he characteristic study,by means of in-situ IR spectroscopy, of chemisorbed species on the Ni-catalysts for the partial oxidation of methane(POM)to syngas demonstrated the existence of CH_x(a)and H_xCO(a)adspecies on...he characteristic study,by means of in-situ IR spectroscopy, of chemisorbed species on the Ni-catalysts for the partial oxidation of methane(POM)to syngas demonstrated the existence of CH_x(a)and H_xCO(a)adspecies on the functioning Ni-catalysts, Several designed experimental investigations on the reactivities of methane with CO_2 and with O_2,respectively,over the Ni-catalysts, and of CO_2 with the prereduced Ni-catalyst,ats well as of the deposited carbon with CO_2 and with O_2,respectlvely,liave been carried out and the reLqults were unfavorable to the two-step mechanistic interpretation proposed for the POM reaction. By means of tlie BOC-MP Approach,energetics of a set of elementary reactions,which may be involved in the POM process,on the clean(111)surface of Ni,Fe,Cu and Pd, re- spectively,has been studied.The result;of the experiments and the calculation of the present work favor the direct catalytic dissociation-plus-surface oxidation-plus-further debdrogenation mechanism as the dominant pathway making major contribution to the POM reaction.展开更多
文摘he characteristic study,by means of in-situ IR spectroscopy, of chemisorbed species on the Ni-catalysts for the partial oxidation of methane(POM)to syngas demonstrated the existence of CH_x(a)and H_xCO(a)adspecies on the functioning Ni-catalysts, Several designed experimental investigations on the reactivities of methane with CO_2 and with O_2,respectively,over the Ni-catalysts, and of CO_2 with the prereduced Ni-catalyst,ats well as of the deposited carbon with CO_2 and with O_2,respectlvely,liave been carried out and the reLqults were unfavorable to the two-step mechanistic interpretation proposed for the POM reaction. By means of tlie BOC-MP Approach,energetics of a set of elementary reactions,which may be involved in the POM process,on the clean(111)surface of Ni,Fe,Cu and Pd, re- spectively,has been studied.The result;of the experiments and the calculation of the present work favor the direct catalytic dissociation-plus-surface oxidation-plus-further debdrogenation mechanism as the dominant pathway making major contribution to the POM reaction.
