Base-Free Conversion of 1, 2-Propanediol to Methyl Lactate in Methanol Over Cu-Modified Au/ Hydroxylapatite Catalysts

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL Catalysis Letters Pub Date : 2024-11-16 DOI:10.1007/s10562-024-04838-0

Junying Tian, Yingying Fan, Tao Wei, Qingxia Guo, Weiguo Fang, Yongle Guo

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Abstract

The catalytic oxidative esterification of 1, 2-propanediol to methyl lactate in a base-free methanol system over Cu-modified Au/HAP catalysts was investigated. The catalysts demonstrated efficient activity in converting 1, 2-propanediol to methyl lactate without any base additives, achieving a conversion of 91.2% and a selectivity of 45% for methyl lactate under optimized conditions of 160 °C, 2 h, and 1.0 MPa O₂ over 2Au12Cu/HAP catalyst. The Au sites were identified as pivotal in catalyzing the oxidation of 1, 2-propanediol, and the basic sites of HAP was hypothesized to play a similar role with base additives to enhance the catalytic activity of Au. Furthermore, modification of Cu to Au was observed to promote the oxidation of the hydroxyacetone intermediate to methyl lactate while effectively suppressing the over-oxidation of methyl lactate, thus increased selectivity of methyl lactate.

Graphical Abstract

1,2-propanediol was convertedto methyl lactateefficientlyin a base-free methanol system over Au-Cu/HAP catalysts

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在铜改性金/羟基磷灰石催化剂上将甲醇中的 1，2-丙二醇无碱转化为乳酸甲酯

研究了铜改性金/氢氧化铝催化剂在无碱甲醇体系中将 1，2-丙二醇催化氧化酯化为乳酸甲酯的过程。在 2Au12Cu/HAP 催化剂上，在 160 ℃、2 小时和 1.0 MPa O2 的优化条件下，催化剂在将 1，2-丙二醇转化为乳酸甲酯时表现出高效的活性，转化率达到 91.2%，乳酸甲酯的选择性达到 45%。金位点被认为是催化 1，2-丙二醇氧化的关键位点，而 HAP 的碱性位点被认为也能发挥类似的作用，其碱添加剂能增强金的催化活性。此外，还观察到将 Cu 改性为 Au 可促进羟基丙酮中间体氧化为乳酸甲酯，同时有效抑制乳酸甲酯的过度氧化，从而提高了乳酸甲酯的选择性。

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.