Abstract
The catalytic performance and reaction mechanism for selective catalytic reduction of NOx by methane in excess oxygen over Rh-loaded sulfated alumina were investigated. Sulfation was observed to influence the properties of catalysts in two aspects: (i) modify the dispersion and electronic state of surface rhodium species and (ii) determine the surface NOy groups. Differences in surface nitrates and their behaviors lead to different mechanisms for CH4-SCR of NO. On Rh/Al2O3, the adsorbed monodentate nitrates (1558 cm−1) could react with methane in the absence of oxygen, while remaining almost inert to the mixture of methane and an excess amount of oxygen. However, nitrates on Rh/Al2O3/SO42−, most probably bidentate nitrates (1600−1598 cm−1), were able to react with methane in the presence of oxygen. Moreover, a proportional relationship between NO conversion rates and intensities of nitrosyl (1936 cm−1) bands was found on Rh/Al2O3/SO42−, and the rate-determining step of NO conversion was probably the reduc...
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