*CO 覆盖率对 Cu2O 上 Cu2O 上 CO2 选择性电催化还原为乙烯的影响,The Journal of Physical Chemistry C

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*CO 覆盖率对 Cu2O 上 Cu2O 上 CO2 选择性电催化还原为乙烯的影响
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2022-11-30 , DOI: 10.1021/acs.jpcc.2c06898
Ruonan Duan ₁ , Laixing Luo ₁ , Wu Qin ₁ , Xianbin Xiao ₁ , Rhonin Zhou ₂ , Zongming Zheng ₁

Affiliation

具有配位不饱和 Cu 位点的Cu ₂ O 表面揭示了 CO ₂向 C ₂ H ₄生产的电还原的优势。了解*CO 覆盖率和真正的活性位点的作用对于很好地掌握催化机制具有重要意义。_在此，_基于密度泛函理论，从_*_CO和关键中间体；C-C耦合步骤的能量分布；并对后续的反应机理进行了研究。结果表明，铜Cu _{2 O(111) 表面上的}_CUS对*CO 吸附和后续反应特别活跃，由于不饱和的 Cu 原子，它是首选位点。*CO 覆盖率通过影响吸附剂-吸附剂相互作用明显调节 *COH 和 *CHO 中间体的吸附稳定性。_{*CO 在 0.13–0.25 范围内的更高覆盖度通过降低 *CH 2}二聚化的能垒促进 C-C 偶联，有利于 C ₂ H ₄的产生。由于 *CHO 比 *COH 更容易生成，因此推测速率决定步骤是 C-C 偶联，在 *CHO 途径中出现最高势垒能。_{结果提供了对 CO 2}的基本了解铜基表面的还原机理，有利于新型催化剂、合理设计和化学燃料生产。

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Effects of *CO Coverage on Selective Electrocatalytic Reduction of CO2 to Ethylene over Cu2O with Undercoordinated Cu Sites

Cu₂O surface with the coordinatively unsaturated Cu sites reveals advantages in the electroreduction of CO₂ toward C₂H₄ production. Understanding the role of *CO coverage and veritable active sites is of great significance for a good command of the catalytic mechanism. Herein, based on density functional theory, the effects of *CO coverage during the reduction of CO₂ to C₂H₄ on various active sites of Cu₂O(111) surface, in terms of the adsorption and structural changes of *CO and key intermediates; the energy profiles of the C–C coupling steps; and the subsequent reaction mechanisms were investigated. Results show that Cu_CUS on the Cu₂O(111) surface is especially reactive toward the *CO adsorption and subsequent reactions, being the preferred site owing to the unsaturated Cu atoms. The *CO coverage obviously tunes the adsorption stability of *COH and *CHO intermediates by affecting the adsorbent–adsorbent interactions. Higher coverage of *CO within 0.13–0.25 promotes the C–C coupling by lowering the energy barrier of *CH₂ dimerization, favoring the C₂H₄ production. Due to the more facile generation of *CHO than *COH, the rate-determining step is speculated to be the C–C coupling with the highest barrier energy occurring in the *CHO pathway. Results provide a fundamental understanding of the CO₂ reduction mechanism on Cu-based surfaces, favoring novel catalysts, rational design, and chemical fuel production.

更新日期：2022-11-30

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