Pyridinic-N Coordination Effect on the Adsorption and Activation of CO2 by Single Vacancy Iron-Doped Graphene,Langmuir

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Pyridinic-N Coordination Effect on the Adsorption and Activation of CO2 by Single Vacancy Iron-Doped Graphene
Langmuir ( IF 3.7 ) Pub Date : 2024-03-18 , DOI: 10.1021/acs.langmuir.3c03327
Hugo Cabrera-Tinoco ₁ , Luis Borja-Castro ₂ , Renato Valencia-Bedregal ₂ , Adela Perez-Carreño ₁ , Aldo Lalupu-García ₁ , Ismael Veliz-Quiñones ₁ , Angel Guillermo Bustamante Dominguez ₂ , Crispin H W Barnes ₃ , Luis De Los Santos Valladares _{3,

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Affiliation

Graphene doped with different transition metals has been recently proposed to adsorb CO₂ and help reduce the greenhouse effect. Iron-doped graphene is one of the most promising candidates for this task, but there is still a lack of full understanding of the adsorption mechanism. In this work, we analyze the electronic structure, geometry, and charge redistribution during adsorption of CO₂ molecules by single vacancy iron-doped graphene by DFT calculations using the general gradient approximation of Perdew, Burke, and Ernzernhof functional (PBE) and the van der Waals density functional (vdW). To understand the impact of the pyridinic-N coordination of the iron atom, we gradually replaced the neighboring carbon atoms by nitrogen atoms. The analysis indicates that chemisorption and physisorption occur when the molecule is adsorbed in the side-on and end-on orientation, respectively. Adsorption is stronger when pyridinic-N coordination increases, and the vdW functional describes the chemical interactions and adsorption energy differently in relation to PBE without significant structural changes. The development of the chemical interactions with the change of coordination in the system is further investigated in this work with crystal overlap Hamilton population (COHP) analysis.

中文翻译：

吡啶-N配位对单空位铁掺杂石墨烯吸附和活化CO2的影响

最近提出掺杂不同过渡金属的石墨烯可以吸附CO ₂并有助于减少温室效应。铁掺杂石墨烯是这项任务最有希望的候选者之一，但仍缺乏对吸附机制的充分了解。在这项工作中，我们利用 Perdew、Burke 和 Ernzernhof 泛函 (PBE) 的一般梯度近似和 van 进行 DFT 计算，分析单空位铁掺杂石墨烯吸附 CO ₂分子过程中的电子结构、几何形状和电荷重新分布。德华密度泛函 (vdW)。为了了解铁原子吡啶-N配位的影响，我们逐渐用氮原子取代邻近的碳原子。分析表明，当分子分别以侧向和端向吸附时，会发生化学吸附和物理吸附。当吡啶-N 配位增加时，吸附更强，并且 vdW 泛函描述的化学相互作用和吸附能与 PBE 不同，且结构没有显着变化。这项工作通过晶体重叠汉密尔顿布居 (COHP) 分析进一步研究了化学相互作用的发展与系统中配位的变化。

更新日期：2024-03-18

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