Reclamation of spent catalysts for the efficient recovery of palladium (Pd) is gaining growing attention due to its scarcity and high supply risk. Currently Pd extraction from spent catalysts through an efficient, economical, and green method has remained a challenge. In this study, Fe3+ is utilized for leaching through oxidation of Pd in a mild condition. Before leaching, distillation was proposed to remove and recover the organics from spent catalysts. The effects of HCl concentration, Fe3+ concentration, NaCl concentration, leaching time, and temperature on the leaching efficiency of Pd were investigated to determine the optimum leaching conditions. The results show that Pd extraction and dissolution of Al2O3 increase with higher HCl concentration. The effect of NaCl on Pd leaching efficiency is significant at low acid concentration (2.0 mol/L HCl). The leaching efficiency was 99.5% for Pd under the following conditions: 2.0 mol/L HCl, 4.0 mol/L NaCl, and 0.67 mol/L Fe3+ at 80 °C for 90 min. The leaching kinetics fits best to the shrinking-core model of surface chemical reaction. The activation energy for the leaching of Pd was 47.6 kJ/mol. PdCl42− was selectively adsorbed by anion exchange resin. The filtrate containing adequate H+, Cl-, and Fe3+ was reused as leaching agent. Pd leaching efficiency was over 96% after five cycle times. This study provides an efficient process for recovery of Pd from spent catalysts.
The global yield of platinum (Pt) recovery from spent catalysts is about 30%. Pt recovery from spent catalysts is one of the most significant methods to reduce its supply risk and meet future demand. The current hydro-leaching processes always involve extremely high acidity (c(H+) > 6.0 mol/L), causing serious environmental issues and consuming large amounts of reagents. This paper studied the recovery of Pt from spent petroleum catalysts in a mild leaching solution (c(H+) = 1.0−2.0 mol/L). The HCl and NaCl were used as leaching agents, while H2O2 was used for oxidation of Pt. The leaching factors, including solid/liquid ratio (S/L), acidity, leaching temperature, and H2O2 usage, were studied. The leaching efficiency of Pt was 95.7% under the conditions of S/L of 1:5 g/mL, HCl of 1.0 mol/L, NaCl of 5.0 mol/L, 10% H2O2/spent catalysts of 0.6 mL/g, and temperature of 90 °C for 2 h. The leaching kinetic of platinum fits best to the Avrami equation. The apparent activation energy for leaching platinum was 114.9 kJ/mol. Furthermore, the effects of the operating variables were assessed and optimized by employing a response surface methodology based on Box-Behnken Design. The result shows that HCl concentration had the greatest impact on the leaching efficiency as compared to the H2O2 concentration and S/L ratio. Pt leaching efficiency was increased to 98.1% at the optimized conditions of HCl of 1.45 mol/L, NaCl of 4.55 mol/L, 10% H2O2/spent catalysts of 0.66 mL/g, and S/L of 1:4.85. The purity of Pt is over 90% by the reduction of iron powder.
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