TY - JOUR
T1 - Photochemistry of aqueous C60 clusters
T2 - Evidence of 1O2 formation and its role in mediating C60 phototransformation
AU - Hou, Wen Che
AU - Jafvert, Chad T.
PY - 2009/7/15
Y1 - 2009/7/15
N2 - The expected rapid expansion of nanotechnology industries has raised concern over the environmental fate and effects of materials created by these industries, including carbon-based fullerenes. In this study, there action mechanism responsible for the photochemical transformation of aqueous C 60 clusters (nC60) in sunlight has been examined. Evidence is presented that under lamps that emit light only within the solar spectrum, 1O2 is produced via aqueous nC60 suspensions, using furfuryl alcohol (FFA) as an indicator. In air-equilibrated suspensions, the losses of 0.2 mM FFA and 0.8 mg/L C60 were >90% and 70% after 15 h, while removing oxygen, the precursor of 1O2, stopped both reactions, indicating that 1O2 was produced and mediated nC 60 phototransformation. Similar reactions performed in deuterium oxide and with added azide ion resulted in accelerated and slowed loss of FFA, respectively, as expected if 1O2 is a reaction intermediate. 1 O2 production (as measured by FFA loss) increased with time as more water-soluble intermediate products accumulated in solution. In summer sunlight (West Lafayette, IN, 86° 55′ W, 40° 26′ N), suspensions of 5 mg/L nC60 produced 1O2 concentrations 1 order of magnitude higher than the average value typically found in natural waters containing the same mass of natural organic carbon.
AB - The expected rapid expansion of nanotechnology industries has raised concern over the environmental fate and effects of materials created by these industries, including carbon-based fullerenes. In this study, there action mechanism responsible for the photochemical transformation of aqueous C 60 clusters (nC60) in sunlight has been examined. Evidence is presented that under lamps that emit light only within the solar spectrum, 1O2 is produced via aqueous nC60 suspensions, using furfuryl alcohol (FFA) as an indicator. In air-equilibrated suspensions, the losses of 0.2 mM FFA and 0.8 mg/L C60 were >90% and 70% after 15 h, while removing oxygen, the precursor of 1O2, stopped both reactions, indicating that 1O2 was produced and mediated nC 60 phototransformation. Similar reactions performed in deuterium oxide and with added azide ion resulted in accelerated and slowed loss of FFA, respectively, as expected if 1O2 is a reaction intermediate. 1 O2 production (as measured by FFA loss) increased with time as more water-soluble intermediate products accumulated in solution. In summer sunlight (West Lafayette, IN, 86° 55′ W, 40° 26′ N), suspensions of 5 mg/L nC60 produced 1O2 concentrations 1 order of magnitude higher than the average value typically found in natural waters containing the same mass of natural organic carbon.
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U2 - 10.1021/es900624s
DO - 10.1021/es900624s
M3 - Article
C2 - 19708350
AN - SCOPUS:67650456895
SN - 0013-936X
VL - 43
SP - 5257
EP - 5262
JO - Environmental Science and Technology
JF - Environmental Science and Technology
IS - 14
ER -