TY - JOUR

T1 - NiCo/Al2O3 nanocatalysts for the synthesis of 5-amino-1-pentanol and 1,5-pentanediol from biomass-derived 2-hydroxytetrahydropyran

AU - Yang, Jian

AU - Zhang, Jia

AU - Benassi, Enrico

AU - Li, Xuemei

AU - Liu, Hailong

AU - Fang, Weiguo

AU - Tian, Junying

AU - Xia, Chungu

AU - Huang, Zhiwei

N1 - This work was financially supported by the National Natural Science Foundation of China ( 21872155 , 22102198 , and 22272187 ), the Strategic Pilot Science and Technology Project of the Chinese Academy of Sciences ( XDA21010700 ), and the CAS "Light of West China" Program . The authors also acknowledge the helpful discussion for Prof. George W. Huber at the University of Wisconsin-Madison.

PY - 2024/3

Y1 - 2024/3

N2 - Al2O3-supported monometallic Ni, Co, and bimetallic Ni–Co nanocatalysts originated from layered double hydroxide precursors were synthesized by co-precipitation method, and used for the synthesis of useful 5-amino-1-pentanol (5-AP) and 1,5-pentanediol (1,5-PD) by reductive amination (RA) or direct hydrogenation of biofurfural-derived 2-hydroxytetrahydropyran (2-HTHP), respectively. In both reactions, the yield of the target products decreased monotonously with the increasing amounts of Co in the NiCo/Al2O3 catalysts, owing probably to the replacement of highly reactive Ni by Co component with inferior hydrogenation activity at the low reaction temperature of 60 °C. However, the incorporation of Co could improve the reducibility of the NiCo/Al2O3 bimetallic catalysts and promote the reaction stability of the catalysts, especially for Ni2Co1/Al2O3, in both reactions with over 180 h time-on-stream. Characterization of the catalysts before and after the reaction showed that the incorporating Co could inhibit the sintering of metal particles and hinder the surface oxidation of the more reactive Ni0 species, thanks to the formation of Ni–Co alloy in the bimetallic catalysts. DFT-based modeling of the reaction mechanisms is also performed, supporting the reaction pathway proposed previously and also the much higher activity of Ni in the RA of 2-HTHP as compared with Co.

AB - Al2O3-supported monometallic Ni, Co, and bimetallic Ni–Co nanocatalysts originated from layered double hydroxide precursors were synthesized by co-precipitation method, and used for the synthesis of useful 5-amino-1-pentanol (5-AP) and 1,5-pentanediol (1,5-PD) by reductive amination (RA) or direct hydrogenation of biofurfural-derived 2-hydroxytetrahydropyran (2-HTHP), respectively. In both reactions, the yield of the target products decreased monotonously with the increasing amounts of Co in the NiCo/Al2O3 catalysts, owing probably to the replacement of highly reactive Ni by Co component with inferior hydrogenation activity at the low reaction temperature of 60 °C. However, the incorporation of Co could improve the reducibility of the NiCo/Al2O3 bimetallic catalysts and promote the reaction stability of the catalysts, especially for Ni2Co1/Al2O3, in both reactions with over 180 h time-on-stream. Characterization of the catalysts before and after the reaction showed that the incorporating Co could inhibit the sintering of metal particles and hinder the surface oxidation of the more reactive Ni0 species, thanks to the formation of Ni–Co alloy in the bimetallic catalysts. DFT-based modeling of the reaction mechanisms is also performed, supporting the reaction pathway proposed previously and also the much higher activity of Ni in the RA of 2-HTHP as compared with Co.

KW - Amino alcohol

KW - Layered double hydroxide

KW - NiCo bimetallic catalysts

KW - Quantum chemical calculations

KW - Reductive amination

UR - https://www.scopus.com/record/display.uri?eid=2-s2.0-85148882206&origin=inward&txGid=dc990fe021f818313ac5b5931cc0d939

UR - https://www.mendeley.com/catalogue/0dce37d8-731d-3931-aa86-38356fd66ba8/

U2 - 10.1016/j.gce.2023.01.003

DO - 10.1016/j.gce.2023.01.003

M3 - Article

VL - 5

SP - 119

EP - 131

JO - Green Chemical Engineering

JF - Green Chemical Engineering

SN - 2666-9528

IS - 1

ER -