Theory-Guided Design of Unconventional Phase Metal Heteronanostructures for Higher-Rate Stable Li-CO2 and Li-Air Batteries.

Lithium-carbon dioxide (Li-CO2) and Li-air batteries hold great potential in achieving carbon neutral given their ultrahigh theoretical energy density and eco-friendly features. However, these Li-gas batteries still suffer from low discharging-charging rate and poor cycling life due to sluggish decomposition kinetics of discharge products especially Li2CO3. Here we report the theory-guided design and preparation of unconventional phase metal heteronanostructures as cathode catalysts for high-performance Li-CO2/air batteries. The assembled Li-CO2 cells with unconventional phase 4H/face-centered cubic (fcc) ruthenium-nickel heteronanostructures deliver a narrow discharge-charge gap of 0.65 V, excellent rate capability and long-term cycling stability over 200 cycles at 250 mA g-1. The constructed Li-air batteries can steadily run for above 150 cycles in ambient air. Electrochemical mechanism studies reveal that 4H/fcc Ru-Ni with high-electroactivity facets can boost redox reaction kinetics and tune discharge reactions towards Li2C2O4 path, alleviating electrolyte/catalyst failures induced by the aggressive singlet oxygen from solo decomposition of Li2CO3.

Zhou J ，Xu Z ，Cui K ，Yin JA ，Chen HC ，Wang Y ，Liu F ，Wang T ，Hao F ，Xiong Y ，Wang C ，Ma Y ，Lu P ，Yin J ，Guo L ，Meng X ，Ye C ，Chen HM ，Zhu Y ，Lu J ，Fan Z ... -  《-》

Boosting the reaction kinetics in aprotic lithium-carbon dioxide batteries with unconventional phase metal nanomaterials.

Zhou J ，Wang T ，Chen L ，Liao L ，Wang Y ，Xi S ，Chen B ，Lin T ，Zhang Q ，Ye C ，Zhou X ，Guan Z ，Zhai L ，He Z ，Wang G ，Wang J ，Yu J ，Ma Y ，Lu P ，Xiong Y ，Lu S ，Chen Y ，Wang B ，Lee CS ，Cheng J ，Gu L ，Zhao T ，Fan Z ... -  《-》

Understanding the Dual-Phase Synergy Mechanism in Mn(2)O(3)-Mn(3)O(4) Catalyst for Efficient Li-CO(2) Batteries.

Liu L ，Zhang L ，Wang K ，Wu H ，Mao H ，Li L ，Sun Z ，Lu S ，Zhang D ，Yu W ，Ding S ... -  《-》

Cationic metal-organic framework derived ruthenium-copper nano-alloys in porous carbon to catalytically boost the cycle life of Li-CO(2) batteries.

Cheng Z ，Wu Z ，Tang Y ，Fan X ，Zhang J ，Chen Y ，Xiang S ，Zhang Z ... -  《-》

MOF-Derived CoSe(2) Nanoparticles/Carbonized Melamine Foam as Catalytic Cathode Enabling Flexible Li-CO(2) Batteries with High Energy Efficiency and Stable Cycling.

Rechargeable aprotic Li-CO2 batteries have aroused worldwide interest owing to their environmentally friendly CO2 fixation ability and ultra-high specific energy density. However, its practical applications are impeded by the sluggish reaction kinetics and discharge product accumulation during cycling. Herein, a flexible composite electrode comprising CoSe2 nanoparticles embedded in 3D carbonized melamine foam (CoSe2/CMF) for Li-CO2 batteries is reported. The abundant CoSe2 clusters can not only facilitate CO2 reduction/evolution kinetics but also serve as Li2CO3 nucleation sites for homogeneous discharge product growth. The CoSe2/CMF-based Li-CO2 battery exhibits a large initial discharge capacity as high as 5.62 mAh cm-2 at 0.05 mA cm-2, a remarkably small voltage gap of 0.72 V, and an ultrahigh energy efficiency of 85.9% at 0.01 mA cm-2, surpassing most of the noble metal-based catalysts. Meanwhile, the battery demonstrates excellent cycling stability of 1620 h (162 cycles) at 0.02 mA cm-2 with an average overpotential of 0.98 V and energy efficiency of 85.4%. Theoretical investigations suggest that this outstanding performance is attributed to the suitable CO2/Li adsorption and low Li2CO3 decomposition energy. Moreover, flexible Li-CO2 pouch cell with CoSe2/CMF cathode displays stable power output under different bending deformations, showing promising potential in wearable electronic devices.

Wang K ，Liu L ，Liu D ，Wei Y ，Liu Y ，Wang X ，Vasenko AS ，Li M ，Ding S ，Xiao C ，Pan H ... -  《-》