TY - JOUR
T1 - The influence of pore structures and Lewis acid sites on selective hydrogenolysis of guaiacol to benzene over Ru/TS-1
AU - Xin, Yingying
AU - Zheng, Zhaoxia
AU - Luo, Zhicheng
AU - Jiang, Chengzhen
AU - Gao, Shaofeng
AU - Wang, Zhihao
AU - Zhao, Chen
N1 - Publisher Copyright:
© 2022 Institute of Process Engineering, Chinese Academy of Sciences
PY - 2022/10
Y1 - 2022/10
N2 - Here, we report a Ru/TS-1 catalyst for selective hydrogenolysis of guaiacol to benzene in the aqueous phase at conditions of 240 °C and 0.2 MPa H2, achieving a benzene yield of 86% with a hydrogenolysis rate of 103.1 mmol g−1 h−1. It was found that Silicalite-1 (MFI type) with suitable pore sizes supported Ru nanoparticles (NPs) favored for hydrogenolysis of guaiacol, whereas de-aluminated Ru/HBEA, Ru/HY and Ru/MWW (without acidic sites) accelerated the parallel reactions of hydrogenation of aromatics. In addition, Ru NPs located at the orifice of Silicalite-1 was proved to be more electron-deficient and active than Ru NPs on the outer surface, as evidenced by CO-IR characterization and activity tests on Ru/Silicalite-1 (with and without templates). Moreover, Brønsted acid sites (BAS) on Ru/MFI highly promoted the hydrogenation rates of aromatics, while Lewis acid sites (LAS) on Ru/TS-1 and Ru/MFI led to a linear increase of guaiacol hydrogenolysis rate to benzene, probably due to the enhanced absorbance capability of guaiacol and phenol on the LAS of MFI. Thus, pore structure properties of MFI coupled with abundant LAS (TS-1) as well as Ru NPs on the orifice of pores of TS-1 construct a promising catalyst for achieving efficient aromatic hydrocarbons from selective hydrogenolysis of lignin.
AB - Here, we report a Ru/TS-1 catalyst for selective hydrogenolysis of guaiacol to benzene in the aqueous phase at conditions of 240 °C and 0.2 MPa H2, achieving a benzene yield of 86% with a hydrogenolysis rate of 103.1 mmol g−1 h−1. It was found that Silicalite-1 (MFI type) with suitable pore sizes supported Ru nanoparticles (NPs) favored for hydrogenolysis of guaiacol, whereas de-aluminated Ru/HBEA, Ru/HY and Ru/MWW (without acidic sites) accelerated the parallel reactions of hydrogenation of aromatics. In addition, Ru NPs located at the orifice of Silicalite-1 was proved to be more electron-deficient and active than Ru NPs on the outer surface, as evidenced by CO-IR characterization and activity tests on Ru/Silicalite-1 (with and without templates). Moreover, Brønsted acid sites (BAS) on Ru/MFI highly promoted the hydrogenation rates of aromatics, while Lewis acid sites (LAS) on Ru/TS-1 and Ru/MFI led to a linear increase of guaiacol hydrogenolysis rate to benzene, probably due to the enhanced absorbance capability of guaiacol and phenol on the LAS of MFI. Thus, pore structure properties of MFI coupled with abundant LAS (TS-1) as well as Ru NPs on the orifice of pores of TS-1 construct a promising catalyst for achieving efficient aromatic hydrocarbons from selective hydrogenolysis of lignin.
KW - Benzene
KW - Biomass
KW - Guaiacol
KW - Selective hydrogenolysis
KW - Zeolites
UR - https://www.scopus.com/pages/publications/85103238475
U2 - 10.1016/j.gee.2020.12.024
DO - 10.1016/j.gee.2020.12.024
M3 - 文章
AN - SCOPUS:85103238475
SN - 2096-2797
VL - 7
SP - 1014
EP - 1023
JO - Green Energy and Environment
JF - Green Energy and Environment
IS - 5
ER -
