TECHNICAL PAPERS
Feb 1, 2005

Repeated Reductive and Oxidative Treatments of Granular Activated Carbon

Publication: Journal of Environmental Engineering
Volume 131, Issue 2

Abstract

Fenton oxidation and reductive treatment solutions were applied to granular activated carbon (GAC) to chemically regenerate the adsorbent. No adsorbate was present on the GAC so physicochemical effects from chemically aggressive regeneration could be distinguished from the potential effects of accumulation of reaction byproducts. Fifteen sequential oxidation treatments with hydrogen peroxide (H2O2) and fifteen sequential reduction/oxidation treatments with hydroxylamine and H2O2 on Fe-amended GAC were evaluated. The GAC Iodine number, N2 Brunauer–Emmett–Teller surface area, microporosity, and total porosity declined with sequential treatments, but meso- and macroporosity essentially remained unchanged. Similar changes in Iodine number, surface area, and pore volume distribution suggest that the effects of treatment are functionally dependent on oxidation and independent of hydroxylamine reduction. An inverse relationship was established between the number of chemical treatments and contaminant (methyl tert-butyl ether, 2-chlorophenol, trichloroethylene) adsorption. Loss in sorptive capacity was attributed to the combined and undifferentiated effects of reductions in microporosity and surface area, alterations in surface chemistry (overabundance of surface oxides), and to a lesser degree, micropore blockage by iron oxides.

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Acknowledgments

The writers acknowledge S. Beach, M. Blankenship, Dr. D. Fine, Dr. G. Jungclaus, Dr. W. Lyon, A. Mitchell, L. Pennington, Dr. B. Pivetz, Dr. J. Qian, and Dr. N. Xu (ManTech Environmental Research Services Corp., Ada, Okla.), and D. Rushing (East Central University, Ada, OK) for their invaluable assistance.

References

American Society for Testing Materials (ASTM). (1998). “Standard test method for the determination of iodine number of activated carbon.” ASTM Method No. D 4607-94, Annual Book of ASTM Standards Method, Philadelphia.
Boehm, H. P (1966). “Chemical identification of surface group.” Advances in catalysis, P. P. Eley, H. Pines, and P. B. Weisz, eds., Vol. 16, Academic, New York, 179.
Boltz, D. F., and Howell, J. A. eds. (1978). Colorimetric determination of nonmetals, Wiley–Interscience, New York
Buxton, G. V., Greenstock, C., Hellman, W. P., and Ross, A. B. (1988). “Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms, and hydroxyl radicals (OHO) in aqueous solution.” J. Phys. Chem. Ref. Data, 17(2), 513–886.
Carrasco-Marin, F., Mueden, A., Centeno, T. A., Stoeckli, F., and Moreno-Castilla, C. J. (1997). “Water adsorption on activated carbons with different degrees of oxidation.” J. Chem. Soc., Faraday Trans., 93(12), 2211–2215.
Choma, J., Burakiewicz-Mortka, W., Jaroniec, M., Li, Z., and Klinik, J. (1999). “Monitoring changes in surface and structural properties of porous carbons modified by different oxidizing agents.” J. Colloid Interface Sci., 214, 438–446.
Cookson, J. T. (1980). Activated carbon adsorption of organics from the aqueous phase, Vol. 1., I. H. Suffet and M. J. McGuire, eds. Ann Arbor Science Publishers, Ann Arbor, Mich. 379–396.
Franz, M., Arafat, H. A., and Pinto, N. G. (2000). “Effect of chemical surface heterogeneity on the adsorption mechanisms of dissolved aromatics on activated carbon.” Carbon, 38, 1807–1819.
Gil, A., de la Puente, G., and Grange, P. (1997). “Evidence of textural modifications of an activated carbon on liquid-phase oxidation treatments.” Microporous Mater., 12, 51–61.
Gregg, S. J., and Sing, K. S. W. (1982). Adsorption, surface area, and porosity, 2nd Ed. Academic, London.
Huling, S. G., Arnold, R. G., Sierka, R. A., and Miller, M. R. (1998). “Measurement of hydroxyl radical activity in a soil slurry using 4POBN.” Environ. Sci. Technol., 32(21), 3436–3441.
Huling, S. G., Arnold, R. G., Jones, P. K., and Sierka, R. A. (2000a). “Predicting Fenton-driven degradation using a contaminant analog.” J. Environ. Eng., 126(4), 348–353.
Huling, S. G., Arnold, R. G., Sierka, R. A., Jones, P. K., and Fine, D. (2000b). “Contaminant adsorption and oxidation via Fenton reaction.” J. Environ. Eng., 126(7), 595–600.
Huling, S. G., Arnold, R. G., Sierka, R. A., and Miller, M. A. (2001). “Influence of peat on Fenton oxidation.” Water Res., 35(7), 1687–1694.
Huling, S. G., Jones, P. K., Arnold, R. G., and Ela, W. P. (2004). “Fenton-driven chemical regeneration of MTBEspent granular activated carbon.” Water Res. (in press).
Karanfil, T., Schlautman, M. A., Kilduff, J. E., and Weber, W. J. (1994). “Impacts of dissolved oxygen on the sorption of humic substances and the subsequent inhibition of o-cresol uptake by granular activated carbon.” Water Res., 28(7), 1673–1678.
Karanfil, T., Schlautman, M. A., Kilduff, J. E., and Weber, W. J. (1996). “Adsorption of organic macromolecules by granular activated carbon. II: Influence of dissolved oxygen.” Environ. Sci. Technol., 30(7), 2195–2201.
Karanfil, T., and Kilduff, J. E. (1999). “Role of granular activated carbon surface chemistry on the adsorption of organic compounds. I:Priority pollutants.” Environ. Sci. Technol., 33(18), 3217–3224.
Kilduff, J. E., and King, J. C. (1997). “Effect of carbon adsorbent surface properties on the uptake and solvent regeneration of phenol.” Ind. Eng. Chem. Res., 36(5), 1603–1613.
Kommineni, S., et al. (2002). “NDMA treatment by sequential GAC adsorption and Fenton-driven destruction.” Environ. Eng. Sci., 20(4), 361–373.
Leon, C. A., Leon, D., and Radovic, L. R. (1994). “Interfacial chemistry and electrochemistry of carbon surfaces.” Chem. Phys. Carbon, 24, 213–310.
Li, L., Quinlivan, P. A., and Knappe, D. R. U. (2002). “Effects of activated carbon surface chemistry and pore structure on the adsorption of organic contaminants from aqueous solution.” Carbon, 40, 2085–2100.
Mackay, D., Shiu, W. Y., and Ma, K. C. (1993). Illustrated handbook of physical–chemical properties of environmental fate for organic chemicals, Lewis, Boca Raton, Fla.
McClure, A., and Megonnell, N. (2000). “A big advance in cleaning up small MTBE levels.” Environ. Prot., 2(5), 20–25.
Moreno-Castilla, C. (1995). “Activated carbon surface modifications by nitric acid, hydrogen peroxide, and ammonium persulfate treatments.” Langmuir, 11, 4386–4392.
Pendleton, P. (1997). “Properties of activated carbon controlling 2-Methylisoborneol adsorption.” Carbon, 35(8), 1141–1149.
Reed, B. E., Vaughan, R., and Jiang, L. (2000). “As (III), As (V), Hg, and Pb removal by Fe-oxide impregnated activated carbon.” J. Environ. Eng., 126(9), 869–873.
Schwertman, U. (1990). Soil colloids and their associations in aggregates, M. F. deBoot, M. H. B. Hayes, and A. Herbillion, eds., Plenum, New York, 57–103.
Smith, B. F. L., and Mitchell, B. D. (1987). A handbook of determinative methods in clay mineralogy, Chap. 8, M. J. Wilson, ed., Chapman and Hall, New York, 275–294.
Snoeyink, V. L., Lai, H. T., Johnson, J. H., and Young, J. F. (1974). Symposium on the chemistry of water supply, treatment, and distribution, Ann Arbor Science Publishers, Ann Arbor, Mich., 232–252.
Suh, D. J., Park, T. J., and Ihm, S. K. (1993). “Effects of surface oxygen groups of carbon supports on the characteristics of PdC catalysts.” Carbon, 31(3), 427–435.
Vidic, R. D., and Suidan, M. T. (1991). “Role of dissolved oxygen on the adsorption capacity of activated carbon for synthetic and natural organic matter.” Environ. Sci. Technol., 25(9), 1612–1618.
Zeid, N. A., Nakhla, G., Farooq, S., and Osei-Twum, E. (1995). “Activated carbon adsorption in oxidizing environments.” Water Res., 29(2), 653–660.

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Published In

Go to Journal of Environmental Engineering
Journal of Environmental Engineering
Volume 131Issue 2February 2005
Pages: 287 - 297

History

Received: Aug 18, 2003
Accepted: Dec 30, 2003
Published online: Feb 1, 2005
Published in print: Feb 2005

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Authors

Affiliations

Scott G. Huling [email protected]
Environmental Engineer, U.S. Environmental Protection Agency, Office of Research and Development, National Risk Management Research Laboratory, P.O. Box 1198, Ada, OK 74820 (corresponding author). E-mail: [email protected]
Patrick K. Jones
Chemist, U.S. Environmental Protection Agency, Office of Research and Development, National Risk Management Research Laboratory, P.O. Box 1198, Ada, OK 74820.
Wendell P. Ela, M.ASCE
Assistant Professor, Dept. of Chemical and Environmental Engineering, Univ. of Arizona at Tucson, Tucson, AZ 85721.
Robert G. Arnold, M.ASCE
Professor, Dept. of Chemical and Environmental Engineering, Univ. of Arizona at Tucson, Tucson, AZ 85721.

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