Adsorption and Reactivity of CO2 on Defective Graphene Sheets
Adsorption and Reactivity of CO2 on Defective Graphene Sheets
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DOI：
10.1021/jp807087y
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发表时间：
2009-01-15
影响因子：
2.9
通讯作者：
Cabrera-Sanfelix, Pepa
中科院分区：
文献类型：
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作者：
Cabrera-Sanfelix, Pepa
已进行密度泛函计算来研究 CO2 在由单个石墨烯片代表的缺陷石墨 (0001) 上的吸附。在强物理吸附状态下，与空位缺陷的相互作用给出了类似于 136 meV 的计算分子结合能。随后，在克服相对于气相的大约1eV的势垒后，将发生通过内酯基团形成的化学吸附，放热约为1.4eV。在克服类似于 0.9 eV 和类似于 1.0 eV 的连续能垒之后，从这种化学吸附状态的进一步反应路径导致 CO2 通过环氧基团的形成而解离，随后进行氧重组和 O-2 解吸。相对于初始状态，全局最小值（“O-2 解吸 + 石墨烯片”）需要释放约 3.4 eV 的能量。
Density-functional calculations have been performed to investigate the adsorption of CO2 on defected graphite (0001) represented by a single graphene sheet. The interaction with a vacancy defect gives a computed molecular binding energy of similar to 136 meV in a strong physisorbed state. Subsequently, chemisorption by lactone group formation will occur after overcoming a barrier of similar to 1 eV relative to the gas phase, with an exothermicity of about 1.4 eV. Further reaction paths from this chemisorbed state lead to dissociation of the CO2 through the formation of epoxy groups followed by oxygen recombination and desorption of O-2, after overcoming successive energy barriers of similar to 0.9 and similar to 1.0 eV. The global minimum ("O-2 desorbed + graphene sheet") entails an energy release of about 3.4 eV with respect to the initial state.