Han Xinlei, Zhou Yuchen, Chen Shuangmei, Chen Huanhao, Zhang Jiuxuan, Qu Zhengyan, Zeng Feng, Ji Tuo, Jiang Hong, Cao Wei, Tang Zhenchen, Chen Rizhi
State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, Jiangsu, 211816, China.
Angew Chem Int Ed Engl. 2025 Jul;64(27):e202505518. doi: 10.1002/anie.202505518. Epub 2025 May 9.
Efficient upcycling of polyolefin waste into liquid fuels remains challenging due to over-cracking and the lack of sufficient acidity in non-zeolitic catalysts. Here, we report a Ni/niobium oxide nanorod (Ni/NbO) catalyst that achieves 95% selectivity to C alkanes at full polyethylene (PE) conversion under mild conditions (240 °C), with minimal gaseous products (4%). The catalyst reaches a high liquid fuel formation rate of 1274 g g h, rivaling noble metal systems. Its performance is governed by the morphology and crystallinity of NbO nanorods, which provide sufficient acidity without micropore confinement, mitigating diffusion limitations and over-cracking. Detailed operando infrared spectroscopy and computational studies reveal, for the first time, that Brønsted acid sites, generated in situ via hydrogen spillover on the (110) facet, are the key catalytic sites in niobium oxide-based catalysts. The density of these acid sites exhibits a linear correlation with hydrocracking activity. The catalyst also demonstrates high efficiency across diverse polyolefin feedstocks and excellent reusability, offering a scalable and cost-effective solution for plastic upcycling.
由于过度裂解以及非沸石催化剂缺乏足够的酸度，将聚烯烃废料高效升级转化为液体燃料仍然具有挑战性。在此，我们报道了一种镍/氧化铌纳米棒（Ni/NbO）催化剂，该催化剂在温和条件（240°C）下实现了全聚乙烯（PE）转化时对C烷烃95%的选择性，气态产物最少（4%）。该催化剂的液体燃料生成速率高达1274 g g h，可与贵金属体系相媲美。其性能受NbO纳米棒的形态和结晶度控制，NbO纳米棒提供了足够的酸度而没有微孔限制，减轻了扩散限制和过度裂解。详细的原位红外光谱和计算研究首次揭示，通过氢溢流在（110）晶面上原位生成的布朗斯台德酸位点是氧化铌基催化剂中的关键催化位点。这些酸位点的密度与加氢裂化活性呈线性相关。该催化剂还在多种聚烯烃原料上表现出高效率和出色的可重复使用性，为塑料升级循环提供了一种可扩展且经济高效的解决方案。
