Theoretical DFT Study on the Mechanisms of CO/CO2 Conversion in Chemical Looping Catalyzed by Calcium Ferrite,The Journal of Physical Chemistry A

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Theoretical DFT Study on the Mechanisms of CO/CO2 Conversion in Chemical Looping Catalyzed by Calcium Ferrite
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2021-09-10 , DOI: 10.1021/acs.jpca.1c04431
Jing Wang ₁ , Jiande Gu ₁ , Asif Rony ₂ , Maohong Fan ₂ , Jerzy Leszczynski ₁

Affiliation

The CO/CO₂ conversion mechanism on the calcium ferrite (CFO) surface in chemical looping was explored by a computational study using the density functional theory approach. The CFO catalytic reaction pathway of 2CO + O₂ → 2CO₂ conversion has been elucidated. Our results show that the Fe center in CFO plays the key role as a catalyst in the CO/CO₂ conversion. Two energetically stable spin states of CFO, quintet and septet, serve as the effective catalysts. The presence of the triplet O₂ molecule caused the conversion of these two spin-state structures into each other along the catalytic reaction pathway. A double release of CO₂ was predicted following this reaction mechanism. The rate-determining step is the formation of the 2CO₂–CFO complex (P4) in the quintet state (19.0 kcal/mol). The predicted energy barriers for all the steps suggest that the proposed pathway is plausible.

中文翻译：

铁氧体钙催化化学循环中CO/CO2转化机理的理论DFT研究

通过使用密度泛函理论方法的计算研究，探索了化学循环中铁酸钙 (CFO) 表面的 CO/CO ₂转化机制。阐明了2CO + O ₂ → 2CO ₂转化的CFO催化反应途径。我们的结果表明，CFO 中的 Fe 中心作为 CO/CO ₂转化的催化剂起着关键作用。CFO 的两种能量稳定的自旋态，五重奏和七重奏，作为有效的催化剂。三重态 O ₂分子的存在导致这两种自旋态结构沿催化反应途径相互转化。CO _{2 的}双重释放预测遵循这种反应机制。决定速率的步骤是形成五重态 (19.0 kcal/mol)的 2CO ₂ –CFO 复合物 (P4)。所有步骤的预测能量障碍表明所提出的途径是合理的。

更新日期：2021-09-23

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