Electronic Configuration‐Modulated Dual‐Active Nanocomposite NiAlO_x for Promoting Plastic‐To‐Green Hydrogen

Abstract Chemical upcycling of plastic waste to produce green H₂ has emerged as a promising avenue. Highly efficient and robust NiAlO_x catalysts with dual active nanocomposite (NiO‐NiAl₂O₄) through a facile electronic configuration modulation strategy are synthesized for the decomposition‐catalytic steam reforming (DCSR) of plastic wastes for enhancing H₂ production while alleviating carbon deposition. Of these dual‐active nanocomposite catalysts, NiAlO_x‐800 presents the highest proportions of Ni²⁺ cations and oxygen vacancies, contributing to the enhance structural stability and catalytic activity. NiAlO_x‐800 subjected to the DCSR process achieves the highest gas yield (244.42 mmol g_plastic⁻¹) with an extremely high H₂ proportion of 70.14 vol%, due to its superior catalytic cracking and reforming ability. Furthermore, a high carbon conversion efficiency (≈100%) is achieved, suggesting that the C content in plastic is completely transformed into gases. More importantly, the catalyst's robustness and stability are evaluated in the time course study, where it maintains an exceptionally high gas yield (252.23 mmol g_plastic⁻¹) with 71.52 vol% of H₂ after 200 min. In situ DRIFTS characterization is also performed to unravel the reaction mechanisms. Thus, this work innovatively explores a new strategy for developing an electronic configuration‐modulated nanocomposite catalyst for upcycling waste plastics into highly pure green H₂.