Cu/ZnO催化剂上逆向水煤气变换反应反应机理的MonteCarlo模拟

MONTE CARLO SIMULATION FOR MECHANISM OF REVERSE WATERGAS SHIFT REACTION OVER Cu/ZnO CATALYST

采用ＭｏｎｔｅＣａｒｌｏ方法模拟了ＣＯ２在Ｃｕ／ＺｎＯ催化剂上的解离反应，发现在ＣＯ２的解离过程中只有ＣＯ生成；若用Ｈ２对生成的表面吸附氧进行还原，所生成的Ｈ２Ｏ量与前期生成的ＣＯ量相同，说明在Ｃｕ／ＺｎＯ上ＣＯ２和Ｈ２之间发生了化学计量的氧化还原反应，即逆向水煤气反应可能以表面氧化还原反应机理进行。此外，通过比较模拟与实验结果，推断在本实验条件下，氢在ＺｎＯ上发生溢流。

The reverse water gas shift reaction (RWGS) and the CO 2 dissociation over Cu/ZnO catalyst were simulated with Monte Carlo (MC) method It was found that only CO molecules and oxygen species wre formed during the dissociation of CO 2 on Cu/ZnO catalyst When the oxygen species were hydrogenated to H 2O, the amount of H 2O formed was almost the same as that of CO previously formed This indicated that all of the oxygen species formed from CO 2 were reduced to H 2O, and that the surface oxidation and reduction reaction between CO 2 and H 2 occurred on Cu/ZnO Therefore, it was suggested that the RWGS reaction proceeded via the surface redox mechanism under present experimental conditions By comparing the simulation and experimental results on the RWGS reaction, besides, it was deduced that the spillover of H 2 took place on ZnO during the RWGS reaction