A Nonaqueous Mg‐CO2 Battery with Low Overpotential

Abstract Mg‐CO 2 batteries, which exploit the greenhouse gas CO 2 as cathode active species, are an appealing next‐generation battery candidate due to their high efficiency energy storage and value‐added CO 2 utilization. However, compared with other metal‐CO 2 systems, few aprotic Mg‐CO 2 batteries have been reported so far as a result of several crucial problems including the comparatively slow redox reaction kinetics, a large decomposition energy barrier of the reduction products, and poor reversibility in their multi‐electron three‐phase cathodic reactions in nonaqueous environments. Herein, a rechargeable Mg‐CO 2 battery is developed by using a Mo 2 C‐CNTs catalytic cathode, a nonaqueous electrolyte, and a magnesium metal anode. The Mo 2 C‐CNTs catalytic cathode can greatly reduce the charge overpotential of the Mg‐CO 2 battery through tuning the CO 2 reduction pathways. The results of a variety of ex situ and in situ experiments as well as theoretical calculations show the Mo 2 C catalyst not only induces surface molecular adsorption for faster reaction kinetics but also improves the selectivity toward MgC 2 O 4 in the CO 2 reduction process for a higher Faraday efficiency. An exceptional low voltage hysteresis is achieved for the Mg‐CO 2 battery. This work demonstrates a promising strategic option for rechargeable nonaqueous Mg‐CO 2 batteries for simultaneously addressing energy and environmental issues.