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首页> 外文期刊>Applied Surface Science >Mutualistic decomposition pathway of formaldehyde on O-predosed δ-MnO_2
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Mutualistic decomposition pathway of formaldehyde on O-predosed δ-MnO_2

机译：O掺杂的δ-MnO_2上甲醛的相互分解途径

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摘要

delta-MnO2 has been regarded as a promising catalyst to eliminate hazardous formaldehyde (HCHO). Surface groups play an important role in achieving the superior catalytic performance, while its underlying reaction mechanisms still remain ambiguous. In this work, a multiscale simulation combining atomic density functional theory and mesoscopic kinetic Monte Carlo is employed to explore the HCHO decomposition on delta-MnO2. Results show that in contrast to clean and hydroxyl(OH)-predosed surface, HCHO can be completely decomposed on oxygen (O)-decorated delta-MnO2 due to the low activation energy. Especially, a mutualistic reaction pathway with the energy barrier of rate-limiting step 60-80% lower than that of noble metals is recognized on O-predosed surface, which accounts for the excellent catalytic performance of delta-MnO2. Specifically, the reaction pathway enabled by O species (HCHO -> CH2O2 -> HCOO -> CO2) opens the second pathway (HCHO -> CHO -> OC -> CO2); meanwhile, the OH consumption in the second reaction facilitates the first O-assisted oxidization process in reverse. Moreover, an optimal OH/O ratio is proposed for further improving catalytic performance. This work reveals the novel decomposition mechanism of oxygen containing group assisted catalytic reactions, which is useful for the design of delta-MnO2 catalyst.
机译：δ-MnO2被认为是消除有害甲醛（HCHO）的有前途的催化剂。表面基团在实现优异的催化性能方面起着重要作用，而其潜在的反应机理仍然不明确。在这项工作中，结合原子密度泛函理论和介观动力学蒙特卡洛法的多尺度模拟被用于探索δMnO2上的HCHO分解。结果表明，与清洁的羟基表面不同，由于活化能低，HCHO可以在氧（O）修饰的δ-MnO2上完全分解。尤其是，在O掺杂的表面上发现了一种限速步骤的能量屏障比贵金属的能量屏障低60-80％的相互反应路径，这说明了δ-MnO2的出色催化性能。具体而言，O物种（HCHO-> CH2O2-> HCOO-> CO2）启动的反应途径打开了第二种途径（HCHO-> CHO-> OC-> CO2）；同时，第二反应中的OH消耗反过来促进了第一O-辅助的氧化过程。此外，提出了最佳的OH / O比以进一步改善催化性能。这项工作揭示了含氧基团辅助催化反应的新型分解机理，这对于设计δ-MnO2催化剂是有用的。

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