Deciphering the Distribution and Crystal-Chemical Environment of Arsenic, Lead, Silica, Phosphorus, Tin, and Zinc in a Porous Ferrihydrite Grain Using Transmission Electron Microscopy and Atom Probe Tomography
Abstract
Here the interaction of contaminants and nutrients with soil constituents is controlled by processes in intergranular and intragranular pore spaces of organic matter or/and common secondary minerals such as ferrihydrite, ~Fe3+10O14(OH)2. This contribution shows that distribution and clustering of the contaminants As, P, Pb, Si, Sn, and Zn in a porous ferrihydrite grain is greatly affected by the heterogeneous size distribution and chemical composition of the pores as well as the ability of their polyhedra to polymerize with the same type of polyhedron. Transmission electron microscopy (TEM) and atom probe tomography (APT) studies are conducted on focused ion beam (FIB) sections extracted from a porous ferrihydrite grain from the smelter-impacted topsoil in Sudbury, Ontario, Canada. The ferrihydrite grain has pore spaces ranging in diameter from tens to hundreds of nanometers. TEM and scanning-TEM studies indicate that the surfaces of the pore walls are enriched in Si. APT data in conjunction with First Near Neighbor (1NN) analyses indicate different degrees of clustering of Pb, As, Sn, Zn, Si, and P within the sample and selected domains. Careful evaluations of 3D atomic plots and 1NN distances indicates the occurrence of polymerized arsenite-, silica-, Sn-, and Zn-polyhedra within pore spaces of the ferrihydrite.more »
- Authors:
-
[1];
[2];
[2]
- Univ. of Manitoba, Winnipeg, MB (Canada)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1865149
- Report Number(s):
- PNNL-SA-168344
Journal ID: ISSN 2472-3452
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Earth and Space Chemistry
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 3; Journal ID: ISSN 2472-3452
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; atom probe tomography (APT); transmission electron microscopy (TEM); ferrihydrite; porosity; arsenic; lead; phosphate; silica
Citation Formats
Schindler, Michael, Schreckenbach, Max, Akbari Alavijeh, Mozhgan, Wirth, Mark G., Qafoku, Odeta, Kovarik, Libor, and Perea, Daniel E. Deciphering the Distribution and Crystal-Chemical Environment of Arsenic, Lead, Silica, Phosphorus, Tin, and Zinc in a Porous Ferrihydrite Grain Using Transmission Electron Microscopy and Atom Probe Tomography. United States: N. p., 2022.
Web. doi:10.1021/acsearthspacechem.1c00374.
Schindler, Michael, Schreckenbach, Max, Akbari Alavijeh, Mozhgan, Wirth, Mark G., Qafoku, Odeta, Kovarik, Libor, & Perea, Daniel E. Deciphering the Distribution and Crystal-Chemical Environment of Arsenic, Lead, Silica, Phosphorus, Tin, and Zinc in a Porous Ferrihydrite Grain Using Transmission Electron Microscopy and Atom Probe Tomography. United States. https://doi.org/10.1021/acsearthspacechem.1c00374
Schindler, Michael, Schreckenbach, Max, Akbari Alavijeh, Mozhgan, Wirth, Mark G., Qafoku, Odeta, Kovarik, Libor, and Perea, Daniel E. Mon .
"Deciphering the Distribution and Crystal-Chemical Environment of Arsenic, Lead, Silica, Phosphorus, Tin, and Zinc in a Porous Ferrihydrite Grain Using Transmission Electron Microscopy and Atom Probe Tomography". United States. https://doi.org/10.1021/acsearthspacechem.1c00374. https://www.osti.gov/servlets/purl/1865149.
@article{osti_1865149,
title = {Deciphering the Distribution and Crystal-Chemical Environment of Arsenic, Lead, Silica, Phosphorus, Tin, and Zinc in a Porous Ferrihydrite Grain Using Transmission Electron Microscopy and Atom Probe Tomography},
author = {Schindler, Michael and Schreckenbach, Max and Akbari Alavijeh, Mozhgan and Wirth, Mark G. and Qafoku, Odeta and Kovarik, Libor and Perea, Daniel E.},
abstractNote = {Here the interaction of contaminants and nutrients with soil constituents is controlled by processes in intergranular and intragranular pore spaces of organic matter or/and common secondary minerals such as ferrihydrite, ~Fe3+10O14(OH)2. This contribution shows that distribution and clustering of the contaminants As, P, Pb, Si, Sn, and Zn in a porous ferrihydrite grain is greatly affected by the heterogeneous size distribution and chemical composition of the pores as well as the ability of their polyhedra to polymerize with the same type of polyhedron. Transmission electron microscopy (TEM) and atom probe tomography (APT) studies are conducted on focused ion beam (FIB) sections extracted from a porous ferrihydrite grain from the smelter-impacted topsoil in Sudbury, Ontario, Canada. The ferrihydrite grain has pore spaces ranging in diameter from tens to hundreds of nanometers. TEM and scanning-TEM studies indicate that the surfaces of the pore walls are enriched in Si. APT data in conjunction with First Near Neighbor (1NN) analyses indicate different degrees of clustering of Pb, As, Sn, Zn, Si, and P within the sample and selected domains. Careful evaluations of 3D atomic plots and 1NN distances indicates the occurrence of polymerized arsenite-, silica-, Sn-, and Zn-polyhedra within pore spaces of the ferrihydrite. Deciphering adsorption, polymerization, and nucleation processes in porous Fe-(hydr)oxides and other soil constituents requires multianalytical approaches and, in this regard, we discuss the advantages and disadvantages of the combination of TEM and APT for characterizing complex environmental samples at the atomic to nanometer scale.},
doi = {10.1021/acsearthspacechem.1c00374},
journal = {ACS Earth and Space Chemistry},
number = 3,
volume = 6,
place = {United States},
year = {Mon Feb 28 00:00:00 EST 2022},
month = {Mon Feb 28 00:00:00 EST 2022}
}
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