X-ray Spectroscopic Quantification of Phosphorus Transformation in Saharan Dust during Trans-Atlantic Dust Transport

Than T.N. Dam; Alon Angert; Michael D. Krom; Laura Bigio; Yongfeng Hu; Kevin A. Beyer; Olga L. Mayol-Bracero; Gilmarie Santos-Figueroa; Casimiro Pio; Mengqiang Zhu

doi:10.1021/acs.est.1c01573

X-ray Spectroscopic Quantification of Phosphorus Transformation in Saharan Dust during Trans-Atlantic Dust Transport

Than T.N. Dam, Alon Angert, Michael D. Krom, Laura Bigio, Yongfeng Hu, Kevin A. Beyer, Olga L. Mayol-Bracero, Gilmarie Santos-Figueroa, Casimiro Pio, Mengqiang Zhu^*

^*Corresponding author for this work

Fredy & Nadine Herrmann Institute of Earth Sciences

Research output: Contribution to journal › Article › peer-review

13 Scopus citations

Abstract

Saharan dust is an important phosphorus (P) supply to remote and oligotrophic parts of the oceans and American lowland tropical rainforests. Phosphorus speciation in aeolian dust ultimately controls the release and bioavailability of P after dust deposition, but the speciation in Saharan dust and its change during the trans-Atlantic transport remains unclear. Using P K-edge X-ray absorption near edge structure (XANES) spectroscopy, we showed that with increasing dust traveling distance from the Sahara Desert to Cape Verde and to Puerto Rico, about 570 and 4000 km, respectively, the proportion of Ca-bound P (Ca-P), including both apatite and non-apatite forms, decreased from 68-73% to 50-71% and to 21-37%. The changes were accompanied by increased iron/aluminum-bound P proportion from 14-25% to 23-46% and to 44-73%, correspondingly. Laboratory simulation experiments suggest that the changes in P speciation can be ascribed to increasing degrees of particle sorting and atmospheric acidification during dust transport. The presence of relatively soluble non-apatite Ca-P in the Cape Verde dust but not in the Puerto Rico dust is consistent with the higher P water solubility of the former than the latter. Our findings provide insights into the controls of atmospheric processes on P speciation, solubility, and stability in Saharan dust.

Original language	American English
Pages (from-to)	12694-12703
Number of pages	10
Journal	Environmental Science & Technology
Volume	55
Issue number	18
DOIs	https://doi.org/10.1021/acs.est.1c01573
State	Published - 21 Sep 2021

Bibliographical note

Funding Information:
This work was supported by the U.S. National Science Foundation Faculty Early Career Development Program (EAR-1752903). Dust and soil samples were collected during research projects funded by GIF Grant 1139/2011 and ISF Grant 870/08. O.L.M.-B and G.S.-F. thank the support of NSF AGS 0936879 and EAR-072247, the Conservation Trust of Puerto Rico for their use of their facilities at the nature reserve of Cabezas de San Juan, and the RISE program. A part of the research described in this work was performed at the Canadian Light Source, which is supported by the Natural Sciences and Engineering Research Council of Canada, the National Research Council Canada, the Canadian Institutes of Health Research, the Province of Saskatchewan, Western Economic Diversification Canada, and the University of Saskatchewan. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357.

Publisher Copyright:
© 2021 American Chemical Society

Keywords

Saharan dust
XANES spectroscopy
phosphorus
speciation
trans-Atlantic dust transport

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10.1021/acs.est.1c01573

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title = "X-ray Spectroscopic Quantification of Phosphorus Transformation in Saharan Dust during Trans-Atlantic Dust Transport",

abstract = "Saharan dust is an important phosphorus (P) supply to remote and oligotrophic parts of the oceans and American lowland tropical rainforests. Phosphorus speciation in aeolian dust ultimately controls the release and bioavailability of P after dust deposition, but the speciation in Saharan dust and its change during the trans-Atlantic transport remains unclear. Using P K-edge X-ray absorption near edge structure (XANES) spectroscopy, we showed that with increasing dust traveling distance from the Sahara Desert to Cape Verde and to Puerto Rico, about 570 and 4000 km, respectively, the proportion of Ca-bound P (Ca-P), including both apatite and non-apatite forms, decreased from 68-73% to 50-71% and to 21-37%. The changes were accompanied by increased iron/aluminum-bound P proportion from 14-25% to 23-46% and to 44-73%, correspondingly. Laboratory simulation experiments suggest that the changes in P speciation can be ascribed to increasing degrees of particle sorting and atmospheric acidification during dust transport. The presence of relatively soluble non-apatite Ca-P in the Cape Verde dust but not in the Puerto Rico dust is consistent with the higher P water solubility of the former than the latter. Our findings provide insights into the controls of atmospheric processes on P speciation, solubility, and stability in Saharan dust.",

keywords = "Saharan dust, XANES spectroscopy, phosphorus, speciation, trans-Atlantic dust transport",

author = "Dam, {Than T.N.} and Alon Angert and Krom, {Michael D.} and Laura Bigio and Yongfeng Hu and Beyer, {Kevin A.} and Mayol-Bracero, {Olga L.} and Gilmarie Santos-Figueroa and Casimiro Pio and Mengqiang Zhu",

note = "Funding Information: This work was supported by the U.S. National Science Foundation Faculty Early Career Development Program (EAR-1752903). Dust and soil samples were collected during research projects funded by GIF Grant 1139/2011 and ISF Grant 870/08. O.L.M.-B and G.S.-F. thank the support of NSF AGS 0936879 and EAR-072247, the Conservation Trust of Puerto Rico for their use of their facilities at the nature reserve of Cabezas de San Juan, and the RISE program. A part of the research described in this work was performed at the Canadian Light Source, which is supported by the Natural Sciences and Engineering Research Council of Canada, the National Research Council Canada, the Canadian Institutes of Health Research, the Province of Saskatchewan, Western Economic Diversification Canada, and the University of Saskatchewan. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Publisher Copyright: {\textcopyright} 2021 American Chemical Society",

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doi = "10.1021/acs.est.1c01573",

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AU - Dam, Than T.N.

AU - Angert, Alon

AU - Krom, Michael D.

AU - Bigio, Laura

AU - Hu, Yongfeng

AU - Beyer, Kevin A.

AU - Mayol-Bracero, Olga L.

AU - Santos-Figueroa, Gilmarie

AU - Pio, Casimiro

AU - Zhu, Mengqiang

N1 - Funding Information: This work was supported by the U.S. National Science Foundation Faculty Early Career Development Program (EAR-1752903). Dust and soil samples were collected during research projects funded by GIF Grant 1139/2011 and ISF Grant 870/08. O.L.M.-B and G.S.-F. thank the support of NSF AGS 0936879 and EAR-072247, the Conservation Trust of Puerto Rico for their use of their facilities at the nature reserve of Cabezas de San Juan, and the RISE program. A part of the research described in this work was performed at the Canadian Light Source, which is supported by the Natural Sciences and Engineering Research Council of Canada, the National Research Council Canada, the Canadian Institutes of Health Research, the Province of Saskatchewan, Western Economic Diversification Canada, and the University of Saskatchewan. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Publisher Copyright: © 2021 American Chemical Society

PY - 2021/9/21

Y1 - 2021/9/21

N2 - Saharan dust is an important phosphorus (P) supply to remote and oligotrophic parts of the oceans and American lowland tropical rainforests. Phosphorus speciation in aeolian dust ultimately controls the release and bioavailability of P after dust deposition, but the speciation in Saharan dust and its change during the trans-Atlantic transport remains unclear. Using P K-edge X-ray absorption near edge structure (XANES) spectroscopy, we showed that with increasing dust traveling distance from the Sahara Desert to Cape Verde and to Puerto Rico, about 570 and 4000 km, respectively, the proportion of Ca-bound P (Ca-P), including both apatite and non-apatite forms, decreased from 68-73% to 50-71% and to 21-37%. The changes were accompanied by increased iron/aluminum-bound P proportion from 14-25% to 23-46% and to 44-73%, correspondingly. Laboratory simulation experiments suggest that the changes in P speciation can be ascribed to increasing degrees of particle sorting and atmospheric acidification during dust transport. The presence of relatively soluble non-apatite Ca-P in the Cape Verde dust but not in the Puerto Rico dust is consistent with the higher P water solubility of the former than the latter. Our findings provide insights into the controls of atmospheric processes on P speciation, solubility, and stability in Saharan dust.

AB - Saharan dust is an important phosphorus (P) supply to remote and oligotrophic parts of the oceans and American lowland tropical rainforests. Phosphorus speciation in aeolian dust ultimately controls the release and bioavailability of P after dust deposition, but the speciation in Saharan dust and its change during the trans-Atlantic transport remains unclear. Using P K-edge X-ray absorption near edge structure (XANES) spectroscopy, we showed that with increasing dust traveling distance from the Sahara Desert to Cape Verde and to Puerto Rico, about 570 and 4000 km, respectively, the proportion of Ca-bound P (Ca-P), including both apatite and non-apatite forms, decreased from 68-73% to 50-71% and to 21-37%. The changes were accompanied by increased iron/aluminum-bound P proportion from 14-25% to 23-46% and to 44-73%, correspondingly. Laboratory simulation experiments suggest that the changes in P speciation can be ascribed to increasing degrees of particle sorting and atmospheric acidification during dust transport. The presence of relatively soluble non-apatite Ca-P in the Cape Verde dust but not in the Puerto Rico dust is consistent with the higher P water solubility of the former than the latter. Our findings provide insights into the controls of atmospheric processes on P speciation, solubility, and stability in Saharan dust.

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KW - XANES spectroscopy

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KW - speciation

KW - trans-Atlantic dust transport

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X-ray Spectroscopic Quantification of Phosphorus Transformation in Saharan Dust during Trans-Atlantic Dust Transport

Abstract

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Keywords

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