Energy & Environmental Materials >

2024 , Vol. 7 >Issue 3: 12638

DOI: https://doi.org/10.1002/eem2.12638

Selective Hydrodeoxygenation of Lignin-Derived Vanillin via Hetero-Structured High-Entropy Alloy/Oxide Catalysts

  • Yan Sun 1 ,
  • Kaili Liang 1 ,
  • Ren Tu 1 ,
  • Xudong Fan 1 ,
  • Charles Q. Jia 2 ,
  • Zhiwen Jia 1 ,
  • Yingnan Li 1 ,
  • Hui Yang 1 ,
  • Enchen Jiang 1 ,
  • Hanwen Liu 3 ,
  • Yonggang Yao , 3 ,
  • Xiwei Xu , 1
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  • 1. Key Laboratory for Biobased Materials and Energy of Ministry of Education, College of Materials and Energy, South China Agricultural University, Guangzhou 510640, China
  • 2. Department of Chemical Engineering and Applied Chemistry, University of Toronto, 200 College Street, Toronto ON M5S3E5, Canada
  • 3. State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
yaoyg@hust.edu.cn
xuxiwei200801@hotmail.com

Received date: 12 Nov 2022

Revised date: 09 Feb 2023

Copyright

2023 2023 The Authors. Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.
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Abstract

The chemoselective hydrodeoxygenation of natural lignocellulosic materials plays a crucial role in converting biomass into value-added chemicals. Yet their complex molecular structures often require multiple active sites synergy for effective activation and achieving high chemoselectivity. Herein, it is reported that a high-entropy alloy (HEA) on high-entropy oxide (HEO) hetero-structured catalyst for highly active, chemoselective, and robust vanillin hydrodeoxygenation. The heterogenous HEA/HEO catalysts were prepared by thermal reduction of senary HEOs (NiZnCuFeAlZrOx), where exsolvable metals (e.g., Ni, Zn, Cu) in situ emerged and formed randomly dispersed HEA nanoparticles anchoring on the HEO matrix. This catalyst exhibits excellent catalytic performance: 100% conversion of vanillin and 95% selectivity toward high-value 2-methyl-4 methoxy phenol at low temperature of 120 ℃, which were attributed to the synergistic effect among HEO matrix (with abundant oxygen vacancies), anchored HEA nanoparticles (having excellent hydrogenolysis capability), and their intimate hetero-interfaces (showing strong electron transferring effect). Therefore, our work reported the successful construction of HEA/HEO heterogeneous catalysts and their superior multifunctionality in biomass conversion, which could shed light on catalyst design for many important reactions that are complex and require multifunctional active sites.

Key words： biomass conversion; heterogeneous catalysts; high-entropy oxide; high-entropy alloys; lignin pyrolysis

Cite this article

Yan Sun , Kaili Liang , Ren Tu , Xudong Fan , Charles Q. Jia , Zhiwen Jia , Yingnan Li , Hui Yang , Enchen Jiang , Hanwen Liu , Yonggang Yao , Xiwei Xu . Selective Hydrodeoxygenation of Lignin-Derived Vanillin via Hetero-Structured High-Entropy Alloy/Oxide Catalysts[J]. Energy & Environmental Materials, 2024 , 7(3) : 12638 . DOI: 10.1002/eem2.12638

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