p–d Orbital Hybridization Induced by p-Block Metal-Doped Cu Promotes the Formation of C2+ Products in Ampere-Level CO2 Electroreduction,Journal of the American Chemical Society

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p–d Orbital Hybridization Induced by p-Block Metal-Doped Cu Promotes the Formation of C2+ Products in Ampere-Level CO2 Electroreduction
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-02-17 , DOI: 10.1021/jacs.2c12743
Pengsong Li _{1,

2} , Jiahui Bi _{1,

2} , Jiyuan Liu _{1,

2} , Yong Wang _{1,

2} , Xinchen Kang _{1,

2} , Xiaofu Sun _{1,

2} , Jianling Zhang _{1,

2} , Zhimin Liu _{1,

2} , Qinggong Zhu _{1,

2} , Buxing Han _{1,

2,

3}

Affiliation

Large-current electrolysis of CO₂ to multi-carbon (C₂₊) products is critical to realize the industrial application of CO₂ conversion. However, the poor binding strength of *CO intermediates on the catalyst surface induces multiple competing pathways, which hinder the C₂₊ production. Herein, we report that p–d orbital hybridization induced by Ga-doped Cu (CuGa) could promote efficient CO₂ electrocatalysis to C₂₊ products at ampere-level current density. It was found that CuGa exhibited the highest C₂₊ productivity with a remarkable Faradaic efficiency (FE) of 81.5% at a current density of 0.9 A/cm², and the potential at such a high current density was −1.07 V versus reversible hydrogen electrode. At 1.1 A/cm², the catalyst still maintained a high C₂₊ productivity with an FE of 76.9%. Experimental and theoretical studies indicated that the excellent performance of CuGa results from the p–d hybridization of Cu and Ga, which not only enriches reactive sites but also enhances the binding strength of the *CO intermediate and facilitates C–C coupling. The p–d hybridization strategy can be extended to other p-block metal-doped Cu catalysts, such as CuAl and CuGe, to boost CO₂ electroreduction for C₂₊ production. As far as we know, this is the first work to promote electrochemical CO₂ reduction reaction to generate the C₂₊ product by p–d orbital hybridization interaction using a p-block metal-doped Cu catalyst.

中文翻译：

p-嵌段金属掺杂 Cu 诱导的 p-d 轨道杂化促进安培级 CO2 电还原中 C2+ 产物的形成

_{CO 2}大电流电解制多碳（C ₂₊）产品是实现CO ₂转化工业应用的关键。然而，*CO中间体在催化剂表面的结合强度较差，导致了多种竞争途径，阻碍了C ₂₊的产生。在此，我们报告了由 Ga 掺杂的 Cu (CuGa) 诱导的 p-d 轨道杂化可以在安培级电流密度下促进高效的 CO ₂电催化生成 C _2+产物。结果发现，CuGa在 0.9 A/cm ^{2的电流密度下表现出最高的 C}_{2+生产率和 81.5% 的显着法拉第效率 (FE)}，并且在如此高的电流密度下的电位相对于可逆氢电极为-1.07 V。在 1.1 A/cm ²时，催化剂仍保持较高的 C ₂₊生产率，FE 为 76.9%。实验和理论研究表明，CuGa 的优异性能源于 Cu 和 Ga 的 p-d 杂化，这不仅丰富了反应位点，而且增强了 *CO 中间体的结合强度，促进了 C-C 偶联。p-d 杂化策略可以扩展到其他 p 嵌段金属掺杂 Cu 催化剂，例如 CuAl 和 CuGe，以促进 CO ₂电还原以生产 C ₂₊。据我们所知，这是第一个促进电化学CO _2的工作使用 p 嵌段金属掺杂 Cu 催化剂通过 p–d 轨道杂化相互作用生成 C _{2+产物的还原反应。}

更新日期：2023-02-17

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