Strong Boron–Carbon Bonding Interaction Drives CO2 Reduction to Ethanol over the Boron-Doped Cu(111) Surface: An Insight from the First-Principles Calculations,The Journal of Physical Chemistry C

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Strong Boron–Carbon Bonding Interaction Drives CO2 Reduction to Ethanol over the Boron-Doped Cu(111) Surface: An Insight from the First-Principles Calculations
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-12-30 , DOI: 10.1021/acs.jpcc.0c09661
Jian-Sen Wang ₁ , Guo-Chen Zhao ₁ , Yong-Qing Qiu ₂ , Chun-Guang Liu ₃

Affiliation

Facile conversion of CO₂ into useful multicarbon products is of broad interest in the field of energy storage and controllable carbon emission. However, electrochemical CO₂ reduction to ethanol on the Cu(111) surface is limited to the high applied potential and low selectivity. Herein, we demonstrate that the Cu-based electrocatalysts modified by boron (B) single-atom greatly reduce the thermodynamic energy barrier and improve selectivity relative to pristine Cu(111) in the hydrogenation of CO₂ to ethanol. Electronic structure analysis reveals that the doped B atom, as a charge transfer medium, not only works in supplying electrons to stabilize the intermediates but also undergoes distinct reaction paths compared with pristine Cu(111) to improve the selectivity of ethanol. Moreover, the formation of the robust B–C bond and the unique isomerization step keep the C atoms of the intermediates in an opposite-charged state, which makes C–C coupling facile to generate ethanol. These findings would be very useful to guide the search for a new catalyst for electrochemical CO₂ reduction with high ethanol selectivity based on the abundant Cu-based materials.

中文翻译：

强大的硼碳键相互作用推动掺杂硼的Cu（111）表面上的CO ₂还原为乙醇：从第一性原理计算中得出的见解

在能量存储和可控制的碳排放领域，将CO ₂轻松转化为有用的多碳产品受到广泛关注。但是，电化学CO ₂在Cu（111）表面上还原为乙醇的过程仅限于高施加电势和低选择性。在这里，我们证明了硼（B）单原子修饰的铜基电催化剂大大降低了热力学能垒，并提高了相对于原始铜（111）在CO ₂加氢中的选择性乙醇。电子结构分析表明，掺杂的B原子作为电荷转移介质，不仅可以提供电子来稳定中间产物，而且与原始Cu（111）相比，还可以经历不同的反应路径，从而提高了乙醇的选择性。此外，强大的B–C键的形成和独特的异构化步骤使中间体的C原子保持相反的电荷状态，这使得C–C偶联易于生成乙醇。这些发现对于指导基于丰富的铜基材料寻找具有高乙醇选择性的电化学还原CO ₂的新催化剂将非常有用。

更新日期：2021-01-14

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