Journal
NEW JOURNAL OF CHEMISTRY
Volume 46, Issue 47, Pages 22672-22685Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2nj03482d
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Funding
- National Natural Science Foundation of China
- high-level talent program of the University Reform and Development Fund from the Central Government
- [22278068]
- [2020GSP17]
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By studying catalysts with different P/Ni ratios, the mechanism of P in hydrodeoxygenation reaction was revealed. P promotes the formation of smaller active sites and increases the acidity of acid sites. The selectivity of products can be optimized by adjusting the P content in Ni-P catalysts, leading to efficient hydrodeoxygenation catalysis.
To deeply understand the role of P in hydrodeoxygenation (HDO), SiO2-supported Ni and Ni-P catalysts with different P/Ni ratios (x) were prepared. The as-prepared samples were characterized by various characterization methods. The HDO activity and product distribution over the Ni/SiO2 and N-P/SiO2-x were compared and the effects of x on the structure, acidity, formation mechanism of active phases and HDO performance were studied taking m-cresol HDO as a model reaction. The results showed that the introduction of P promotes the formation of smaller active sites and contributes to the creation of weak and medium strength acid sites through the formation of P-OH groups and Ni delta+ in Ni2P. HDO over the Ni/SiO2 catalyst occurs mainly via the hydrogenation (HYD) route with 3-methyl-cyclohexanol (3-MCHnol) as the main product. However, for Ni-P/SiO2-x catalysts, methyl-cyclohexane (MCH) selectivity increases first and then decreases with the increase of x, reaching a maximum of 95% at x = 1. The acidity generated by the introduction of P contributes to increased MCH selectivity, while the dehydration of 3-MCHnol to MCH occurs mainly on acid sites. However, the excessively high P content (x >= 2.0) leads to a significant increase of MB (toluene) selectivity, which is associated with the increase in Ni(i) sites. About 100% m-cresol conversion was achieved with Ni-P/SiO2-1.0 when the m-cresol (g)/catalyst (g) ratio was 3, with MCH (99.4%) as the major product, showing great promise for deep HDO catalysis.
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