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The objective of this investigation was to develop a surface complexation modeling approach to account for proton and metal (Cd, Pb) binding onto many-layered graphene oxide (MLGO) across a range of pH and ionic strength conditions. MLGO particles exhibit large buffering capacities between pH 3 and pH 10 and the buffering behavior is only nominally influenced by ionic strength. In contrast, batch metal sorption experiments illustrate that the striking capacity of MLGO to sorb metals substantially diminishes with increases in ionic strength. X-ray absorption spectroscopy measurements were used to establish reaction stoichiometries and indicate that both Cd and Pb associate with single sites on the MLGO surface. The difference in sorption behaviors for protons and metals is best modeled using a 4-site non-electrostatic surface complexation model that accounts for ionic strength effects as a competition between Na from the background electrolyte and Cd/Pb for available MLGO sorption sites. Using this approach, titration data are used to constrain the site concentrations and p K a values for MLGO binding sites. The p K a values (±1 σ ) are calculated as 4.55 (±0.91), 6.52 (±0.49), 8.48 (±0.21), and 9.98 (±0.21). We then use these parameters and the metal sorption data to determine thermodynamic stability constants for each important Cd– and Pb–MLGO surface complex. The site concentrations and equilibrium constants provided herein are critical for developing and testing remediation strategies for specific water chemistries. [ABSTRACT FROM AUTHOR]