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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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