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Exploring the Radical Nature of a Carbon Surface by Electron Paramagnetic Resonance and a Calibrated Gas Flow
Published on: April 24, 2014
Interfacial Electric Fields Drive Fast Hydroxyl Radical Production in Black-Carbon-Bearing Microdroplets
Yangyang Liu1, Le Yang1, Qiuyue Ge1
1Shanghai Key Laboratory of Air Quality and Environmental Health, National Observations and Research Station for Wetland Ecosystems of the Yangtze Estuary, IRDR International Center of Excellence on Risk Interconnectivity and Governance on Weather, Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, Peoples' Republic of China.
Abstract:
While black carbon (BC) is generally recognized as a substrate for various heterogeneous atmospheric-relevant reactions of significance, its intrinsic oxidative potential─specifically the production of hydroxyl radicals (•OH)─has received minimal attention. Here, we demonstrate that the gas-liquid-solid interface of BC-bearing microdroplet aerosols functions as a highly active catalytic microreactor in the atmosphere. The interfacial environment leads to ultrafast •OH production (even up to ∼12 μmol s-1) via a mechanism driven by a strong electric field. This localized force induces Field-Induced Carrier Separation (FICS), which overcomes exciton binding energy and suppresses electron-hole recombination. Furthermore, we identify a synergy between this electric field and photoaging that promotes surface defect proliferation, establishing a positive feedback loop that sustains rapid redox cycling. These findings reveal BC aerosols not merely as a radiative forcing agent, but as potent, overlooked natural "photocatalysts" that significantly amplify atmospheric oxidative capacity and accelerate secondary aerosol formation.
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