期刊
ACS APPLIED MATERIALS & INTERFACES
卷 9, 期 36, 页码 30711-30721出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.7b09482
关键词
adsorption mode; adsorption energy; isobutane dehydrogenation; hydrogenolysis; Ni/SiO2 catalyst; Sri addition
资金
- National Natural Science Foundation of China [21606257, U1362201]
The reaction of isobutane over Ni/SiO2 catalyst changes from hydrogenolysis to dehydrogenation when Sn is introduced. The adsorption modes and energies of isobutane and isobutene over the Ni/SiO2 catalyst with and without SA addition were determined by in situ FTIR and a novel transient response adsorption approach. In the absence of Sn, isobutene is adsorbed in a double-site mode with H atoms in two methyl groups of isobutane, facilitating hydrogenolysis of isobutane. After the addition of Sn, a single-site adsorption mode with the H atom in the methylidyne group is speculated instead, which is beneficial to the rupture of the C-H bond rather than the C-C bond. Moreover, the double-site adsorption mode of isobutene with the C=C bond and the H atom in a methyl group is turned into single-site mode with the C=C bond after the introduction of Sn. As for the adsorption energy of isobutene, the introduction of Sn leads to an obvious decrease from 74 to 50 kJ mol(-1) and facilitates the prompt desorption of isobutene, resulting in a high selectivity of 81.9 wt %.
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