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
- Authors
- Karanwal, N.; Sibi, M.G.; Khan, M.K.; Myint, A.A.; Chan, Ryu B.; Kang, J.W.; Kim, J.
- Issue Date
- 5-3월-2021
- Publisher
- American Chemical Society
- Keywords
- 1,4-pentanediol; biomass; Cu-Ni alloy; hydrogen spillover; levulinic acid; one-pot conversion
- Citation
- ACS Catalysis, v.11, no.5, pp.2846 - 2864
- Indexed
- SCIE
SCOPUS
- Journal Title
- ACS Catalysis
- Volume
- 11
- Number
- 5
- Start Page
- 2846
- End Page
- 2864
- URI
- https://scholar.korea.ac.kr/handle/2021.sw.korea/129092
- DOI
- 10.1021/acscatal.0c04216
- ISSN
- 2155-5435
- Abstract
- 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 °C and a H2 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 γ-valerolactone (GVL) at the Brønsted 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 H2 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. © 2021 American Chemical Society.
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