TY - JOUR
T1 - Advancing Ce–Cu–Al2O3 catalysts for waste-to-energy through strategic surface coordination modulation
AU - Ahn, Seon Yong
AU - Oh, Min Ju
AU - Shim, Jae Oh
AU - Roh, Hyun Seog
N1 - Publisher Copyright:
© 2024 Elsevier B.V.
PY - 2025/2/1
Y1 - 2025/2/1
N2 - Here, by varying the precipitation sequence during the synthesis of Ce–Cu–Al2O3 catalysts, surface-exposed atoms were controlled to dramatically enhance the intrinsic activity and stability. The reaction results revealed that the number of active sites were crucial at low temperatures. At high temperatures, the oxygen storage capacity and surface concentration of Ce3+ and Cu+ became key, with Ce or Al exposure protecting active Cu species from sintering-induced deactivation. Characterization and catalytic reaction results confirmed the superior WGS performance of the one-pot coprecipitated Ce–Cu–Al2O3 catalyst, which features abundant active Cu species, providing adsorption sites for CO activation and a lower energy barrier for H2O dissociation (reaction rate: 76.35 μmolCOgcat−1s−1; turnover frequency: 0.694 s−1 at kinetic conditions). In addition, this catalyst exhibited high stability over 50 h, significantly outperforming the sequential impregnated Ce/Cu/Al2O3 catalyst, highlighting the importance of surface coordination structure in improving catalytic performance.
AB - Here, by varying the precipitation sequence during the synthesis of Ce–Cu–Al2O3 catalysts, surface-exposed atoms were controlled to dramatically enhance the intrinsic activity and stability. The reaction results revealed that the number of active sites were crucial at low temperatures. At high temperatures, the oxygen storage capacity and surface concentration of Ce3+ and Cu+ became key, with Ce or Al exposure protecting active Cu species from sintering-induced deactivation. Characterization and catalytic reaction results confirmed the superior WGS performance of the one-pot coprecipitated Ce–Cu–Al2O3 catalyst, which features abundant active Cu species, providing adsorption sites for CO activation and a lower energy barrier for H2O dissociation (reaction rate: 76.35 μmolCOgcat−1s−1; turnover frequency: 0.694 s−1 at kinetic conditions). In addition, this catalyst exhibited high stability over 50 h, significantly outperforming the sequential impregnated Ce/Cu/Al2O3 catalyst, highlighting the importance of surface coordination structure in improving catalytic performance.
KW - High-temperature water–gas shift
KW - Precipitation sequence
KW - Surface coordination structure
KW - Waste-derived synthesis gas
KW - active Cu species
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U2 - 10.1016/j.cej.2024.159015
DO - 10.1016/j.cej.2024.159015
M3 - Article
AN - SCOPUS:85213864797
SN - 1385-8947
VL - 505
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
M1 - 159015
ER -