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Hertkorn, N. ; Perdue, E.M.* ; Kettrup, A.

A potentiometric and 113Cd NMR study of cadmium complexation by natural organic matter at two different magnetic field strengths.

Anal. Chem. 76, 6327-6341 (2004)

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Open Access Green as soon as Postprint is submitted to ZB.

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The binding of cadmium to Suwannee River natural organic matter (NOM) has been investigated across a broad range of Cd/C ratios (0.00056−0.0056) and pH values (3.5−11) by ¹¹³Cd NMR spectroscopy at two magnetic field strengths (B₀ = 9.4 and 11.7 T). Caused by the very peculiar and highly complex nature of the Cd−NOM exchanging system, these ¹¹³Cd NMR spectra are characterized by a pH- and concentration-dependent superposition of slow, intermediate, and fast chemical exchange. The complex interplay of solution chemistry and chemical exchange requires a thorough mapping of this Cd−NOM chemically exchanging system through NMR acquisition at two magnetic field strengths and a systematic variation of Cd/C ratios and pH values. The interpretation of ¹¹³Cd NMR spectra is greatly facilitated and constrained by simultaneous measurements of pH and pCd, which allows a model-independent calculation of organically bound Cd²⁺ under all experimental conditions. Within the range of chemical conditions applied in this study, ¹¹³Cd NMR spectrometric evidence is consistent with coordination of cadmium by oxygen, nitrogen, and sulfur ligands in NOM. Under all experimental conditions, cadmium is primarily coordinated to oxygen; however, several lines of evidence point to the participation of nitrogen ligands, even in acidic solutions where nitrogen ligands are primarily bound to protons. Under alkaline conditions, up to one-third of cadmium may be coordinated to nitrogen, and a small, but unquantifiable, percentage of cadmium is coordinated to sulfur ligands, as evidenced by far-low-field ¹¹³Cd NMR resonances.

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