Recycled Tandem Catalysts Promising Ultralow Overpotential Li‐CO2 Batteries

Abstract

AbstractLithium‐carbon dioxide (Li‐CO2) batteries are regarded as a prospective technology to relieve the pressure of greenhouse emissions but are confronted with sluggish CO2 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 CO2 reduction and evolution reactions (CO2RR and CO2ER) 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 CO2RR and CO2ER, 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‐CO2 batteries.