Lithium-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 (CO2 RR and CO2 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 CO2 RR and CO2 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-CO2 batteries.
Keywords: Li-CO2 batteries; bidirectional catalysts; in-built electric fields; overpotential; spent lithium-ion batteries.
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