Improving CO2-to-C2+ Product Electroreduction Efficiency via Atomic Lanthanide Dopant-Induced Tensile-Strained CuOx Catalysts,Journal of the American Chemical Society

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Improving CO2-to-C2+ Product Electroreduction Efficiency via Atomic Lanthanide Dopant-Induced Tensile-Strained CuOx Catalysts
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-04-24 , DOI: 10.1021/jacs.3c02428
Jiaqi Feng ₁ , Limin Wu _{1,

2} , Shoujie Liu ₃ , Liang Xu ₁ , Xinning Song _{1,

2} , Libing Zhang _{1,

2} , Qinggong Zhu _{1,

2} , Xinchen Kang _{1,

2} , Xiaofu Sun _{1,

2} , Buxing Han _{1,

2,

4}

Affiliation

Cu is a promising electrocatalyst in CO₂ reduction reaction (CO₂RR) to high-value C₂₊ products. However, as important C–C coupling active sites, the Cu⁺ species is usually unstable under reduction conditions. How atomic dopants affect the performance of Cu-based catalysts is interesting to be studied. Herein, we first calculated the difference between the thermodynamic limiting potentials of CO₂RR and the hydrogen evolution reaction, as well as the *CO binding energy over Cu₂O doped with different metals, and the results indicated that doping atomic Gd into Cu₂O could improve the performance of the catalyst effectively. On the basis of the theoretical study, we designed Gd₁/CuO_x catalysts. The distinctive electronic structure and large ion radii of Gd not only keep the Cu⁺ species stable during the reaction but also induce tensile strain in Gd₁/CuO_x, resulting in excellent performance of the catalysts for electroreduction of CO₂ to C₂₊ products. The Faradic efficiency of C₂₊ products could reach 81.4% with a C₂₊ product partial current density of 444.3 mA cm^–2 at −0.8 V vs a reversible hydrogen electrode. Detailed experimental and theoretical studies revealed that Gd doping enhanced CO₂ activation on the catalyst, stabilized the key intermediate O*CCO, and reduced the energy barrier of the C–C coupling reaction.

中文翻译：

通过原子镧系掺杂剂诱导的拉伸应变 CuOx 催化剂提高 CO2 到 C2+ 产品的电还原效率

Cu 在 CO ₂还原反应 (CO ₂ RR) 到高价值 C ₂₊产品中是一种很有前途的电催化剂。然而，作为重要的 C-C 偶联活性位点，Cu ⁺物种在还原条件下通常不稳定。原子掺杂剂如何影响铜基催化剂的性能值得研究。_{在此，我们首先计算了CO 2} RR和析氢反应的热力学极限电位的差异，以及不同金属掺杂Cu ₂ O上的*CO结合能，结果表明，在Cu _{2中掺杂原子Gd}O可以有效提高催化剂的性能。在理论研究的基础上，我们设计了Gd ₁ /CuO _x催化剂。Gd 独特的电子结构和大离子半径不仅使 Cu ⁺物种在反应过程中保持稳定，而且在 Gd ₁ /CuO _x_{中引起拉伸应变，从而使 CO 2}电还原为 C ₂₊产物的催化剂具有优异的性能. _{C 2+}产品法拉第效率可达81.4%，C ₂₊产品分电流密度为444.3 mA cm ^–2在-0.8 V vs 可逆氢电极。详细的实验和理论研究表明，Gd 掺杂增强了催化剂上的CO _{2活化，稳定了关键中间体 O*CCO，并降低了 C-C 偶联反应的能垒。}

更新日期：2023-04-24

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