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借助脉冲反应、质谱-程序升温表面反应(MS-TPSR)等技术研究了Ni/α-Al2O3催化剂上甲烷催化部分氧化制合成气(POM)的反应机理.结果表明,NiO上CH4不能解离产生H2只有当NiO被CH4还原为Ni0后,CH4才能解高产生H2,Ni0是CH4活化和POM反应的活性相;POM反应机理遵循直接氧化机理,CH4和O2均在Ni0上活化,活化过程形成的Ni…C和Niδ…Oδ物种是反应历程中的关键物种,Niδ+…Oδ物种高选择性地与CH4解离产生的碳物种Ni…C反应生成CO.
The reaction mechanism of partial oxidation of methane to synthesis gas (POM) over Ni / α-Al2O3 catalyst was studied by means of pulse reaction and MS-TPSR. The results show that CH4 can not be dissociated to produce H2 on NiO. Only when NiO is reduced to Ni0 by CH4, CH4 can produce high H2. Ni0 is the active phase of CH4 activation and POM reaction. The mechanism of POM follows the direct oxidation mechanism, CH4 and O2 Are activated on Ni0, the Ni ... C and Niδ ... Oδ species formed during the activation process are the key species in the reaction process, and the Niδ + ... Oδ species selectively react with the Ni species C ... generated by the dissociation of CH4 to form CO.