Journal
CHEMICAL ENGINEERING JOURNAL
Volume 438, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.135577
Keywords
Phenolics; Hydrodeoxygenation; Arenes; MeOH; Competitive adsorption; MoOx/BaO@SBA-15
Categories
Funding
- National Key R&D Program of China [2019YFD1100602]
- National Natural Science Foundation of China [21978158, 22173105]
- Natural Science Foundation of Shandong province [ZR2020QB051, ZR2020QB052]
Ask authors/readers for more resources
Hydrodeoxygenation (HDO) is an effective strategy to upgrade lignin-derived bio-oils into high value-added chemicals such as arenes. However, the challenge lies in selective hydrogenolysis of oxygen-containing groups while keeping the unsaturated aromatic rings intact. In this study, a catalyst with rich oxygen defects was synthesized to induce nonplanar adsorption of phenolics, weakening the C-Ar-OR bonds and preventing excessive hydrogenation of aromatic rings. The addition of BaO coating promoted the adsorption of phenol and enhanced the one-step HDO of guaiacol into benzene and toluene.
The bio-oils derived from fast pyrolysis of lignin contain large amount of phenolic components. Owing to the high oxygen content, these bio-oils could not be used as traffic liquid fuels. Hydrodeoxygenation (HDO) was an effective strategy to upgrade these phenolics into high value-added chemicals such as arenes. However, the challenge of upgrading phenolics into arenes lies in selective hydrogenolysis of the oxygen-containing groups (e. g. -OCH3 and -OH) while keeping the unsaturated aromatic rings intact. However, the competitive adsorption behavior of produced intermediates likely inhibits the further HDO of phenol to arenes. In this work, MoOx/SBA-15 with rich oxygen defects was synthesized, which is capable of inducing phenolics adsorbed in a nonplanar manner, weakening the intensity of C-Ar-OR (R = CH3 or H) bonds and preventing the excessive hydrogenation of aromatic rings. In addition, BaO coating was decorated on MoOx/SBA-15 to tune the surface acid-base properties so as to promote the adsorption of phenol and consume MeOH via alkylation reaction with phenol, enhancing guaiacol one-step HDO into benzene and toluene. Based on catalyst evaluation and characterization as well as density functional theory (DFT) calculations, the catalytic mechanism of phenolics HDO reaction over MoOx/ BaO@SBA-15 was analyzed and discussed. Current work helps not only gain deep insights into the competitive interaction for mixed phenolics HDO reaction, but also shed light on the design and synthesis of high-efficient HDO catalysts for upgrading crude bio-oils into arenes.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available