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FTIR, XRD, and XPS analyses indicated that Pb2+ and Zn2+ were absorbed on the biochars primarily via chemical complexation with aromatic functional groups. Quantum chemistry calculations confirmed that these functional groups (e.g., -OH and-COOH) tended to bind more strongly with Pb2+ than with Zn2+ due to the former's lower binding energies, which also accounted for the notable decrease in adsorption of Zn2+ in the presence of Pb2+. In addition, compared to carboxyl groups, hydroxyl groups had smaller binding energies and stronger metal