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Bench-scale studies were conducted to examine the effects of source water composition on the efficiency of arsenic removal by coagulation with ferric chloride and alum. Parameters examined included initial arsenic concentrations and oxidation state, pH and the presence of co-occurring inorganic solutes and natural organic matter. The results of laboratory experiments and predictions based on surface complexation modeling are compared to elucidate the mechanisms of arsenic removal and to identify factors controlling arsenic removal efficiencies.