TY - JOUR
T1 - Hydrogen Spillover-Induced Brønsted Acidity Enables Controllable Hydrocracking of Polyolefin Waste to Liquid Fuels
AU - Han, Xinlei
AU - Zhou, Yuchen
AU - Chen, Shuangmei
AU - Chen, Huanhao
AU - Zhang, Jiuxuan
AU - Qu, Zhengyan
AU - Zeng, Feng
AU - Ji, Tuo
AU - Jiang, Hong
AU - Cao, Wei
AU - Tang, Zhenchen
AU - Chen, Rizhi
N1 - Publisher Copyright:
© 2025 Wiley-VCH GmbH.
PY - 2025
Y1 - 2025
N2 - 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/NbOx) catalyst that achieves 95% selectivity to C5–20 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 gliquid gNi−1 h−1, rivaling noble metal systems. Its performance is governed by the morphology and crystallinity of NbOx 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.
AB - 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/NbOx) catalyst that achieves 95% selectivity to C5–20 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 gliquid gNi−1 h−1, rivaling noble metal systems. Its performance is governed by the morphology and crystallinity of NbOx 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.
KW - Brønsted acidity
KW - Heterogeneous catalysis
KW - Hydrogen spillover
KW - Niobium oxide
KW - Polyolefin upcycling
UR - http://www.scopus.com/inward/record.url?scp=105004678228&partnerID=8YFLogxK
U2 - 10.1002/anie.202505518
DO - 10.1002/anie.202505518
M3 - 文章
AN - SCOPUS:105004678228
SN - 1433-7851
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
ER -