TY - JOUR
T1 - Elucidating the role of La3+/Sm3+ in the carbon paths of dry reforming of methane over Ni/Ce-La(Sm)-Cu-O using transient kinetics and isotopic techniques
AU - Hussien, Aseel G.S.
AU - Damaskinos, Constantinos M.
AU - Dabbawala, Aasif
AU - ANJUN, Dalaver H.
AU - Vasiliades, Michalis A.
AU - Khaleel, Maryam T.A.
AU - Wehbe, Nimer
AU - Efstathiou, Angelos M.
AU - Polychronopoulou, Kyriaki
N1 - KAUST Repository Item: Exported on 2021-12-28
Acknowledgements: Aseel Gamal Suliman Hussien and Kyriaki Polychronopoulou acknowledge the financial support from the Abu Dhabi Department of Education and Knowledge (ADEK) through the Abu Dhabi Award Research Excellence (AARE) 2017, grant No. AARE2017-258. Khalifa University is acknowledged for the financial support through the grant RC2-2018-024. The Cyprus Research and Innovation Foundation through the grant INFRASTRUCTURES/1216/0070, and the Research Committee of the University of Cyprus are gratefully acknowledged for the financial support of this work.
PY - 2021/12/16
Y1 - 2021/12/16
N2 - The different effects of the presence of La3+ and Sm3+ heteroatoms in the 5 wt% Ni/45Ce-45(Sm or La)-10Cu-O catalytic system on the carbon deposition and removal reaction paths in the dry reforming of methane (DRM) at 750 °C were investigated using transient kinetic and isotopic experiments. The relative initial rates of carbon oxidation by lattice oxygen of support and that by oxygen derived from CO2 dissociation under DRM reaction conditions were quantified. Ni nanoparticles (23-nm) supported on La 3+-doped ceria exhibited at least 3 times higher initial rates of carbon oxidation to CO by lattice oxygen, and ~ 13 times lower rates of carbon accumulation than Ni (18-nm) supported on Sm3+-doped ceria. The concentration and mobility of labile surface oxygen at the Ni-support interface region seems to correlate with carbon accumulation. Ni/Ce-La(or Sm)-–10Cu-O formed NiCu alloy nanoparticles, partly responsible for lowering carbon deposition and increasing carbon oxidation rates to CO.
AB - The different effects of the presence of La3+ and Sm3+ heteroatoms in the 5 wt% Ni/45Ce-45(Sm or La)-10Cu-O catalytic system on the carbon deposition and removal reaction paths in the dry reforming of methane (DRM) at 750 °C were investigated using transient kinetic and isotopic experiments. The relative initial rates of carbon oxidation by lattice oxygen of support and that by oxygen derived from CO2 dissociation under DRM reaction conditions were quantified. Ni nanoparticles (23-nm) supported on La 3+-doped ceria exhibited at least 3 times higher initial rates of carbon oxidation to CO by lattice oxygen, and ~ 13 times lower rates of carbon accumulation than Ni (18-nm) supported on Sm3+-doped ceria. The concentration and mobility of labile surface oxygen at the Ni-support interface region seems to correlate with carbon accumulation. Ni/Ce-La(or Sm)-–10Cu-O formed NiCu alloy nanoparticles, partly responsible for lowering carbon deposition and increasing carbon oxidation rates to CO.
UR - http://hdl.handle.net/10754/674178
UR - https://linkinghub.elsevier.com/retrieve/pii/S0926337321011401
UR - http://www.scopus.com/inward/record.url?scp=85121462496&partnerID=8YFLogxK
U2 - 10.1016/j.apcatb.2021.121015
DO - 10.1016/j.apcatb.2021.121015
M3 - Article
SN - 0926-3373
VL - 304
SP - 121015
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
ER -