Electron Penetration Effect of Ni Single Atom Boosting CO2 to CO in PH-Universal Electrolytes

Electrocatalytic CO2 reduction (ECR) powered by renewable electricity has attracted of wide attention because of its advantages to produce high-value-added chemicals and fuels. Additionally, ECR played a crucial role in addressing the challenge of excessive fossil fuel consumption caused by global warming. Herein, a unique armor structure with Ni nanoparticles coated by a carbon shell containing Ni & horbar;N & horbar;C (Ni & horbar;NP@Ni & horbar;SA) for industrial ECR to CO in pH-universal electrolytes is designed. Ni & horbar;NP@Ni & horbar;SA catalyst exhibits approximate to 100% CO Faradaic efficiency, and CO partial current density can reach 500, 361, and 615 mA cm(-2) in strong alkaline (pH 14), neutral (pH 7.2) and strong acidic (pH 1) electrolytes, respectively. Moreover, Ni & horbar;NP@Ni & horbar;SA can drive the rechargeable Zn-CO2 battery with a high power density of 3.45 mW cm(-2), and outstanding stability over 36 h. The structural characterizations and theoretical calculation together present that the electron penetration effect of Ni & horbar;NP@Ni & horbar;SA can strengthen the electronic enrichment state of Ni single atom, which facilitates the reaction kinetics of ECR by decreasing the formation energy barrier of key intermediate *COOH. This work pioneers a new design strategy to enhance the activity of single-atom catalysts and seek high-efficiency electrocatalysts for ECR in pH-universal electrolytes.