its effect on sulfate formation. Present work demonstrates that SO2 uptake coefficient is enhanced by 17 times on mineral dust particles driven by CO3â-. It can be produced through two routes over mineral dust surfaces: i) hydroxyl radical + CO32-; ii) holes (h+) + CO32-. Employing a suite of laboratory investigations of sulfate formation in the presence of carbonate radical on the model and authentic dust particles, field measurements of sulfate and (bi)carbonate ions within ambient PM, together with density functional theory (DFT) calculations for single electron transfer processes in terms of CO3â--initiated S(IV) oxidation, a new role of carbonate radical in atmospheric chemistry is elucidated.

Carbonate Ion

Inert gas

Mineral dust

Atmospheric chemistry

Inert

10.5194/acp-2021-564-rc1

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Citations (0)

Carbonate radical ion as a key driver of rapid atmospheric sulfate formation

npj Climate and Atmospheric Science (2025)

Yangyang Liu Wei Li Qiuyue Ge Xiaozhong Fang Tao Wang

10.1038/s41612-025-00905-4

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