Highly efficient conversion of glycerol to lactic acid over CeCuOx@C catalysts derived from Ce-Cu-benzenetricarboxylate
摘要
A series of CeCuOx@C catalysts with different Ce contents was prepared from Ce-Cu-BTC precursors by hydrothermal synthesis followed by pyrolysis under an N2 atmosphere. The influence of Ce incorporation on the phase composition, textural properties, surface redox states, and catalytic behavior in glycerol conversion to lactic acid was systematically investigated. XRD results confirmed the coexistence of metallic Cu and Cu2O phases, while XPS analysis revealed Cu0/Cu+ and Ce3+/Ce4+ redox pairs together with oxygen-vacancy-related surface oxygen species. Among the catalysts studied, 5%CeCuOx@C exhibited the largest specific surface area, 106 m2 g−1, and the most favorable Cu-Ce interfacial structure. Under an air atmosphere at 190 °C for 6 h, this catalyst achieved complete glycerol conversion and 90.56% lactic acid selectivity. The enhanced selectivity was associated with the balanced distribution of Cu0/Cu+ and Ce3+/Ce4+ species, which promoted glycerol activation, oxygen-vacancy formation, and the selective transformation of reaction intermediates toward lactic acid. The 5%CeCuOx@C catalyst also showed good reusability over six consecutive cycles, with glycerol conversion remaining at 99.31% and lactic acid selectivity above 85% in the sixth run. These results demonstrate that controlled Ce incorporation is effective for regulating Cu-Ce interfacial redox properties and improving lactic acid formation over MOF-derived non-noble-metal catalysts.