Abstract
Aqueous Zn-CO2 batteries can not only convert CO2 into high-value chemicals but also store/output electric energy for external use. However, their performance is limited by sluggish and complicated CO2 electroreduction at the cathode. Herein, a dual-anion regulated Bi electrocatalyst is developed to selectively reduce CO2 to formate with a Faradaic efficiency of up to 97% at a large current density of 250mAcm-2. With O and/or F, the rate-determine step of CO2 electroreduction has been manipulated (from the first hydrogenation to *HCOOH desorption step) with a reduced energy barrier. Significantly, the fabricated Zn-CO2 battery exhibits a high discharge voltage of 1.2V, optimal power density of 4.51mWcm-2, remarkable energy density of 802Whkg-1, and energy-conversion efficiency of 70.74%, stability up to 200 cycles and 68h. This study provides possible strategies to fabricate reversible and energetic aqueous Zn-CO2 batteries by addressing cathodic problems.
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