TY - JOUR
T1 - Continuous hydrocyclization of aqueous levulinic acid to γ-valerolactone over bi-functional Ru/NbOPO4/SBA-15 catalyst under mild conditions
AU - Mani, Mariappan
AU - Mariyaselvakumar, Mariyamuthu
AU - Samikannu, Ajaikumar
AU - Panda, Asit Baran
AU - Konwar, Lakhya Jyoti
AU - Mikkola, Jyri Pekka
N1 - Funding Information:
The PRIS registration number of this publication is CSIR-CSMCRI – 04/2022 . Financial support from SERB ( SRG/2020/000325 ) and MLP0028 from CSIR , New Delhi are gratefully acknowledged. The authors also thank the Analytical Division and Centralized Instrumental Facilities of this institute for analytical support.
Funding Information:
The PRIS registration number of this publication is CSIR-CSMCRI – 04/2022. Financial support from SERB (SRG/2020/000325) and MLP0028 from CSIR, New Delhi are gratefully acknowledged. The authors also thank the Analytical Division and Centralized Instrumental Facilities of this institute for analytical support.
Publisher Copyright:
© 2022 Elsevier B.V.
PY - 2022/8/5
Y1 - 2022/8/5
N2 - Herein, we demonstrate that surface acid-base properties have marked effect upon the performance (activity, selectivity and stability) of supported Ru catalysts upon tandem hydrocyclization (hydrogenation-dehydration) of aqueous levulinic acid. A mesoporous bi-functional Ru/NbOPO4/SBA-15 catalyst incorporating highly dispersed Ru sites and well balanced strong Brønsted acidic sites (optimum B/L and M+S/W ratio) was identified, which outperformed the benchmark monofuncational (Ru/SBA-15, Ru/MCM-41) and physically blended bi-functional catalysts (Ru catalysts mixed with acid co-catalysts e.g. NbOPO4/Amberlyst-15). Further, the catalyst also demonstrated remarkable stability in a fixed-bed reactor, maintaining steady activity and γ-valerolactone selectivity (72–86%) during ca. 300 h time on stream (10 bar, 90–100 °C), corroborating its industrial potential. The exceptional performance and durability of the bi-functional catalyst was attributed to the presence of well dispersed hydrothermally and chemically stable acid (NbOPO4) and redox (Ru) sites.
AB - Herein, we demonstrate that surface acid-base properties have marked effect upon the performance (activity, selectivity and stability) of supported Ru catalysts upon tandem hydrocyclization (hydrogenation-dehydration) of aqueous levulinic acid. A mesoporous bi-functional Ru/NbOPO4/SBA-15 catalyst incorporating highly dispersed Ru sites and well balanced strong Brønsted acidic sites (optimum B/L and M+S/W ratio) was identified, which outperformed the benchmark monofuncational (Ru/SBA-15, Ru/MCM-41) and physically blended bi-functional catalysts (Ru catalysts mixed with acid co-catalysts e.g. NbOPO4/Amberlyst-15). Further, the catalyst also demonstrated remarkable stability in a fixed-bed reactor, maintaining steady activity and γ-valerolactone selectivity (72–86%) during ca. 300 h time on stream (10 bar, 90–100 °C), corroborating its industrial potential. The exceptional performance and durability of the bi-functional catalyst was attributed to the presence of well dispersed hydrothermally and chemically stable acid (NbOPO4) and redox (Ru) sites.
KW - Bi-functional catalyst
KW - Catalyst deactivation
KW - Flow chemistry
KW - Supported Ru-catalysts
KW - Tandem hydrocyclization
KW - γ-valerolactone
UR - http://www.scopus.com/inward/record.url?scp=85133252862&partnerID=8YFLogxK
U2 - 10.1016/j.apcata.2022.118744
DO - 10.1016/j.apcata.2022.118744
M3 - Article
AN - SCOPUS:85133252862
SN - 0926-860X
VL - 643
JO - Applied Catalysis A: General
JF - Applied Catalysis A: General
M1 - 118744
ER -