Data from the large and diverse Adirondack Lake Survey were used to calibrate four simple organic acid analog models in an effort to quantify the influence of naturally occurring organic acids on lake waterpH and acid‐neutralizing capacity (ANC). The organic acid analog models were calibrated to observations ofpH, dissolved organic carbon (DOC), and organic anion (An−) concentrations from a reduced data set representing 1128 individual lake samples, expressed as 41 observations of meanpH, in intervals of 0.1pH units frompH 3.9 to 7.0. Of the four organic analog approaches examined, including the Oliver et al. (1983) model, as well as monoprotic, diprotic, and triprotic representations, the triprotic analog model yielded the best fit (r2= 0.92) to the observed data. Moreover, the triprotic model was qualitatively consistent with observed patterns of change in organic solute charge density as a function ofpH. A low calibrated value for the first H+dissociation constant (pKal= 2.62) and the observation that organic anion concentrations were significant even at very lowpH (<4) indicate that naturally occurring organic solutes in these waters have strongly acidic functional groups. Inclusion of organic acidity in model calculations resulted in good agreement between measured and predicted values of lake waterpH and ANC. Assessments to project the response of surface waters to future changes in atmospheric deposition, through the use of acidification models, will need to include representations of organic acids in model structure to make accurate predictions ofpH and
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