Abstract
The advances in understanding the kinetic behavior of certain environmental electron transfer (ET) systems are presented. Emphasis is placed on the homogeneous ET chemistry of transition metals, particularly the FeII/III system, in various relevant forms. In the context of modern ET theory, we examine the utility of computational chemistry methods for the calculation of ET quantities such as the reorganization energy and electronic coupling matrix element. We discuss successful application of the methods to topics of homogeneous oxidation of dissolved metal ions by molecular oxygen in aqueous solution, as well as the prediction of electron mobility in solid phase iron oxide crystals. The examples illustrate the significant potential for many more advances in understanding environmental ET systems through the combination of ET theory and computational chemistry.
Article PDF
Similar content being viewed by others
Avoid common mistakes on your manuscript.
References
Stumm W, Morgan JJ (1981) Aquatic chemistry. Wiley, New York
Zachara JM, Fredrickson JK, Li SM, Kennedy DW, Smith SC, Gassman PL (1998). Am Mineral 83:1426
Rosso KM, Smith DMA, Wang ZM, Ainsworth CC, Fredrickson JK (2004). J Phys Chem 108:3292
Newman DK, Kolter R (2000). Nature 405:94
Nurmi JT, Tratnyek PG (2002). Environ Sci Technol 36:617
Maurice PA, Hochella MF Jr, Parks GA, Sposito G, Schwertmann U (1995). Clays Clay Miner 43:29
Stone AT, Morgan JJ (1987) In: Stumm W (ed) Aquatic surface chemistry, Wiley, New York, p 221
Ilton ES, Haiduc A, Moses CO, Heald SM, Elbert DC, Veblen DR (2004). Geochim Cosmochim Acta 68:2417
Peterson ML, White AF, Brown GE Jr, Parks GA (1997). Environ Sci Technol 31:1573
Cui DQ, Eriksen TE (1996). Environ Sci Technol 30:2263
Scott MJ, Morgan JJ (1996). Environ Sci Technol 30:1990
Elsner M, Haderlein SB, Kellerhals T, Luzi S, Zwank L, Angst W, Schwarzenbach RP (2004). Environ Sci Technol 38:2058
Strathmann TJ, Stone AT (2003). Geochim Cosmochim Acta 67:2775
Pecher K, Haderlein SB, Schwarzenbach RP (2002). Environ Sci Technol 36:1734
Amonette JE, Workman DJ, Kennedy DW, Fruchter JS, Gorby YA (2000). Environ Sci Technol 34:4606
Butler EC, Hayes KF (1998). Environ Sci Technol 32:1276
Marcus RA (1956). J Chem Phys 24:966
Sutin N (1962). Annu Rev Nucl Sci 12:285
Dogonadze RR, Kuznetsov AM, Zakaraya MG, Ulstrup J, Inst Electrochem MU (1979). Tunneling Biol Syst [Proc Symp], p 145
Hush NS (1967). Prog Inorg Chem 8:391
Bricker O (1965). Am Mineral 50:1296
Diem D, Stumm W (1984). Geochim Cosmochim Acta 48:1571
Singer PC, Stumm W (1970). Science 167:1121
Lowson RT (1982). Chem Rev 82:461
Millero FJ (1985). Geochim Cosmochim Acta 49:547
Millero FJ, Sotolongo S, Izaguirre M (1987). Geochim Cosmochim Acta 51:793
Millero FJ, Izaguirre M (1989). J Sol Chem 18:585
Millero FJ (1989). Mar Chem 28:1
King DW, Lounsbury HA, Millero FJ (1995). Environ Sci Technol 29:818
King DW (1998). Environ Sci Technol 32:2997
Morgan JJ (2005). Geochim Cosmochim Acta 69:35
Hem JD (1963). US Geol Soc Water Supp 1667-A:A1
Morgan JJ (1967) In: Faust S, Hunter J (eds) Principles and applications of water chemistry. Wiley, New York, p 561
Sellers RM, Simic MG (1976). J Am Chem Soc 98:6145
Bakac A, Espenson JH (1993). Acc Chem Res 26:519
Bakac A, Scott SL, Espenson JH, Rodgers KR (1995). J Am Chem Soc 117:6483
Mulvaney P, Swayambunathan V, Grieser F, Meisel D (1988). J Phys Chem 92:6732
Mulvaney P, Cooper R, Grieser F, Meisel D (1988). Langmuir 4:1206
Mulvaney P, Swayambunathan V, Grieser F, Meisel D (1990). Langmuir 6:555
Rosso KM, Smith DMA, Dupuis M (2003). J Chem Phys 118:6455
Williams AGB, Scherer MM (2004). Environ Sci Technol 38:4782
Rosso KM, Zachara JM, Fredrickson JK, Gorby YA, Smith SC (2003). Geochim Cosmochim Acta 67:1081
Freier S, Greenshpan P, Hillman P, Shechter H (1962). Phys Lett 2:191
Lielmezs J, Chaklader ACD (1965). J Appl Phys 36:866
Ma Y, Johnson PD, Wassdahl N, Guo J, Skytt P, Nordgren J, Kevan SD, Rubensson J-E, Boske T, Eberhardt W (1993). Phys Rev B 48:2109
Mochizuki S (1977). Physica Status Solidi A 41:591
Morin FJ (1954). Phys Rev 93:1195
Goodenough JB (1971) In: Reiss H (ed) Progress in solid state chemistry, vol 5. Pergamon Press, Oxford, p 149
Dimitrijevic NM, Savic D, Micic OI, Nozik AJ (1984). J Phys Chem 88:4278
Cherepy NJ, Liston DB, Lovejoy JA, Deng HM, Zhang JZ (1998). J Phys Chem B 102:770
Rosso KM, Dupuis M (2004). J Chem Phys 120:7050
Sherman DM (1987). Phys Chem Miner 14:355
Franck J (1925). Trans Faraday Soc 21:536
Condon EU (1928). Phys Rev 32:858
Sutin N (1986) In: Zuckermann JJ (ed) Electron transfer and electochemical reactions; photochemical and other energized reactions, vol 15. VCH, New York, p 16
Newton MD, Sutin N (1984). Ann Rev Phys Chem 35:437
Landau L (1932). Phys Z Sowjet 1:89
Zener C (1932). Proc Roy Soc A137:696
Brunschwig BS, Logan J, Newton MD, Sutin N (1980). J Am Chem Soc 102:5798
Marcus RA, Sutin N (1985). Biochim Biophys Acta 811:265
Iordanova N, Dupuis M, Rosso KM (2005). J Chem Phys 122:144305
Nelsen SF, Blackstock SC, Kim Y (1987). J Am Chem Soc 109:677
Klimkans A, Larsson S (1994). Chem Phys 189:25
Rosso KM, Rustad JR (2000). J Phys Chem A 104:6718
Rosso KM, Morgan JJ (2002). Geochim Cosmochim Acta 66:4223
Zhang XD, Wang YN, Guo JX, Zhang QY (1999). J Photochem Photobiol A Chem 121:1
Kuharski RA, Bader JS, Chandler D, Sprik M, Klein ML, Impey RW (1988). J Chem Phys 89:3248
Rustad JR, Rosso KM, Felmy AR (2004). J Chem Phys 120:7607
Ando K (2001). J Chem Phys 115:5228
Vener MV, Leontyev IV, Basilevsky MV (2003). J Chem Phys 119:8038
Brunschwig BS, Ehrenson S, Sutin N (1986). J Phys Chem 90:3657
German ED, Kuznetsov AM (1981). Electrochim Acta 26:1595
Leontyev IV (2004). Theor Chem Acc 111:110
Farazdel A, Dupuis M, Clementi E, Aviram A (1990). J Am Chem Soc 112:4206
Amini A, Harriman A (2003). J Photochem Photobiol C 4:155
Cave RJ, Newton MD (1996). Chem Phys Lett 249:15
King HF, Stanton RE, Kim H, Wyatt RE, Parr RG (1967). J Chem Phys 47:1936
Dupuis M, Rys J, King HF (1976). J Chem Phys 65:111
Dupuis M (2001). Comp Phys Comm 134:150
Apra E, Bylaska EJ, de Jong W, Hackler MT, Hirata S, Pollack L, Smith DMA, Straatsma TP, Windus TL, Harrison RJ, Nieplocha J, Tipparaju V, Kumar M, Brown E, Cisneros G, Dupuis M, Fann GI, Fruchtl H, Garza J, Hirao K, Kendall R, Nichols JA, Tsemekhman K, Valiev M, Wolinski K, Anchell J, Bernholdt D, Borowski P, Clark T, Clerc D, Dachsel H, Deegan M, Dyall K, Elwood D, Glendening E, Gutowski M, Hess A, Jaffe J, Johnson B, Ju J, Kobayashi H, Kutteh R, Lin Z, Littlefield R, Long X, Meng B, Nakajima T, Niu S, Rosing M, Sandrone G, Stave M, Taylor H, Thomas G, van Lenthe J, Wong A, Zhang Z (2003) NWChem: a computational chemistry package designed to run on high-performance parallel supercomputers, version 4.5 (Pacific Northwest National Laboratory)
Mulliken RS (1952). J Am Chem Soc 64:811
Newton MD (2003). Coord Chem Rev 238:167
Stumm W, Morgan JJ (1996). Aquatic chemistry. Wiley, New York
Haber F, Weiss J (1934). Proc Roy Soc London A147:332
Fallab S (1967). Angew Chem Int Ed 6:496
Creutz C, Sutin N (1986) In: Zuckermann JJ (ed) Electron-transfer and electochemical reactions; photochemical and other energized reactions, vol 15. VCH, New York, p 47
Rosso KM, Smith DMA, Dupuis M (2004). 108:5242
Rosso KM, Rustad JR, Gibbs GV (2002). J Phys Chem A 106:8133
Martin RL, Hay PJ, Pratt LR (1998). J Phys Chem A 102:3565
Sham TK, Hastings JB, Perlman ML (1981). Chem Phys Lett 83:391
Logan J, Newton MD (1983). J Chem Phys 78:4086
Tembe BL, Friedman HL, Newton MD (1982). J Chem Phys 76:1490
Newton MD (1988). J Phys Chem 92:3049
Ohta K, Morokuma K (1987). J Phys Chem 91:401
Bu YX, Liu CB (1999). J Mol Struct Theochem 490:7
Bu YX, Sun HT, Niu HB (1999). J Comp Chem 20:989
German ED, Kuznetsov AM, Efremenko I, Sheintuch M (1999). J Phys Chem A 103:10699
Lind J, Shen X, Merenyi G, Jonsson BO (1989). J Am Chem Soc 111:7654
Richens DT (1997) The chemistry of aqua ions. Wiley, New York
Luther GW III (1990) In: Stumm W (ed) Aquatic chemical kinetics. Wiley, New York City, p 173
Goddard WA, Olafson BD (1975). Proc Natl Acad Sci USA 72:2335
Olafson BD, Goddard WA (1977). Proc Natl Acad Sci USA 74:1315
Scherlis DA, Estrin DA (2002). Int J Quantum Chem 87:158
Nakau T (1960). J Phys Soc Jpn 15:727
Cox PA (1980). Chem Phys Lett 69:340
Tsuda N, Nasu K, Fujimori A, Siratori K (2000) Electronic conduction in oxides, vol 94. Springer, Berlin Heidelberg New York
van Daal HJ, Bosman AJ (1967). Phys Rev 158:736
Papaioannou JC, Patermarakis GS, Karayianni HS (2005). J Phys Chem Solids 66:839
Gleitzer C (ed) (1997) Electrical properties of oxide materials, vol 125–126. Trans Tech Publications, Switzerland, p 355
Bolhuis PG, Chandler D, Dellago C, Geissler PL (2002). Annu Rev Phys Chem 53:291
Fedurco M (2000). Coord Chem Rev 209:263
Gray HB, Winkler JR (2003) In: Kadish KM, Smith KM, Guilard R (eds) The Porphyrin Handbook, vol 11. Elsevier, p 51
Kuznetsov AM, Ulstrup J (2004). J Electroanal Chem 564:209
Smith DMA, Dupuis M, Vorpagel ER, Straatsma TP (2003). J Am Chem Soc 125:2711
Li J, Fisher CL, Chen JL, Bashford D, Noodleman L (1996). Inorg Chem 35:4694
Sham TK, Hastings JB, Perlman ML (1980). J Am Chem Soc 102:5904
Kanno H (1988). J Phys Chem 92:4232
Johnson DA, Nelson PG (1999). Inorg Chem 38:4949
Newton MD (1986). J Phys Chem 90:3734
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Rosso, K.M., Dupuis, M. Electron transfer in environmental systems: a frontier for theoretical chemistry. Theor Chem Acc 116, 124–136 (2006). https://doi.org/10.1007/s00214-005-0016-x
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s00214-005-0016-x