Details

Autor(en) / Beteiligte

• Guo, Jing
• Shao, Heng
• Gao, Le
• Ma, Wancheng
• Zhang, Wei
• Huang, Long
• Chu, Haibin

Titel

Efficient aqueous-phase hydrogenation of -xylylenediamine to 1,3-cyclohexandimethylamine over a highly active and stable ruthenium catalyst

Ist Teil von

• Reaction chemistry & engineering, 2024-06, Vol.9 (7), p.1836-1844

Erscheinungsjahr

2024

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• A highly active and stable ruthenium catalyst supported on alkylamine-functionalized γ-Al 2 O 3 was developed for the hydrogenation of m -xylylenediamine (MXDA) to 1,3-cyclohexandimethylamine (1,3-BAC) in aqueous phase. γ-Al 2 O 3 was amino-functionalized by surface silylation with 3-aminopropyltrethoxysilane, and then Ru species was anchored onto modified γ-Al 2 O 3 via coordination with the amino group (-NH 2 ). The catalyst was characterized by Fourier-transform infrared spectroscopy (FT-IR), H 2 temperature-programmed reduction (H 2 -TPR), X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), CO temperature-programmed desorption (CO-TPD), inductively coupled plasma-atomic emission spectrometry (ICP-AES), etc. This modification led to the formation of highly dispersed Ru, and greatly enhanced the catalytic performance. After reaction for 5 h at a temperature of 100 °C and pressure of 4 MPa H 2 , the conversion of MXDA and selectivity of 1,3-BAC reached 99.7% and 95.0%, respectively. Moreover, this modification also significantly inhibited the leaching of Ru due to the strong interaction between Ru and -NH 2 revealed by XPS and H 2 -TPR characterization, and suppressed the phase transformation of γ-Al 2 O 3 , which greatly improved the stability of the catalyst. The MXDA conversion and 1,3-BAC selectivity had no obvious decrease after six consecutive cycles. The strong interaction between Ru and -NH 2 in Ru/NH 2 -Al 2 O 3 led to the formation of highly dispersed Ru and modification of its electronic properties, and consequently greatly enhanced its performance and stability.