TY - JOUR
T1 - Enhanced release of palladium and platinum from catalytic converter materials exposed to ammonia and chloride bearing solutions
AU - Aruguete, Deborah M.
AU - Murayama, Mitsuhiro
AU - Blakney, Terry
AU - Winkler, Christopher
N1 - Funding Information:
This project was supported by Penn State Behrend startup funds (DMA), the Virginia Tech National Center for Earth and Environmental Nanotechnology Infrastructure (NanoEarth), a member of the National Nanotechnology Coordinated Infrastructure (NNCI), supported by NSF (ECCS 1542100). The transmission electron microscopy was carried out at the Virginia Tech Nanoscale Characterization and Fabrication Laboratory (ICTAS-NCFL) and the elemental analysis at the Penn State Energy and Environmental Laboratories (EESL). DMA thanks the following Penn State personnel: Mr Matthew Gon-zales (Penn State EESL) for extensive discussion on ICP-MS data and Ms. Rose Kerr (Penn State Behrend) for laboratory assistance. She thanks the following Virginia Tech faculty, students, and staff for assistance with instrumentation and laboratory space: Mr Rui Serra Maia, Ms. Athena Tilley, Dr Weinan Leng, Dr Michael Hochella, and Dr Marc Michel. She thanks Dr Lisa Nogaj of Gannon University for providing access to an ultracentrifuge. She is grateful to Dr William Casey (UC Davis) and Dr Bernhard Peucker-Ehrenbrink (Woods Hole Oceanographic) for insightful discussions that inspired this research, and Dr Adam Wallace (U Delaware) for reviewing this paper. Finally, she thanks the two anonymous reviewers for suggestions that improved this paper signicantly.
Publisher Copyright:
© 2019 The Royal Society of Chemistry.
PY - 2019/1
Y1 - 2019/1
N2 - The environmental levels of platinum group elements (PGEs) are steadily rising, primarily due to exhaust emissions of vehicle catalytic converter (VCC) materials containing solid PGEs. Once these VCC materials reach soil and water, the PGEs may be transported in the form of nanoparticles (dimensions 1-100 nm) or they may be mobilized by forming coordination complexes with ligands in the environment. Chloride (Cl-) and ammonia (NH3) are two ligands of particular concern due to their ubiquity as well as their potential to form the chemotherapy drug cisplatin (Pt(NH3)2Cl2) or other potentially bioactive complexes. This initial study examines the release of Pd and Pt into solutions exposed to VCC materials at pH 8 and 25 °C, using elemental analysis of metal content in post-exposure extracts. The solutions had total ammonia nitrogen concentrations (TAN, [NH4+] + [NH3]) of 0 μM, 5.56 μM, 55.6 μM and 1.13 × 105 μM (0 ppm, 0.1 ppm, 1 ppm, and 2147 ppm). The former three represent background environmental levels had a minimal effect on release. However, when combined with 1.13 × 105 μM Cl- (4000 ppm Cl-), 55.6 μM TAN induced a marked increase in metal release (∼41× for Pd). High TAN solutions induced more Pd and Pt release than equimolar NaCl solutions. Materials characterization revealed that ∼4 nm palladium-containing nanoparticles were present, spatially associated with nanoparticles of γ-Al2O3; ceria-zirconia nanoparticles were also present but did not have any metal associated with them. Platinum-containing nanoparticles were not observed.
AB - The environmental levels of platinum group elements (PGEs) are steadily rising, primarily due to exhaust emissions of vehicle catalytic converter (VCC) materials containing solid PGEs. Once these VCC materials reach soil and water, the PGEs may be transported in the form of nanoparticles (dimensions 1-100 nm) or they may be mobilized by forming coordination complexes with ligands in the environment. Chloride (Cl-) and ammonia (NH3) are two ligands of particular concern due to their ubiquity as well as their potential to form the chemotherapy drug cisplatin (Pt(NH3)2Cl2) or other potentially bioactive complexes. This initial study examines the release of Pd and Pt into solutions exposed to VCC materials at pH 8 and 25 °C, using elemental analysis of metal content in post-exposure extracts. The solutions had total ammonia nitrogen concentrations (TAN, [NH4+] + [NH3]) of 0 μM, 5.56 μM, 55.6 μM and 1.13 × 105 μM (0 ppm, 0.1 ppm, 1 ppm, and 2147 ppm). The former three represent background environmental levels had a minimal effect on release. However, when combined with 1.13 × 105 μM Cl- (4000 ppm Cl-), 55.6 μM TAN induced a marked increase in metal release (∼41× for Pd). High TAN solutions induced more Pd and Pt release than equimolar NaCl solutions. Materials characterization revealed that ∼4 nm palladium-containing nanoparticles were present, spatially associated with nanoparticles of γ-Al2O3; ceria-zirconia nanoparticles were also present but did not have any metal associated with them. Platinum-containing nanoparticles were not observed.
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U2 - 10.1039/c8em00370j
DO - 10.1039/c8em00370j
M3 - Article
C2 - 30520493
AN - SCOPUS:85060403232
SN - 2050-7887
VL - 21
SP - 133
EP - 144
JO - Journal of Environmental Monitoring
JF - Journal of Environmental Monitoring
IS - 1
ER -