Theoretical study on geometric, electronic and catalytic performances of Fe dopant pairs in graphene,Physical Chemistry Chemical Physics

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Theoretical study on geometric, electronic and catalytic performances of Fe dopant pairs in graphene
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2017-09-08 00:00:00 , DOI: 10.1039/c7cp05683d
Yanan Tang _{1,

2,

3,

4,

5} , Huadou Chai _{1,

2,

3,

4,

5} , Weiguang Chen _{1,

2,

3,

4,

5} , Xiao Cui _{1,

2,

3,

4,

5} , Yaqiang Ma _{5,

6,

7,

8} , Mingyu Zhao _{5,

6,

7,

8} , Xianqi Dai _{1,

2,

3,

4,

5}

Affiliation

The formation geometries, electronic structures and catalytic properties of monovacancy and divacancy graphene sheets with two embedded Fe dopants (2Fe-MG and 2Fe-DG) have been systematically investigated using the first-principles calculations. It was found that the configuration of 2Fe-DG is slightly more stable than that of 2Fe-MG sheets and the two doped Fe atoms in graphene (2Fe-graphene) as active sites could regulate the stability of gas molecules. In addition, the adsorption of O₂ and CO molecules could modulate the electronic and magnetic properties of 2Fe-graphene systems. Moreover, the adsorption behaviors of reactants could determine the reaction pathway and energy barrier of the catalytic oxidation of CO. On the 2Fe-graphene substrates, the adsorptive decomposition of O₂ molecules (<0.20 eV) and the subsequent Eley–Rideal (ER) reaction (2O_ads + 2CO → CO₂) (<0.60 eV) have low energy barriers. In comparison, the CO₃ complex is quite stable and its formation needs to overcome a higher energy barrier (>0.90 eV). Hence, the dissociation of O₂ as an initial step is an energetically more favored process. These results provide valuable guidance for the design of functionalized graphene-based devices.

中文翻译：

石墨烯中Fe掺杂对的几何，电子和催化性能的理论研究

使用第一性原理计算系统地研究了具有两种嵌入的Fe掺杂剂（2Fe-MG和2Fe-DG）的单空位和双空位石墨烯片的形成几何形状，电子结构和催化性能。发现2Fe-DG的构型比2Fe-MG片的构型稍微稳定一些，并且石墨烯中的两个掺杂的Fe原子（2Fe-石墨烯）作为活性位点可以调节气体分子的稳定性。另外，O ₂和CO分子的吸附可以调节2Fe-石墨烯体系的电子和磁性。此外，反应物的吸附行为可以决定CO催化氧化的反应途径和能垒。在2Fe-石墨烯基体上，O ₂的吸附分解分子（<0.20 eV）和随后的Eley-Rideal（ER）反应（2O _ads + 2CO→CO ₂）（<0.60 eV）具有较低的能垒。相比之下，CO ₃络合物非常稳定，其形成需要克服更高的能垒（> 0.90 eV）。因此，作为初始步骤，O ₂的解离在能量上是更有利的过程。这些结果为功能化的基于石墨烯的器件的设计提供了有价值的指导。

更新日期：2017-09-22

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