Rechargeable aqueous aluminum batteries(AABs)with high energy-to-price ratios,abundant element reserves,and intrinsic safety are promising candidates for large-scale energy storage.However,the inherent hydrogen evolut...Rechargeable aqueous aluminum batteries(AABs)with high energy-to-price ratios,abundant element reserves,and intrinsic safety are promising candidates for large-scale energy storage.However,the inherent hydrogen evolution reaction(HER)of aluminum(Al)metal anode with inferior kinetics irreversibly hinders their practical implementation.Herein,we propose,for the first time,a double interfacial layer on the Al anode with drastically reduced HER and accelerated kinetics for AABs.Benefiting from the large band gap of the dual-interfacial layer(integration of Sn and SnS(SS-Al)),the stable voltage window of the electrolyte is remarkably expanded with the potential negatively shifting from−2.34 to−2.98 V at−5.0 mA/cm^(2).Fur-thermore,the synergistic effect from both the SnS outer layer(lower desolvation energy barrier)and the Sn interlayer with improved aluminumophilic properties contributes to accelerated kinetics.Consequently,the optimized SS-Al electrode main-tains one of the best long-term stability among interface-modified Al anodes(more than 700 h at 0.05 mA/cm^(2)with a low initial overpotential of 50.0 mV)in symmetric batteries.Practically,the large-size full-cell prototypes deliver high performance over 1,000 cycles at 1.0 A/g.Overall,this novel interface modification strategy provides a promising pathway for the anode devel-opment in AABs.展开更多
Organic electrode materials with renewability,environmental benignity,and structural tunability have attracted increasing attention for lithium-ion batteries,but their practical application is hindered by low mass loa...Organic electrode materials with renewability,environmental benignity,and structural tunability have attracted increasing attention for lithium-ion batteries,but their practical application is hindered by low mass loadings(<2 mg cm^(-2))and inadequate areal capacities(<0.5 mAh cm^(-2)),primarily due to low electronic conductivity and sluggish ion diffusion.Here,we address these limitations by introducing a scalable spray-drying method to synthesize hierarchical organic/carbon composites.By using lithium terephthalate(Li_(2)TP),carbon nanotubes(CNTs),and polyvinylpyrrolidone as precursors,we fabricate Li_(2)TP-H,a composite featuring Li_(2)TP nanoparticles(~20 nm)assembled into microspheres with 3D CNTs networks.This hierarchical design ensures efficient ion and electron transport,yielding a high capacity retention of 91.6%(from 298 to 273 mAh g^(-1))when increasing mass loading from 2 to 43 mg cm^(-2).The resulting areal capacity of 11.7 mAh cm^(-2)ranks among the highest reported for organic electrodes.Moreover,the methodology is extendable to other carboxylate-based compounds,with all derivatives exhibiting enhanced performance under a high-mass-loading of 10 mg cm^(-2).This work provides a new paradigm for developing high-areal-capacity organic electrodes,representing a pivotal step toward commercializing organic battery technologies.展开更多
基金supported by the National Natural Science Foundation of China(52374295)the National Key Research and Development Program of China(2022YFB2402400).
文摘Rechargeable aqueous aluminum batteries(AABs)with high energy-to-price ratios,abundant element reserves,and intrinsic safety are promising candidates for large-scale energy storage.However,the inherent hydrogen evolution reaction(HER)of aluminum(Al)metal anode with inferior kinetics irreversibly hinders their practical implementation.Herein,we propose,for the first time,a double interfacial layer on the Al anode with drastically reduced HER and accelerated kinetics for AABs.Benefiting from the large band gap of the dual-interfacial layer(integration of Sn and SnS(SS-Al)),the stable voltage window of the electrolyte is remarkably expanded with the potential negatively shifting from−2.34 to−2.98 V at−5.0 mA/cm^(2).Fur-thermore,the synergistic effect from both the SnS outer layer(lower desolvation energy barrier)and the Sn interlayer with improved aluminumophilic properties contributes to accelerated kinetics.Consequently,the optimized SS-Al electrode main-tains one of the best long-term stability among interface-modified Al anodes(more than 700 h at 0.05 mA/cm^(2)with a low initial overpotential of 50.0 mV)in symmetric batteries.Practically,the large-size full-cell prototypes deliver high performance over 1,000 cycles at 1.0 A/g.Overall,this novel interface modification strategy provides a promising pathway for the anode devel-opment in AABs.
文摘Organic electrode materials with renewability,environmental benignity,and structural tunability have attracted increasing attention for lithium-ion batteries,but their practical application is hindered by low mass loadings(<2 mg cm^(-2))and inadequate areal capacities(<0.5 mAh cm^(-2)),primarily due to low electronic conductivity and sluggish ion diffusion.Here,we address these limitations by introducing a scalable spray-drying method to synthesize hierarchical organic/carbon composites.By using lithium terephthalate(Li_(2)TP),carbon nanotubes(CNTs),and polyvinylpyrrolidone as precursors,we fabricate Li_(2)TP-H,a composite featuring Li_(2)TP nanoparticles(~20 nm)assembled into microspheres with 3D CNTs networks.This hierarchical design ensures efficient ion and electron transport,yielding a high capacity retention of 91.6%(from 298 to 273 mAh g^(-1))when increasing mass loading from 2 to 43 mg cm^(-2).The resulting areal capacity of 11.7 mAh cm^(-2)ranks among the highest reported for organic electrodes.Moreover,the methodology is extendable to other carboxylate-based compounds,with all derivatives exhibiting enhanced performance under a high-mass-loading of 10 mg cm^(-2).This work provides a new paradigm for developing high-areal-capacity organic electrodes,representing a pivotal step toward commercializing organic battery technologies.
