Heterolytic H2 activation over platinum supported on oxygen-vacancy-rich CeO2 (Pt/CeO2-Vo) for efficient reductive amination of levulinic acid to pyrrolidones under ambient conditions

Weizhen Xie; Yining Zhang; Jiacheng Li; Yue Tang; Yaqi Shi; Lu Lin; Xing Tang

doi:10.1016/j.jobab.2026.100253

Volume 11 Issue 3

Jun. 2026

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Weizhen Xie, Yining Zhang, Jiacheng Li, Yue Tang, Yaqi Shi, Lu Lin, Xing Tang. Heterolytic H2 activation over platinum supported on oxygen-vacancy-rich CeO2 (Pt/CeO2-Vo) for efficient reductive amination of levulinic acid to pyrrolidones under ambient conditions[J]. Journal of Bioresources and Bioproducts, 2026, 11(3): 100253. doi: 10.1016/j.jobab.2026.100253

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Weizhen Xie, Yining Zhang, Jiacheng Li, Yue Tang, Yaqi Shi, Lu Lin, Xing Tang. Heterolytic H₂ activation over platinum supported on oxygen-vacancy-rich CeO₂ (Pt/CeO₂-V_o) for efficient reductive amination of levulinic acid to pyrrolidones under ambient conditions[J]. Journal of Bioresources and Bioproducts, 2026, 11(3): 100253. doi: 10.1016/j.jobab.2026.100253

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Heterolytic H₂ activation over platinum supported on oxygen-vacancy-rich CeO₂ (Pt/CeO₂-V_o) for efficient reductive amination of levulinic acid to pyrrolidones under ambient conditions

doi: 10.1016/j.jobab.2026.100253

Xiamen Key Laboratory of Clean and High-Valued Applications for Biomass, Fujian Engineering and Research Center of Clean and High-Valued Technologies for Biomass, College of Energy, Xiamen University, Xiamen 361102, China

Funds:

This work was supported by National Natural Science Foundation of China (No. U22A20421

No. 22378338), the Project for Science and Technology Plan of Fujian Province of China (No. 2024H4007).

Received Date: 2025-12-16
Accepted Date: 2026-03-20
Rev Recd Date: 2026-03-12

Available Online: 2026-07-04

Publish Date: 2026-06-01

Abstract

Abstract

Reductive amination of biomass-derived levulinic acid (LA) to N-substituted-5-methyl-2-pyrrolidone (BMP), versatile nitrogen-containing chemicals, under ambient conditions is highly desirable but challenging due to inefficient H₂ activation. To address this limitation, a platinum (Pt)-based catalyst supported on oxygen-vacancy-rich CeO₂ (Pt/CeO₂-V_o) was developed, comprising uniformly dispersed Pt/PtO₂ heterostructures with adjacent Pt-O-Ce interfacial sites. At these Pt-O-Ce interfaces, electron-deficient Pt and electron-rich O atoms, modulated by neighboring oxygen vacancies, facilitate in situ hydrogen spillover from Pt nanoparticles, generating highly reactive H^δ⁺-O…Pt-H^δ^- pairs that enable the efficient hydrogenation of the condensation intermediates formed between LA and amine substrates. Therefore, Pt/CeO₂-V_o achieved a high BMP yield of 95.2% with a productivity of 476.0 mol/(mol·h) within 1 h under ambient conditions. Even at a high LA concentration of 11.4% (w), the yield remained above 90%, demonstrating the catalyst’s efficiency under ambient conditions. It also showed excellent recyclability over six consecutive cycles and maintained stable performance for over 80 h in a fixed-bed flow reactor. This work underscores the critical importance of interfacial engineering in optimizing Pt-based catalysts and provides a robust and sustainable strategy for biomass upgrading under mild conditions.
- Levulinic acid,
- N-substituted-5-methyl-2-pyrrolidone,
- Oxygen vacancy,
- Reductive amination,
- Ambient condition

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References(56)

References

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