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Adsorption is a widely used method for pollution removal and for the recovery of valuable species. In recent years, the use of metal–organic compounds among the adsorbents used in adsorption studies has increased. In this study, the performance of the water-insoluble Fe complex as a metal organic framework (MOF-Fe-Ta) of water-soluble tannic acid, which is not used as an adsorbent in uranium recovery and removal, was investigated. For the characterization of the new synthesized material, Fourier transform infrared, scanning electron microscopy, and X-ray diffraction analyses were performed. The changes in the adsorption process based on various parameters were investigated and discussed. The point of zero charges value of the adsorbent was found as 5.52. It was noticed that the adsorption increases as the pH increases. Analyzing the effect of concentration on adsorption, we determined which model explained the adsorption better. The monolayer capacity of the adsorbent determined in light of the Langmuir model was reported as 0.347 mol kg –1 . The Freundlich constant, namely the β value obtained in the Freundlich model, which is a measure of surface heterogeneity, was found to be 0.434, and the E DR value, which was found from the Dubinin–Raduskevich model and accepted as a measure of adsorption energy, was 10.3 kJ mol –1 . The adsorption was kinetically explained by the pseudo-second-order model and the adsorption rate constant was reported as 0.15 mol –1 kg min –1 . The effect of temperature on adsorption was studied; it was emphasized that adsorption was energy consuming, that is, endothermic and Δ H was found as 7.56 kJ mol –1 . The entropy of adsorption was positive as 69.3 J mol –1 K –1 . As expected, the Gibbs energy of adsorption was negative (−13.1 kJ mol –1 at 25 °C), so adsorption was considered as a spontaneous process. Additionally, the power and mechanism of the interaction between studied adsorbent and adsorbate are explained through density functional theory computations. Computationally obtained data supported the experimental studies.

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