Abstract
A formulation based on defect-generated dissolution stepwaves of the variation of dissolution rate with the degree of undersaturation is validated by near-atomic-scale observations of surfaces, Monte Carlo simulations, and experimental bulk dissolution rates. The dissolution stepwaves emanating from etch pits provide a train of steps similar to those of a spiral but with different behavior. Their role in accounting for the bulk dissolution rate of crystals provides a conceptual framework for mineral dissolution far from equilibrium. Furthermore, the law extends research to conditions closer to equilibrium and predicts a nonlinear decrease in the rate of dissolution as equilibrium is approached, which has implications for understanding artificial and natural processes involving solid-fluid reactions.
References
47
Referenced
404
- Y. Satio Statistical Physics of Crystal Growth (World Scientific Singapore 1998).
-
A. C. Lasaga Kinetic Theory in the Earth Sciences (Princeton Univ. Press Princeton NJ 1998).
(
10.1515/9781400864874
) -
Hillner P. E., Gratz A. J., Manne F., Hansma P. K., Geology 20, 359 (1992).
(
10.1130/0091-7613(1992)020<0359:ASIOCG>2.3.CO;2
) / Geology by Hillner P. E. (1992) -
Gratz A. J., Bird P., Geochim. Cosmochim. Acta 57, 965 (1993).
(
10.1016/0016-7037(93)90033-S
) / Geochim. Cosmochim. Acta by Gratz A. J. (1993) -
Bosbach D., Rammensee W., Geochim. Cosmochim. Acta 58, 843 (1994).
(
10.1016/0016-7037(94)90509-6
) / Geochim. Cosmochim. Acta by Bosbach D. (1994) -
Dove P. M., Hochella M. F., Geochim. Cosmochim. Acta 57, 705 (1993).
(
10.1016/0016-7037(93)90381-6
) / Geochim. Cosmochim. Acta by Dove P. M. (1993) -
Dove P. M., Platt F. M., Chem. Geol. 127, 331 (1996).
(
10.1016/0009-2541(95)00127-1
) / Chem. Geol. by Dove P. M. (1996) -
A. F. White S. L. Brantley Eds. Chemical Weathering Rates of Silicate Minerals vol. 31 of Reviews in Mineralogy (Mineral Society of America Washington DC 1995).
(
10.1515/9781501509650
) 10.1016/0016-7037(84)90294-1
-
Berner R. A., Schott J., Am. J. Sci. 282, 1214 (1982).
(
10.2475/ajs.282.8.1214
) / Am. J. Sci. by Berner R. A. (1982) - A. F. White in (8) pp. 407–462.
-
Rufe E., Hochella M. F., Science 285, 874 (1999).
(
10.1126/science.285.5429.874
) / Science by Rufe E. (1999) -
MacInnis I. N., Brantley S. L., Geochim. Cosmochim. Acta 56, 1113 (1992).
(
10.1016/0016-7037(92)90049-O
) / Geochim. Cosmochim. Acta by MacInnis I. N. (1992) 10.1016/S0016-7037(96)00337-7
-
Jordan G., et al., Geochim. Cosmochim. Acta 63, 3183 (1999).
(
10.1016/S0016-7037(99)00225-2
) / Geochim. Cosmochim. Acta by Jordan G. (1999) -
McCoy J. M., LaFemina J. P., Surf. Sci. 373, 288 (1997).
(
10.1016/S0039-6028(96)01156-9
) / Surf. Sci. by McCoy J. M. (1997) -
Gratz A. J., Bird P., Quiro G. B., Geochim. Cosmochim. Acta 54, 2911 (1990).
(
10.1016/0016-7037(90)90109-X
) / Geochim. Cosmochim. Acta by Gratz A. J. (1990) -
Jordan G., Rammensee W., Geochim. Cosmochim. Acta 62, 941 (1998).
(
10.1016/S0016-7037(98)00030-1
) / Geochim. Cosmochim. Acta by Jordan G. (1998) 10.1016/0016-7037(94)90176-7
-
Luttge A., Bolton E. W., Lasaga A. C., Am. J. Sci. 299, 652 (1999).
(
10.2475/ajs.299.7-9.652
) / Am. J. Sci. by Luttge A. (1999) - A. Luttge U. Winkler A. C. Lasaga in preparation.
-
Cabrera N., Levine M. M., Philos. Mag. 1, 480 (1956).
(
10.1080/14786435608238124
) / Philos. Mag. by Cabrera N. (1956) -
Frank F. C., Acta Crystallogr. 4, 497 (1951).
(
10.1107/S0365110X51001690
) / Acta Crystallogr. by Frank F. C. (1951) -
Cabrera N., Levine M. M., Plaskett J. S., Phys. Rev. 96, 1153 (1954).
(
10.1103/PhysRev.96.1153
) / Phys. Rev. by Cabrera N. (1954) - A. C. Lasaga in Extended Abstracts Fourth International Symposium on Water-Rock Interactions (Univ. of Okiyama Press Okiyama Japan 1983) pp. 269–274.
-
___, Blum A. E., Geochim. Cosmochim. Acta 50, 2363 (1986).
(
10.1016/0016-7037(86)90088-8
) / Geochim. Cosmochim. Acta by ___ (1986) -
Brantley S. L., Crane S. R., Crerar D. A., Hellmann R., Stallard R., Geochim. Cosmochim. Acta 50, 2349 (1986).
(
10.1016/0016-7037(86)90087-6
) / Geochim. Cosmochim. Acta by Brantley S. L. (1986) -
Gilmer G. H., J. Cryst. Growth 35, 15 (1976).
(
10.1016/0022-0248(76)90209-8
) / J. Cryst. Growth by Gilmer G. H. (1976) -
___, Science 208, 355 (1980).
(
10.1126/science.208.4442.355
) / Science by ___ (1980) - A. E. Blum A. C. Lasaga in Aquatic Surface Chemistry W. Stumm Ed. (Wiley New York 1987) pp. 255–292.
10.1016/0016-7037(88)90224-4
-
Cygan R. T., et al., Chem. Geol. 78, 229 (1989).
(
10.1016/0009-2541(89)90060-0
) / Chem. Geol. by Cygan R. T. (1989) -
Schott J., et al., Geochim. Cosmochim. Acta 53, 373 (1989).
(
10.1016/0016-7037(89)90389-X
) / Geochim. Cosmochim. Acta by Schott J. (1989) -
Blum A. E., Yund R. A., Lasaga A. C., Geochim. Cosmochim. Acta 54, 283 (1990).
(
10.1016/0016-7037(90)90318-F
) / Geochim. Cosmochim. Acta by Blum A. E. (1990) -
Heinisch H. L., Sines G., Goodman J. W., Kirby S. H., J. Geophys. Res. 80, 1885 (1975).
(
10.1029/JB080i014p01885
) / J. Geophys. Res. by Heinisch H. L. (1975) -
Van der Hoek B., Van der Eerden J. R., Bennema P., J. Cryst. Growth 56, 621 (1982).
(
10.1016/0022-0248(82)90045-8
) / J. Cryst. Growth by Van der Hoek B. (1982) -
Lasaga A. C., Soler J. M., Ganor J., Burch T. E., Nagy K. L., Geochim. Cosmochim. Acta 58, 2361 (1994).
(
10.1016/0016-7037(94)90016-7
) / Geochim. Cosmochim. Acta by Lasaga A. C. (1994) -
Nagy K. L., Lasaga A. C., Geochim. Cosmochim. Acta 56, 3093 (1992).
(
10.1016/0016-7037(92)90291-P
) / Geochim. Cosmochim. Acta by Nagy K. L. (1992) -
Mogollon J. L., Ganor J., Soler J. M., Lasaga A. C., Am. J. Sci. 296, 729 (1996).
(
10.2475/ajs.296.7.729
) / Am. J. Sci. by Mogollon J. L. (1996) -
Burch T. E., Nagy K. L., Lasaga A. C., Chem. Geol. 105, 137 (1993).
(
10.1016/0009-2541(93)90123-Z
) / Chem. Geol. by Burch T. E. (1993) -
Taylor A., Blum J. D., Lasaga A. C., Geochim. Cosmochim. Acta 64, 2389 (2000).
(
10.1016/S0016-7037(00)00361-6
) / Geochim. Cosmochim. Acta by Taylor A. (2000) -
Cama J., Ganor J., Ayora C., Lasaga A. C., Geochim. Cosmochim. Acta 64, 2701 (2000).
(
10.1016/S0016-7037(00)00378-1
) / Geochim. Cosmochim. Acta by Cama J. (2000) -
P. Ortoleva Geochemical Self-Organization (Oxford Univ. Press Oxford 1994).
(
10.1093/oso/9780195044768.001.0001
) - J. I. Drever D. W. Clow in (8) pp. 463–483.
-
B. J. Wood J. V. Walther in Fluid-Rock Interactions During Metamorphism J. V. Walther B. J. Wood Eds. (Springer New York 1986) pp. 89–108.
(
10.1007/978-1-4612-4896-5_4
) 10.1126/science.288.5470.1411
- We thank R. S. Arvidson and A. Seilacher for thoughtful discussions and M. Hochella and anonymous reviewers for their helpful comments. We also gratefully acknowledge support for this study from the Department of Energy (grant DE-FG02-90ER14153) the NSF (grants EAR-9628238 and EAR-9526794) and the Alexander von Humboldt Foundation.
Dates
Type | When |
---|---|
Created | 23 years, 1 month ago (July 27, 2002, 5:52 a.m.) |
Deposited | 1 year, 7 months ago (Jan. 9, 2024, 4:38 p.m.) |
Indexed | 19 hours, 47 minutes ago (Aug. 31, 2025, 7:31 p.m.) |
Issued | 24 years, 5 months ago (March 23, 2001) |
Published | 24 years, 5 months ago (March 23, 2001) |
Published Print | 24 years, 5 months ago (March 23, 2001) |
@article{Lasaga_2001, title={Variation of Crystal Dissolution Rate Based on a Dissolution Stepwave Model}, volume={291}, ISSN={1095-9203}, url={http://dx.doi.org/10.1126/science.1058173}, DOI={10.1126/science.1058173}, number={5512}, journal={Science}, publisher={American Association for the Advancement of Science (AAAS)}, author={Lasaga, Antonio C. and Luttge, Andreas}, year={2001}, month=mar, pages={2400–2404} }