Catalytic performance of La-modified Cu/SiO2 in the hydrogenation of methyl acetate

Q3 Energy

燃料化学学报 Pub Date : 2024-02-01 DOI:10.1016/S1872-5813(23)60382-2

Chuanming ZHANG, Weijie LI, Jincan KANG, Lina LIN, Changxin LI, Lincai LI, Haoyu ZOU, Hongping ZHU

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引用次数: 0

Abstract

A series of Cu/SiO₂ catalysts modified with lanthanum (La) (30Cu-nLa/SiO₂, n=0, 0.5, 1 and 2) were synthesized using the ethanol (EtOH)-assisted ammonia-evaporation method; their catalytic performance in the gas-phase hydrogenation of methyl acetate (MeOAc) to produce ethanol (EtOH) was investigated. The results indicate that the catalytic performance of Cu/SiO₂ can be greatly enhanced by La modification. In particular, the 30Cu-0.5La/SiO₂ catalyst exhibits excellent performance in the MeOAc hydrogenation; under 230 °C, 2 MPa H₂, an LHSV of 2 h^-1 and an H₂/MeOAc molar ratio of 20, the MeOAc conversion reaches 98.5%, with a total EtOH yield of 97.0%. The N₂-sorption, XRD, ICP-OES, H₂-TPR, FT-IR, TEM, XPS, and AES characterization results reveal that the introduced La metal has a strong interaction with Cu, which can promote the dispersion of the copper species on the SiO₂ support. Moreover, the content of Cu⁺ is increased significantly, which can enhance the electronic interaction with MeOAc via the acyl and methoxide groups and thus promote the hydrogenation of MeOAc to EtOH.

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La 改性 Cu/SiO2 在醋酸甲酯加氢反应中的催化性能

采用乙醇（EtOH）辅助氨蒸发法合成了一系列用镧（La）修饰的 Cu/SiO2 催化剂（30Cu-nLa/SiO2，n=0、0.5、1 和 2），并考察了它们在醋酸甲酯（MeOAc）气相加氢制乙醇（EtOH）过程中的催化性能。结果表明，通过 La 改性可以大大提高 Cu/SiO2 的催化性能。其中，30Cu-0.5La/SiO2 催化剂在 MeOAc 加氢反应中表现出优异的性能；在 230 ℃、2 MPa H2、2 h-1 LHSV 和 H2/MeOAc 摩尔比为 20 的条件下，MeOAc 转化率达到 98.5%，EtOH 总产率为 97.0%。N2-吸附、XRD、ICP-OES、H2-TPR、FT-IR、TEM、XPS 和 AES 表征结果表明，引入的 La 金属与铜有很强的相互作用，能促进铜物种在 SiO2 支持物上的分散。此外，Cu+ 的含量显著增加，可通过酰基和甲氧基增强与 MeOAc 的电子相互作用，从而促进 MeOAc 加氢为 EtOH。

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来源期刊

燃料化学学报 Chemical Engineering-Chemical Engineering (all)

CiteScore

2.80

自引率

0.00%

发文量

5825

期刊介绍： Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.