TY - JOUR
T1 - Reaction pathway design and optimization in heterogeneous catalysis
T2 - I. Optimal proportion of multi-pathways designed by the transient response method
AU - Kobayashi, Masayoshi
AU - Golman, Boris
AU - Kanno, Tohru
AU - Fujisaki, Shintaro
PY - 1997/3/27
Y1 - 1997/3/27
N2 - An optimal proportion of multi-pathways in heterogeneous catalysis has been designed by the transient response method, as a possible model reaction, using carbon monoxide oxidation on differently prepared zinc oxides, on which two different reaction pathways occur in parallel. Two polycrystalline ZnO samples have been studied: one prepared by the New Jersey Zinc Co. (K25-ZnO) and the other by Kanto Chemical Co. (Kan-ZnO). The turnover frequency (TOF) calculated from the apparent steady state rate (SSR) on K25-ZnO (dual reaction path mechanism with L-H and E-R) is 20-370 times larger than one on Kan-ZnO (dual E-R path mechanism) at 150°C. The instantaneous TOF (transient state rate = TSR) evaluated from the transient response curves on K25-ZnO is 1.0-1.5 times higher than the steady state TOF at 150°C. The yield of CO2 produced due to the cyclic operation of the proposed PCO-jump is 31% higher than ones due to steady state operation. The computer simulation analysis concludes that the optimal reaction path proportion is 95.3% for the L-H path and 4.7% for the E-R path at SSR, and 61% for the L-H path and 39% for the E-R path at TSR, which can be designed by choosing gas compositions and operating procedures.
AB - An optimal proportion of multi-pathways in heterogeneous catalysis has been designed by the transient response method, as a possible model reaction, using carbon monoxide oxidation on differently prepared zinc oxides, on which two different reaction pathways occur in parallel. Two polycrystalline ZnO samples have been studied: one prepared by the New Jersey Zinc Co. (K25-ZnO) and the other by Kanto Chemical Co. (Kan-ZnO). The turnover frequency (TOF) calculated from the apparent steady state rate (SSR) on K25-ZnO (dual reaction path mechanism with L-H and E-R) is 20-370 times larger than one on Kan-ZnO (dual E-R path mechanism) at 150°C. The instantaneous TOF (transient state rate = TSR) evaluated from the transient response curves on K25-ZnO is 1.0-1.5 times higher than the steady state TOF at 150°C. The yield of CO2 produced due to the cyclic operation of the proposed PCO-jump is 31% higher than ones due to steady state operation. The computer simulation analysis concludes that the optimal reaction path proportion is 95.3% for the L-H path and 4.7% for the E-R path at SSR, and 61% for the L-H path and 39% for the E-R path at TSR, which can be designed by choosing gas compositions and operating procedures.
KW - CO oxidation ZnO
KW - Multi-pathway reaction
KW - Optimum reaction path
KW - Transient responses
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U2 - 10.1016/S0926-860X(96)00265-7
DO - 10.1016/S0926-860X(96)00265-7
M3 - Article
AN - SCOPUS:30244558948
VL - 151
SP - 193
EP - 205
JO - Applied Catalysis A: General
JF - Applied Catalysis A: General
SN - 0926-860X
IS - 1
ER -