RESEARCH ARTICLE · Science Advances · 2025

Beyond the tropopause hypothesis: Drivers of even mercury isotope fractionation unraveled by 3D modeling

Zhengcheng Song, Shaojian Huang, Peng Zhang, Tengfei Yuan, Xin Miao, Kaihui Tang, Sun Guangyi, Xuewu Fu, Ruoyu Sun, Wang Zheng, Jiubin Chen, Yanxu Zhang

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Abstract

Mercury (Hg) is a globally persistent contaminant with substantial health impact. The mass-independent fractionation of even mercury isotopes (even-MIF, denoted as Δ 200 Hg) is widely used to trace atmospheric Hg sources and fluxes. However, the chemical processes inducing even-MIF remain largely unknown. Here, we develop a three-dimensional atmospheric Hg isotope model linking Hg redox processes with even-MIF. The results show that the previous hypothesis of even-MIF occurring exclusively at the tropopause may not fully explain the global Δ 200 Hg patterns. We speculate OH-initiated reactions and photoreduction of Hg II (p) as likely dominant drivers. Simulations show that even-MIF primarily originates in the free troposphere and propagates downward to surface air. Our results reveal distinct spatial Δ 200 Hg variations that were previously unaccounted for in tracing Hg sources. This study provides critical insights into even-MIF drivers and serves as a reference for using Δ 200 Hg to trace atmospheric Hg sources.

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