Abstract Trifluoroacetic acid (TFA) is a persistent pollutant with potential long‐term effects on the environment and on health. Recent studies using ice core records report large increases (up to tenfold) in Arctic TFA deposition since the 1970s, and trends suggest long‐lived chlorofluorocarbon (CFC) replacements may be a major source. Here, we use a chemical transport model to examine the global TFA budget arising from CFC replacements–hydrochlorofluorocarbons (HCFCs), hydrofluorocarbons (HFCs)–and inhalation anesthetics. Global TFA deposition from these sources increased ∼3.5‐fold from 6.8 (5.9–7.6) Gg/yr in 2000 to 21.8 (18.6–25.0) Gg/yr in 2022, with cumulative deposition reaching 335.5 Gg. We find HCFC‐123, HCFC‐124, and HFC‐134a account for most modeled TFA production and that long‐lived CFC replacements account for virtually all of the observed Arctic deposition trend. At lower latitudes, our analysis supports the recent emergence of hydrofluoroolefins (HFOs) as a TFA source. We conclude that increased TFA monitoring is required.

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