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TS-1 Molecular Sieves Facilitated Aldehyde Stable Production from Gas-Glycerol Dehydration: Using Liquid Feed of Glycerol-Methanol Solution

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Abstract

TS-1 with different Ti/Si molar ratios (0.02 for TS-1a, 0.025 for TS-1b, 0.03 for TS-1c), and Ti–K (TiO2-SiO2) catalysts were prepared through a hydrothermal procedure and characterized by the XRD, BET, SEM/TEM, XPS/ICP, Raman, UV–Vis, FT-IR/Py–IR, and NH3–TPD for gas-glycerol value-added conversion. The acidic [(Ti, Si)O4] sites were considered to be the reactive centers for acetaldehyde production with the selectivity closely related to the concentration of [(Ti, Si)O4] and Smicro/SBET values but not the PyB/PyL value or surface acid density. The [(Ti, Si)O4] in MFI micro-structure promoted acetaldehyde production by 1–2 dehydration and subsequent cracking of gas-glycerol, better than the [(Ti, Si)O4] without MFI micro-structure. Over the TS-1c, gas-glycerol conversion reached 91.5%, with the selectivity towards acetaldehyde and acrolein reaching 34.4% and 29.5%, respectively. Significantly, the catalytic stability of the TS-1c can be obviously improved by using liquid feed of a glycerol-methanol solution.

Graphical Abstract

TS-1c (3.3%) showed glycerol catalytic conversion reached 91.5 % with the selectivity of acetaldehyde and acrolein reaching about 34.4 %, and 29.5 %, respectively. The acidic [(Ti, Si)O4] was confirmed to be the reactive centers for acetaldehyde production, especially for the [(Ti, Si)O4] in MFI micro-structure (with b-axis 300 nm, micro-pores 5.8 Å) promoted acetaldehyde production from 1 to 2 and 1–3 dehydration of glycerol. It was new found the catalytic stability of TS-1c can be obviously improved as using liquid feed of glycerol-methanol solution.

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Acknowledgements

The work was financially supported by Natural Science Foundation project of Chongqing Science and Technology (CSTB2022NSCQ-MSX1497); Youth research project of science and technology of Chongqing municipal education commission (KJQN201800746); Sichuan Science and Technology Program (2021ZHCG0019); Research project of Chongqing Jiaotong University (19JDKJC-A017, XJ2021000901); Talent projects of Guangdong University of Petrochemical Technology (2019rc038); Featured Innovative Talents Project of Guangdong Education Department (2022KTSCX085) and Science and Technology Program of Maoming (2022038)

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Authors and Affiliations

  1. College of Materials Science and Engineering, Chongqing JiaoTong University, Chongqing, 400074, People’s Republic of China

    Hai Lan, Miao Liu, Pucheng Zhao & Qingyun Yang

  2. College of Materials Science and Engineering, Guangdong University of Petrochemical Technology, Maoming, 525000, Guangdong, People’s Republic of China

    Qi Yao

  3. Chengdu Institute of Organic Chemistry, Chinese Academy of Sciences, Chengdu, 610041, People’s Republic of China

    Biao Zhang & Yi Jiang

  4. College of Civil Engineering, Chongqing Jiaotong University, Chongqing, 400074, People’s Republic of China

    Fei Li

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  1. Hai Lan
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Lan, H., Yao, Q., Liu, M. et al. TS-1 Molecular Sieves Facilitated Aldehyde Stable Production from Gas-Glycerol Dehydration: Using Liquid Feed of Glycerol-Methanol Solution. Catal Lett 153, 3480–3491 (2023). https://doi.org/10.1007/s10562-022-04246-2

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