Lignin, a key component of lignocellulosic biomass, offers significant potential as a renewable raw material for the sustainable production of aromatic chemicals. To investigate its heterogeneous catalytic depolymerization, benzyl phenyl ether (BPE) was used as a model compound. Hierarchical ZSM-5 catalysts were synthesized and modified with metal oxides (NiO and CuO). Belitung kaolin and Bayat natural zeolite, natural minerals from Indonesia, were used as silica and alumina sources to synthesize hierarchical ZSM-5 zeolite (labeled as ZSM-5N), which was compared with hierarchical ZSM-5 synthesized using pro-analysis precursors (labeled as ZSM-5S). Comprehensive physicochemical characterization using FTIR, XRD, BET, XRF, SEM-EDX, and NH₃-TPD confirmed the formation of the catalysts. Lignin was isolated from Swietenia Mahagoni L. Jacq. wood waste as a biomass source (61.07% extracted lignin). The NiO/ZSM-5 and CuO/ZSM-5 catalysts offered bifunctional acid–redox-active sites. NiO enhanced BPE conversion and phenol production, whereas CuO favored vanillin formation under milder reaction conditions. Among the modified catalysts, NiO/ZSM-5N achieved the highest BPE conversion (90.11%), yielding 23.25% phenol as the major identified product, comparable to NiO/ZSM-5S (90.13% conversion and 25.14% phenol yield). For isolated lignin, NiO/ZSM-5 favored phenol production at 250 °C, whereas CuO/ZSM-5 promoted vanillin formation under milder conditions (200 °C). These findings demonstrate the feasibility and novelty of utilizing Indonesian natural minerals for the synthesis of hierarchical ZSM-5 catalysts and provide new insights into the effects of NiO and CuO modifications on the conversion of BPE and lignin to phenolic compounds.
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