Enhancing hydrogen activation and transfer is crucial for efficiently producing light aromatic hydrocarbons (LAH) during the upgrading of lignite pyrolysis volatiles. This study established a synergistic catalytic system combining Cu⁺ and Brønsted acid sites to enhance active hydrogen transfer efficiency. Three Cu-modified sheet-like ZSM-5 zeolites were synthesized via impregnation (Cu/HZ5-S), in-situ doping (Cu@HZ5-S), and coordination-assisted deposition (Cu-PA/HZ5-S), respectively. Characterizations demonstrated that Cu dispersion significantly affected Cu-zeolite interactions. Cu-PA/HZ5-S, with optimal Cu dispersion, exhibited superior specific surface area (337 m²·g^-1), pore structure (0.187 cm³·g^-1), and active site exposure. Its intimate Cu-zeolite interaction increased total acid content (from 347.02 and 684.76 to 756.73 mmol·g^-1) and Brønsted acid content (from 162.75 and 316.36 to 497.93 mmol·g^-1) compared to Cu@ZH5-S and Cu/ZH5-S, respectively. The optimized spatially isolated distribution of Cu components within zeolite increased Cu⁺ dispersity, enhancing the synergy via Cu⁺/Brønsted acid combined sites. Cu-PA/HZ5-S achieved the highest LAH yield (70.70 mg·g^-1), surpassing HZ5-S (40.02 mg·g^-1), Cu/HZ5-S (51.63 mg·g^-1), and Cu@HZ5-S (41.89 mg·g^-1). Compared to unmodified ZSM-5, Cu-PA/HZ5-S achieved increased relative content of aromatics by 9.41% and decreased relative content of oxygen-containing compounds by 6.72% in the liquid products. Furthermore, spent Cu-PA/HZ5-S showed the lowest hard coke ratio (52.25 wt.%), lower than HZ5-S (68.55 wt.%), Cu/HZ5-S (67.39 wt.%), and Cu@HZ5-S (63.38 wt.%), mitigating aromatic deposition and improving reusability. Cu+ sites primarily activated, adsorbed initial volatiles, and promoted C-O/C-C cleavage. Brønsted acid sites mediated protonation for LAH formation. The combined and accessible Cu⁺/Brønsted acid sites enhanced active hydrogen transfer, demonstrating significant potential for improving LAH yields from lignite pyrolysis volatiles.
 

sheet-like ZSM-5; active sites; active hydrogen transfer; Brønsted acid sites; catalytic pyrolysis