TY - JOUR
T1 - One-pot synthesis of alanine from glycerol without additional H2 over a rutile-supported Ru catalyst
AU - Li, Jiachen
AU - Tang, Zhenchen
AU - Ahmadi, Majid
AU - Yang, Huaizhou
AU - Gerlach, Dominic
AU - Kooi, Bart J.
AU - Rudolf, Petra
AU - Heeres, Hero J.
AU - Pescarmona, Paolo P.
N1 - Publisher Copyright:
© 2024 The Authors
PY - 2024/12/27
Y1 - 2024/12/27
N2 - We successfully demonstrate the synthesis of alanine from glycerol and NH3 without additional H2, using a novel Ru-catalyst with optimized metal-support interactions. Three heterogeneous catalysts (Ru/TiO2-Anatase, Ru/TiO2-Rutile, and Ru/TiO2-P25) were compared, with Ru/TiO2-Rutile showing superior performance, giving complete glycerol conversion with 37 % alanine and 26 % lactate yield after 6 h at 220 °C. This performance matches that of state-of-the-art catalysts, but with lower Ru loading (leading to an approximately three-fold higher turnover number) and without external H2 supply. Catalyst characterization revealed that the metal-support interactions in Ru/TiO2-Rutile lead to smaller, well-dispersed Ru nanoparticles (d̅ = 2.3 nm) and lower degree of overlayer TiO2-x formation compared to Ru/TiO2-Anatase, which together contribute to higher Ru accessibility (ARu = 22 %) and thus higher number of active sites per unit mass of Ru, despite the lower surface area of rutile. The reusability of Ru/TiO2-Rutile is strongly influenced by the amount of NaOH utilized in the reaction, with a low NaOH: glycerol ratio (1.1) allowing to recycle the catalyst while largely preserving its activity.
AB - We successfully demonstrate the synthesis of alanine from glycerol and NH3 without additional H2, using a novel Ru-catalyst with optimized metal-support interactions. Three heterogeneous catalysts (Ru/TiO2-Anatase, Ru/TiO2-Rutile, and Ru/TiO2-P25) were compared, with Ru/TiO2-Rutile showing superior performance, giving complete glycerol conversion with 37 % alanine and 26 % lactate yield after 6 h at 220 °C. This performance matches that of state-of-the-art catalysts, but with lower Ru loading (leading to an approximately three-fold higher turnover number) and without external H2 supply. Catalyst characterization revealed that the metal-support interactions in Ru/TiO2-Rutile lead to smaller, well-dispersed Ru nanoparticles (d̅ = 2.3 nm) and lower degree of overlayer TiO2-x formation compared to Ru/TiO2-Anatase, which together contribute to higher Ru accessibility (ARu = 22 %) and thus higher number of active sites per unit mass of Ru, despite the lower surface area of rutile. The reusability of Ru/TiO2-Rutile is strongly influenced by the amount of NaOH utilized in the reaction, with a low NaOH: glycerol ratio (1.1) allowing to recycle the catalyst while largely preserving its activity.
KW - Alanine synthesis
KW - Glycerol valorization
KW - Metal-support interaction
KW - Ru nanoparticles
KW - Rutile
UR - http://www.scopus.com/inward/record.url?scp=85213029144&partnerID=8YFLogxK
U2 - 10.1016/j.apcatb.2024.124960
DO - 10.1016/j.apcatb.2024.124960
M3 - Article
AN - SCOPUS:85213029144
SN - 0926-3373
VL - 365
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
M1 - 124960
ER -