Recycled Tandem Catalysts Promising Ultralow Overpotential Li‐CO2 Batteries

Abstract Lithium‐carbon dioxide (Li‐CO 2 ) batteries are regarded as a prospective technology to relieve the pressure of greenhouse emissions but are confronted with sluggish CO 2 redox kinetics and low energy efficiency. Developing highly efficient and low‐cost catalysts to boost bidirectional activities is craved but remains a huge challenge. Herein, derived from the spent lithium‐ion batteries, a tandem catalyst is subtly synthesized and significantly accelerates the CO 2 reduction and evolution reactions (CO 2 RR and CO 2 ER) kinetics with an in‐built electric field (BEF). Combining with the theoretical calculations and advanced characterization techniques, this work reveals that the designed interface‐induced BEF regulates the adsorption/decomposition of the intermediates during CO 2 RR and CO 2 ER, endowing the recycled tandem catalyst with excellent bidirectional activities. As a result, the spent electronics‐derived tandem catalyst exhibits remarkable bidirectional catalytic performance, such as an ultralow voltage gap of 0.26 V and an ultrahigh energy efficiency of 92.4%. Profoundly, this work affords new opportunities to fabricate low‐cost electrocatalysts from recycled spent electronics and inspires fresh perceptions of interfacial regulation including but not limited to BEF to engineer better Li‐CO 2 batteries.