PMID- 20973587 OWN - NLM STAT- MEDLINE DCOM- 20110207 LR - 20131121 IS - 1520-5827 (Electronic) IS - 0743-7463 (Linking) VI - 26 IP - 21 DP - 2010 Nov 2 TI - Understanding the effect of cobalt particle size on Fischer-Tropsch synthesis: surface species and mechanistic studies by SSITKA and kinetic isotope effect. PG - 16558-67 LID - 10.1021/la101555u [doi] AB - Co/gamma-Al(2)O(3) catalysts with particle sizes in the range of 4-15 nm were investigated by isothermal hydrogenation (IH), temperature programmed hydrogenation (TPH), and steady-state isotopic transient kinetic analysis (SSITKA). Kinetic isotope effect experiments were used to probe possible mechanisms on Co/gamma-Al(2)O(3) with different particle size. It was found that CO dissociated on Co/gamma-Al(2)O(3) catalysts at 210 degrees C. The total amount of CO(2) formed following the dissociation depends on the cobalt crystal size. O-Co binding energy was found to be highly dependent on the Co metal particle size, whereas similar C-Co binding energy was found on catalysts with different Co particle size. Very strongly bonded carbon and oxygen surface species increased with decreasing particle size and acted as site blocking species in the methanation reaction. SSITKA experiments showed that the intrinsic activity (1/tau(CH(x))) remained constant as the particle size increased from 4 to 15 nm. The number of surface intermediates (N(CH(x))) increased with increasing particle size. The apparent activation energies were found similar for these catalysts, about 85 kJ/mol. D(2)-H(2) switches further confirmed that the particle size did not change the kinetically relevant steps in the reaction. The reactivity of the active sites on the 4 nm particles was the same as those on the 8, 11, and 15 nm particles, and only the number of total available surface active sites was less on the 4 nm particles than on the others. FAU - Yang, Jia AU - Yang J AD - Department of Chemical Engineering, Norwegian University of Science & Technology, NO-7491 Trondheim, Norway. FAU - Tveten, Erik Z AU - Tveten EZ FAU - Chen, De AU - Chen D FAU - Holmen, Anders AU - Holmen A LA - eng PT - Journal Article PT - Research Support, Non-U.S. Gov't PL - United States TA - Langmuir JT - Langmuir : the ACS journal of surfaces and colloids JID - 9882736 RN - 142M471B3J (Carbon Dioxide) RN - 3G0H8C9362 (Cobalt) RN - 7U1EE4V452 (Carbon Monoxide) RN - 7YNJ3PO35Z (Hydrogen) RN - AR09D82C7G (Deuterium) RN - LMI26O6933 (Aluminum Oxide) SB - IM MH - Aluminum Oxide/chemistry MH - Carbon Dioxide/chemical synthesis/chemistry MH - Carbon Monoxide/chemistry MH - Catalysis MH - Cobalt/*chemistry MH - Deuterium/*chemistry MH - Hydrogen/*chemistry MH - Kinetics MH - Oxidation-Reduction MH - Particle Size MH - Surface Properties EDAT- 2010/10/27 06:00 MHDA- 2011/02/08 06:00 CRDT- 2010/10/27 06:00 PHST- 2010/10/27 06:00 [entrez] PHST- 2010/10/27 06:00 [pubmed] PHST- 2011/02/08 06:00 [medline] AID - 10.1021/la101555u [doi] PST - ppublish SO - Langmuir. 2010 Nov 2;26(21):16558-67. doi: 10.1021/la101555u.