Atomically dispersed Cu and Fe on N-doped carbon materials for CO2 electroreduction: insight into the curvature effect on activity and selectivity,RSC Advances

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Atomically dispersed Cu and Fe on N-doped carbon materials for CO2 electroreduction: insight into the curvature effect on activity and selectivity
RSC Advances ( IF 3.9 ) Pub Date : 2020-11-26 , DOI: 10.1039/d0ra08857a
Yue Zhang ₁ , Lei Fang ₁ , Zexing Cao ₁

Affiliation

CO₂ electroreduction reaction (CO₂ER) by single metal sites embedded in N-doped graphene (M@N-Gr, M = Cu and Fe) and carbon nanotubes (M@N-CNT, M = Cu and Fe) has been explored by extensive first-principles calculations in combination with the computational hydrogen electrode model. Both atomically dispersed Cu and Fe nanostructures, as the single atom catalysts (SACs), have higher selectivity towards CO₂ER, compared to hydrogen evolution reduction (HER), and they can catalyze CO₂ER to CO, HCOOH, and CH₃OH. In comparison with Cu@N-Gr, the limiting potentials for generating CO, HCOOH, and CH₃OH are reduced obviously on the high-curvature Cu@N-CNT. However, the curvature effect is less notable for the single-Fe-atom catalysts. Such discrepancies can be attributed to the d-band center changes of the single Cu and Fe sites and their different dependences on the curvature of carbon-based support materials.

中文翻译：

用于 CO2 电还原的 N 掺杂碳材料上原子分散的 Cu 和 Fe：洞察曲率对活性和选择性的影响

通过嵌入 N 掺杂石墨烯 (M@N-Gr, M = Cu 和 Fe) 和碳纳米管 (M@N-CNT, M = Cu 和 Fe) 中的单个金属位点进行CO ₂电还原反应 (CO ₂ ER)通过广泛的第一性原理计算结合计算氢电极模型进行探索。与析氢还原 (HER) 相比，原子分散的 Cu 和 Fe 纳米结构作为单原子催化剂 (SAC) 对 CO _{2 ER 具有更高的选择性，它们可以将 CO}₂ ER 催化为 CO、HCOOH 和 CH ₃ OH . 与 Cu@N-Gr 相比，产生 CO、HCOOH 和 CH _{3的限制电位}OH 在高曲率 Cu@N-CNT 上明显减少。然而，对于单铁原子催化剂，曲率效应不太明显。这种差异可归因于单个 Cu 和 Fe 位点的 d 带中心变化及其对碳基支撑材料曲率的不同依赖性。

更新日期：2020-11-26

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