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Selective hydroconversion of coconut oil-derived lauric acid to alcohol and aliphatic alkane over MoO _x -modified Ru catalysts under mild conditions.

ABSTRACT: Molybdenum oxide-modified ruthenium on titanium oxide (Ru-(y)MoO _x /TiO₂; y is the loading amount of Mo) catalysts show high activity for the hydroconversion of carboxylic acids to the corresponding alcohols (fatty alcohols) and aliphatic alkanes (biofuels) in 2-propanol/water (4.0/1.0 v/v) solvent in a batch reactor under mild reaction conditions. Among the Ru-(y)MoO _x /TiO₂ catalysts tested, the Ru-(0.026)MoO _x /TiO₂ (Mo loading amount of 0.026 mmol g^-1) catalyst shows the highest yield of aliphatic n-alkanes from hydroconversion of coconut oil derived lauric acid and various aliphatic fatty acid C6-C18 precursors at 170-230 °C, 30-40 bar for 7-20 h. Over Ru-(0.026)MoO _x /TiO₂, as the best catalyst, the hydroconversion of lauric acid at lower reaction temperatures (130 ≥ T ≤ 150 °C) produced dodecane-1-ol and dodecyl dodecanoate as the result of further esterification of lauric acid and the corresponding alcohols. An increase in reaction temperature up to 230 °C significantly enhanced the degree of hydrodeoxygenation of lauric acid and produced n-dodecane with maximum yield (up to 80%) at 230 °C, H₂ 40 bar for 7 h. Notably, the reusability of the Ru-(0.026)MoO _x /TiO₂ catalyst is slightly limited by the aggregation of Ru nanoparticles and the collapse of the catalyst structure.

SUBMITTER: Rodiansono

PROVIDER: S-EPMC9062712 | biostudies-literature | 2022 Apr

REPOSITORIES: biostudies-literature

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Selective hydroconversion of coconut oil-derived lauric acid to alcohol and aliphatic alkane over MoO x -modified Ru catalysts under mild conditions.

Rodiansono Dewi Heny Puspita HP Mustikasari Kamilia K Astuti Maria Dewi MD Husain Sadang S Sutomo

RSC advances 20220401 21

Molybdenum oxide-modified ruthenium on titanium oxide (Ru-(y)MoO x /TiO2; y is the loading amount of Mo) catalysts show high activity for the hydroconversion of carboxylic acids to the corresponding alcohols (fatty alcohols) and aliphatic alkanes (biofuels) in 2-propanol/water (4.0/1.0 v/v) solvent in a batch reactor under mild reaction conditions. Among the Ru-(y)MoO x /TiO2 catalysts tested, the Ru-(0.026)MoO < ...[more]

PMID: 35520112

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Project description:The preparation of zeolite-based bifunctional catalysts with low noble metal loadings while maintaining optimal performance has been studied. We have deposited 0.03 to 1.0 wt % Pt on zeolite H-USY (Si/Al ∼ 30 at./at.) using either platinum(II) tetraammine nitrate (PTA, Pt(NH3)4(NO3)2) or hexachloroplatinic(IV) acid (CPA, H2PtCl6·6H2O) and studied the nanoscale Pt loading heterogeneities and global hydroconversion performance of the resulting Pt/Y catalysts. Pt/Y samples prepared with PTA and a global Pt loading as low as 0.3 wt % Pt (n Pt/n A = 0.08 mol/mol, where nPt is the number of Pt surface sites and n A is the number of acid sites) maintained catalytic performance during n-heptane (T = 210-350 °C, P = 10 bar) as well as n-hexadecane (T = 170-280 °C, P = 5 bar) hydroisomerization similar to a 1.0 wt % Pt sample. For Pt/Y catalysts prepared with CPA, a loading of 0.3 wt % Pt (n Pt/n A = 0.08 mol/mol) sufficed for n-heptane hydroisomerization, whereas a detrimental effect on n-hexadecane hydroisomerization was observed, in particular undesired secondary cracking occurred to a significant extent. The differences between PTA and CPA are explained by differences in Pt loading per zeolite Y crystal (size ∼ 500 nm), shown from extensive transmission electron microscopy energy-dispersive X-ray spectroscopy experiments, whereby crystal-based n Pt/n A ratios could be determined. From earlier studies, it is known that the Al content per crystal of USY varied tremendously and that PTA preferentially is deposited on crystals with higher Al content due to ion-exchange with zeolite protons. Here, we show that this preferential deposition of PTA on Al-rich crystals led to a more constant value of n Pt/n A ratio from one zeolite crystal to another, which was beneficial for catalytic performance. Use of CPA led to a large variation of Pt loading independent of Al content, giving rise to larger variations of n Pt/n A ratio from crystal to crystal that negatively affected the catalytic performance. This study thus shows the impact of local metal loading variations at the zeolite crystal scale (nanoscale) caused by different interactions of metal precursors with the zeolite, which are essential to design and synthesize optimal catalysts, in particular at low noble metal loadings.

Dataset Information

Selective hydroconversion of coconut oil-derived lauric acid to alcohol and aliphatic alkane over MoO _x -modified Ru catalysts under mild conditions.

Publications

Selective hydroconversion of coconut oil-derived lauric acid to alcohol and aliphatic alkane over MoO <sub><i>x</i></sub> -modified Ru catalysts under mild conditions.

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