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Record of pre-industrial atmospheric sulfate in continental interiors

Nature Geoscience volume 16, pages 619–624 (2023)Cite this article

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Abstract

Sulfate aerosols affect climate by scattering radiation and by changing the microphysical properties of water clouds. In much of the continental interiors that are overwhelmed by anthropogenic sulfate today, the nature of pre-industrial atmospheric sulfate remains pure speculation, which hampers our ability to quantify anthropogenic perturbation on climate and uncertainties in global climate models. Here we show that sequential leaching and multiple-isotope measurement enabled us to effectively distinguish sulfate of different origins, including pre-industrial atmospheric sulfate, retained in certain outcropping carbonates. Data from two interior sites in northern China show that one of the sulfate endmembers consistently has an unusually positive 17O anomaly (Δʹ17O at ~+1.8‰) and characteristic δ18O (~1–5‰) and δ34S (~5–10‰) values. We interpret this sulfate endmember to be integrated pre-industrial atmospheric sulfate from at least the last a few thousands of years. A triple oxygen isotope enabled GEOS-Chem chemical transport model revealed a higher Δʹ17O value in northern China and the south-western United States in the past, consistent with our data. Overall, pre-industrial atmospheric sulfate aerosol chemistry in the interior of northern China and south-western United States had a higher pH in cloud water, which may have led to a less cloud cover due to cleaner air and coarser aerosol sizes than today.

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Fig. 1: Cross plots of Δʹ17O-δ34S, Δʹ17O-δ18O and δ18O-δ34S.
Fig. 2: Difference of Δʹ17O values of tropospheric sulfate and the conversion efficiency from SO2 to sulfate between 1986 and 1750.

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Code availability

The GEOS-Chem model used in this study is available at https://doi.org/10.5281/zenodo.3403111. The code used to run the model and to analyse the results is not publicly available, but can be provided upon request by contacting S.H. (hattori@nju.edu.cn).

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Acknowledgements

Financial support is provided by the National Key Research and Development Program of China (2022YFF0800303), the National Natural Science Foundation of China (42173001, 41490635 and 41672334), Nanjing University Start-up fund (to H.B.), MEXT/JSPS KAKENHI (JP16H0584 and JP20H04305), Fundamental Research Funds for the Central Universities (0206/14380150, 0206/14380185 and 0206/14380174), Natural Science Foundation of Henan (202300410178) and Key Scientific Research Project in Colleges and Universities of Henan (18A170001). We thank S. Zhai and S. Ishino for providing support for handling the GEOS-Chem model.

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Authors and Affiliations

  1. International Center for Isotope Effects Research, Nanjing University, Nanjing, China

    Yongbo Peng, Shohei Hattori, Haoran Ma & Huiming Bao

  2. Frontiers Science Center for Critical Earth Material Cycling, State Key Laboratory for Mineral Deposits Research, School of Earth Sciences and Engineering, Nanjing University, Nanjing, China

    Yongbo Peng, Shohei Hattori, Haoran Ma & Huiming Bao

  3. Institute of Nature and Environment Technology, Kanazawa University, Ishikawa, Japan

    Shohei Hattori

  4. School of Resources and Environment, Henan Polytechnic University, Jiaozuo, China

    Pengfei Zuo

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Contributions

H.B., Y.P. and S.H. conceived the research idea; Y.P., P.Z. and H.M. did the analytical treatments; S.H. contributed to the model simulations; and H.B. wrote the paper with writing contributions from all co-authors.

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Correspondence to Huiming Bao.

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Nature Geoscience thanks Theodore Present and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Primary Handling Editor(s): James Super, in collaboration with the Nature Geoscience team.

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Extended data

Extended Data Table 1 Sample names and sulfur and triple oxygen isotope composition of sulfate leached from carbonate outcrops of three sites
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Peng, Y., Hattori, S., Zuo, P. et al. Record of pre-industrial atmospheric sulfate in continental interiors. Nat. Geosci. 16, 619–624 (2023). https://doi.org/10.1038/s41561-023-01211-5

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