Water-assisted ketonization of methyl palmitate to palmitone over metal incorporated TiO2 catalysts†

IF 3.4 3区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Reaction Chemistry & Engineering Pub Date : 2024-05-28 DOI:10.1039/D4RE00111G

Jetsadagorn Pittayatornkul, Tosapol Maluangnont, Siriporn Jongpatiwut, Piyasan Praserthdam, Makoto Ogawa and Tawan Sooknoi

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Abstract

Ketonization of methyl palmitate to palmitone, a bio-lube precursor, was investigated over noble metal (Pt, Ru, and Pd) incorporated TiO₂ catalysts in the presence of water under an atmospheric H₂/N₂ flow. Methyl palmitate underwent hydrolysis to palmitic acid that ketonized to palmitone over Lewis Ti³⁺ sites. The water co-feeding also suppressed hydrodeoxygenation of methyl palmitate and palmitone cracking leading to high palmitone selectivity. The incorporated metals facilitated H₂ dissociation/spillover on TiO₂ which generated more Lewis Ti³⁺ sites for higher ketonization activity. At 400 °C, 0.5Pd/TiO₂ provided ∼90% conversion with >85% palmitone selectivity and >25 h stability, due to its efficient H₂ dissociation/spillover to continually recover Lewis Ti³⁺ sites. Meanwhile 0.5Pt/TiO₂ promoted excessive hydrodeoxygenation, leading to the deactivation from CO poisoning at the metallic Pt sites. The findings of this study offer a sustainable approach for the selective production of bio-lube precursors from renewable fatty acid methyl esters.

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在掺入金属的 TiO2 催化剂上水助酮化棕榈酸甲酯生成棕榈酮

研究了在大气 H2/N2 流动条件下，在含有贵金属（铂、钌和钯）的二氧化钛催化剂上将棕榈酸甲酯酮化为棕榈酮（一种生物润滑油前体）的过程。棕榈酸甲酯水解为棕榈酸，棕榈酸在路易斯 Ti3+ 位点上酮化为棕榈酮。水的共同作用还抑制了棕榈酸甲酯的加氢脱氧和棕榈酮的裂解，从而实现了较高的棕榈酮选择性。加入的金属促进了二氧化钛上的 H2 解离/溢出，从而产生了更多的 Lewis Ti3+ 位点，提高了酮化活性。在 400 ˚C，0.5Pd/TiO2 的转化率约为 90%，棕榈酮选择性为 85%，稳定性为 25 小时。而 0.5Pt/TiO2 则促进了过度的氢脱氧，导致金属铂位点因 CO 中毒而失活。本研究的结果为从可再生脂肪酸甲酯中选择性生产生物润滑油前体提供了一种可持续的方法。

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来源期刊

Reaction Chemistry & Engineering Chemistry-Chemistry (miscellaneous)

CiteScore

6.60

自引率

7.70%

发文量

227

期刊介绍： Reaction Chemistry & Engineering is a new journal reporting cutting edge research into all aspects of making molecules for the benefit of fundamental research, applied processes and wider society. From fundamental, molecular-level chemistry to large scale chemical production, Reaction Chemistry & Engineering brings together communities of chemists and chemical engineers working to ensure the crucial role of reaction chemistry in today’s world.