当前位置: X-MOL 学术Mol. Simulat. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
The kinetic study of the methane oxidation reaction catalyzed by transition metal oxides RuO/RhO/PdO
Molecular Simulation ( IF 2.1 ) Pub Date : 2019-12-06 , DOI: 10.1080/08927022.2019.1699923
Hongxia Liu 1, 2 , Ling Fu 3 , Chaozheng He 4
Affiliation  

ABSTRACT The relative stability and kinetics of CH4 … O2 … MO and the reaction potential energy surface under the transition metal oxide catalysts (RuO/RhO/PdO) during methane oxidation reaction were studied with density functional calculations. The results show that the reaction can be easily carried out under the catalysis of transition metal oxides. The transition barriers and the reaction rate constant all show oscillation modes that are consistent with the increase of atomic number at 298 K. while the calculated reaction energies (Er/kcal mol−1) are gradually increased. The oxidised dioxide can be treated to form metal and oxygen that can still be used as a catalyst for methane oxidation; the resulting oxygen can continue to be used as an oxidant. We also calculated the rate constant of methane oxidation reaction to give the resulting methanol pathway. The calculated dynamic characterisation shows that the rate constant has a positive temperature dependence. Our calculation show that this reaction is exothermic reaction via the RuO/RhO/PdO catalyst, and the reaction is thermodynamically feasible. This study also provides theoretical reference data for us to identify new catalysts for the catalytic oxidation of methane.

中文翻译:

过渡金属氧化物RuO/RhO/PdO催化甲烷氧化反应的动力学研究

摘要 利用密度泛函计算研究了甲烷氧化反应过程中 CH4 … O2 … MO 的相对稳定性和动力学以及过渡金属氧化物催化剂 (RuO/RhO/PdO) 下的反应势能面。结果表明,该反应在过渡金属氧化物的催化下很容易进行。跃迁势垒和反应速率常数均显示振荡模式,与 298 K 时原子序数的增加一致,而计算的反应能 (Er/kcal mol-1) 逐渐增加。氧化后的二氧化物可以被处理形成金属和氧气,这些金属和氧气仍然可以用作甲烷氧化的催化剂;产生的氧气可以继续用作氧化剂。我们还计算了甲烷氧化反应的速率常数,以给出所得的甲醇途径。计算出的动态特性表明速率常数具有正温度依赖性。我们的计算表明,该反应是通过 RuO/RhO/PdO 催化剂的放热反应,并且该反应在热力学上是可行的。本研究也为我们寻找新的甲烷催化氧化催化剂提供了理论参考数据。
更新日期:2019-12-06
down
wechat
bug