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利用程序升温脱附、程序升温还原、程序升温表面反应、程序升温反应和化学捕获反应等手段 ,对Rh/SiO2 催化剂上甲烷部分氧化制合成气反应进行了研究 .结果表明 ,Rh/SiO2 催化剂上甲烷部分氧化制合成气机理属于热解 氧化反应机理 .甲烷首先在催化剂上发生解离吸附 ,产生具有不同H/C比的化学吸附物种CHx(x =1～ 3) .其中 ,具有较高H/C比的CHx 可能是甲烷部分氧化反应的活性物种 ,而具有较低H/C比的CHx 可能是催化剂上积碳并导致催化剂失活的来源 .活性物种CHx在活性氧物种的作用下 ,生成含氧中间体物种CHxO或继续脱氢 .含氧中间体物种进一步分解 ,即生成CO和H2 ;CO2 也可由CHx 或CHxO物种进一步氧化生成
The reaction of partial oxidation of methane to syngas over Rh / SiO2 catalyst was studied by means of temperature programmed desorption, temperature programmed reduction, temperature programmed surface reaction, temperature programmed reaction and chemical trapping reaction. The results showed that on the Rh / SiO2 catalyst The mechanism of partial oxidation of methane to syngas belongs to the mechanism of pyrolysis and oxidation. Methane is first dissociated and adsorbed on the catalyst to produce CHx (x = 1 ~ 3) with different H / C ratio. Among them, / C ratio of CHx may be the active species of partial oxidation of methane, and CHx with a lower H / C ratio may be a source of carbon deposition on the catalyst and lead to catalyst deactivation Active species CHx Under the action of reactive oxygen species, Generate oxygen-containing intermediate species CHxO or continue dehydrogenation.Oxygen-containing intermediate species are further decomposed to produce CO and H2; CO2 may also be further oxidized by CHx or CHxO species