The rational design of a 3D scaffold with optimized electrical conductivity,sodiophilicity,and sufficient internal space is crucial for suppressing the growth of Na dendrites and accommodating the large volume changes...The rational design of a 3D scaffold with optimized electrical conductivity,sodiophilicity,and sufficient internal space is crucial for suppressing the growth of Na dendrites and accommodating the large volume changes of Na metal anodes during the plating/stripping process.Nevertheless,the uniform conductivity and sodiophilicity of conventional scaffolds often lead to Na metal deposition on the top of the scaffold,thereby hindering the complete functional capabilities of the scaffold.To tackle this challenge,we developed a novel imprinted dual-gradient 3D network skeleton that boasts gradients in both sodiophilicity and conductivity.Both theoretical and experimental analyses indicate that Na metal prefers to nucleate and deposit dendrite-free from the bottom of the 3D skeleton due to its superior conductivity and sodiophilicity.This dual-gradient design enables the electrode to achieve low nucleation overpotential of 11 mV and sustain stable operation for 1900 h at 1.5 m A cm^(-2) /1.5 mAh cm^(-2) and1000 h at 20 mA cm^(-2) /20 mAh cm^(-2) ,far superior to the gradientless electrode.When paired with Na_(3)V_(2) (PO_(4))_(3) cathode,the full cell retains a capacity of 67.6 mAh g^(-1) after 1000 stable cycles with a capacity retention rate of 82.4%at a rate of 10 C.This advanced skeleton structure design is poised to advance the development of high-energy-density alkali metal batteries.展开更多
基金supported by the National Natural Science Foundation of China(22209140,52202286)the Qingchuang Technology Support Program of the University in Shandong Province(2024KJH080)+6 种基金the Natural Science Foundation of Shandong Province(ZR2022QE059,ZR2024MB153)the Shandong Laboratory of Advanced Materials and Green Manufacturing at Yantai(Yantai)(AMGM2023A08)the Natural Science Foundation of Zhejiang Province(LQ23B030011,LY24B030006)the Scientific Research Fund of Zhejiang Provincial Education Department(Y202148249)the Science and Technology Plan Project of Wenzhou Municipality(ZG2024055,ZG2022032)the Wenzhou Association for Science and Technology Innovation Program(NLTS2024-013)the Natural Science Foundation of Guangdong Province-Youth Promotion Project(2024A1515030173)。
文摘The rational design of a 3D scaffold with optimized electrical conductivity,sodiophilicity,and sufficient internal space is crucial for suppressing the growth of Na dendrites and accommodating the large volume changes of Na metal anodes during the plating/stripping process.Nevertheless,the uniform conductivity and sodiophilicity of conventional scaffolds often lead to Na metal deposition on the top of the scaffold,thereby hindering the complete functional capabilities of the scaffold.To tackle this challenge,we developed a novel imprinted dual-gradient 3D network skeleton that boasts gradients in both sodiophilicity and conductivity.Both theoretical and experimental analyses indicate that Na metal prefers to nucleate and deposit dendrite-free from the bottom of the 3D skeleton due to its superior conductivity and sodiophilicity.This dual-gradient design enables the electrode to achieve low nucleation overpotential of 11 mV and sustain stable operation for 1900 h at 1.5 m A cm^(-2) /1.5 mAh cm^(-2) and1000 h at 20 mA cm^(-2) /20 mAh cm^(-2) ,far superior to the gradientless electrode.When paired with Na_(3)V_(2) (PO_(4))_(3) cathode,the full cell retains a capacity of 67.6 mAh g^(-1) after 1000 stable cycles with a capacity retention rate of 82.4%at a rate of 10 C.This advanced skeleton structure design is poised to advance the development of high-energy-density alkali metal batteries.