Electrochemical CO2 reduction reaction (CO2RR) using renewable energy to produce valuable multicarbon (C2+) products is a promising approach for carbon emission reduction. In this work, we propose a new strategy to enhance the formation of hydrogen-containing intermediates using the excellent abilities of proton transportation and electronic structure modification of phosphorus (P). To realize this, an in situ electrodeposition method was proposed to prepare P-doped Cu catalysts. It was found that the electrodeposition potential significantly impacts the structure and catalytic performance of P-Cu catalysts. Specifically, the catalyst obtained at − 0.5 V vs. Ag/AgCl exhibited exceptional performance for CO2RR towards C2+ products, achieving a Faradaic efficiency (FE) of ∼ 80.2 % and a partial current density of 40.4 mA cm−2 in an H-type cell. Furthermore, the catalyst demonstrated stability for at least 12 h. Experimental and density functional theory (DFT) studies revealed that the free energy of the hydrogenated process could be significantly reduced by the excellent proton transport ability of P, and the interaction of Cu with the unpaired electrons of carbon could be improved, leading to excellent adsorption ability of Cu for the intermediates and high FE of C2+ products.

中文翻译：

---

通过磷增强质子供给促进电化学 CO2 还原反应中 C2 产物的形成


利用可再生能源的电化学二氧化碳还原反应（CO2RR）生产有价值的多碳（C2+）产品是一种很有前景的碳减排方法。在这项工作中，我们提出了一种利用磷（P）优异的质子传输和电子结构修饰能力来增强含氢中间体形成的新策略。为了实现这一目标，提出了一种原位电沉积方法来制备P掺杂Cu催化剂。研究发现电沉积电位显着影响P-Cu催化剂的结构和催化性能。具体来说，在− 0.5 V vs. Ag/AgCl 下获得的催化剂对 C2+ 产物表现出优异的 CO2RR 性能，在 H 型中实现了约 80.2 % 的法拉第效率 (FE) 和 40.4 mA cm−2 的部分电流密度细胞。此外，该催化剂表现出至少12小时的稳定性。实验和密度泛函理论（DFT）研究表明，P优异的质子传输能力可以显着降低氢化过程的自由能，并且可以改善Cu与碳不成对电子的相互作用，从而实现优异的吸附Cu 的中间体能力和 C2+ 产品的高 FE。