4.8 Article

Trimetallic Cu-Ni-Zn/H-ZSM-5 Catalyst for the One-Pot Conversion of Levulinic Acid to High-Yield 1,4-Pentanediol under Mild Conditions in an Aqueous Medium

期刊

ACS CATALYSIS
卷 11, 期 5, 页码 2846-2864

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c04216

关键词

biomass; levulinic acid; 1,4-pentanediol; one-pot conversion; Cu-Ni alloy; hydrogen spillover

资金

  1. National Research Foundation of Korea (NRF) grant - Ministry of Science and ICT, Republic of Korea [2020R1A2C2003947]
  2. National Research Foundation of Korea (NRF) - Korean Government (MSIP) [2020H1D3A1A02079883, 2020M1A2A2080430, 2020H1D3A2A02043653]
  3. National Research Foundation of Korea [2020M1A2A2079798, 2020H1D3A1A02079883, 2020H1D3A2A02043653, 4199990313853, 2020R1A2C2003947] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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The study found that the trimetallic Zn-promoted Cu-Ni alloy on H-ZSM-5 catalyst can effectively convert levulinic acid to 1,4-pentanediol with a high yield of 93.4% and has the ability for regeneration.
The one-pot direct conversion of levulinic acid (LA) to 1,4-pentanediol (1,4-PDO) was investigated over a trimetallic Zn-promoted Cu-Ni alloy on a H-ZSM-5 (Cu-Ni-Zn/H-ZSM-5) catalyst. Under mild reaction conditions at 130 degrees C and a H-2 pressure of 2.5 MPa for 6 h in an aqueous medium, almost complete conversion of LA to high-yield 1,4-PDO (93.4%) was achieved. The presence of the Zn promoter effectively suppressed the growth of the Cu-Ni alloy nanoparticles (NPs) on the surface of H-ZSM-5. Consequently, the reducibility of the Cu-Ni-Zn alloy was much higher than that of the Cu-Ni alloy. The numerous Lewis acid sites of the Cu-Ni-Zn/H-ZSM-5 catalyst enhanced the adsorption of LA, and the adsorbed LA was converted to.-valerolactone (GVL) at the Bronsted acid sites of H-ZSM-5 followed by hydrogenation at the Cu-Ni alloy sites. Subsequently, the readsorption of GVL was activated at the Lewis acid sites and GVL underwent ring opening, followed by hydrogenation to form 1,4-PDO at the Cu-Ni alloy sites. The H-2 spillover on the Zn-promoted Cu-Ni alloy NPs enhanced the hydrogenation of LA to 1,4-PDO. Because of the mild reaction conditions, the formation of coke and active site sintering was highly suppressed. In addition, metal leaching did not occur over the trimetallic Cu-Ni-Zn/H-ZSM-5 catalyst. Consequently, the Cu-Ni-Zn/H-ZSM-5 catalyst could be used for up to five cycles with minimal activity loss.

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