Novel and promising chloride ion batteries(CIBs)that can operate at room temperature have attracted great attentions,due to the sustainable chloride-containing resources and high theoretical energy density.To achieve ...Novel and promising chloride ion batteries(CIBs)that can operate at room temperature have attracted great attentions,due to the sustainable chloride-containing resources and high theoretical energy density.To achieve the superior electrochemical properties of CIBs,the structure design of electrode materials is essential.Herein,2D NiAl-layered double hydroxide(NiAl-LDH)nanoarrays derived from Al2O3 are in-situ grafted to graphene(G)by atomic layer deposition(ALD)and hydrothermal method.The achieved NiAl-LDH@G hybrids with 2D NiAl-LDH arrays grown perpendicularly on graphene surface,can efficiently prevent the stacking of LDHs and enlarge specific surface area to provide more active sites.The NiAl-LDH@G cathode exhibits a maximum discharge capacity of 223.3 mA h g^(-1)and an excellent reversible capacity of 107 mA h g^(-1)over 500 cycles at 100 mA g^(-1)with a high coulombic efficiency around 96%,whereas pure NiAl-LDH has a discharge capacity of only 48.8 mA h g^(-1)and a coulombic efficiency(CE)of about 78%.More importantly,the NiAl-LDH@G electrode has a stable voltage at 1.9 V and an outstanding discharge capacity of higher than 72 mA h g^(-1)after 120 days.Additionally,XRD,XPS,and EDS have been employed to unveil the electrochemical reaction and Cl-storage mechanism of the NiAlLDH@G cathode in CIBs.This work opens a facile and reasonable way for improving electrochemical performance at anion-type rechargeable batteries in terms of cathode material design and mechanism interpretation.展开更多
The growing demand for substitutes of lithium chemistries in battery leads to a surge in budding novel anion-based electrochemical energy storage,where the chloride ion batteries(CIBs)take over the role.The applicatio...The growing demand for substitutes of lithium chemistries in battery leads to a surge in budding novel anion-based electrochemical energy storage,where the chloride ion batteries(CIBs)take over the role.The application of CIBs is limited by the dissolution and side reaction of chloride-based electrode materials in a liquid electrolyte.On the flipside,its solid-state electrolytes are scarcely reported due to the challenge in realizing fast Cl^(-)conductivity.The present study reports[Al(DMSO)_(6)]Cl_(3),a solid-state metal-organic material,allows chloride ion transfer.The strong Al-Cl bonds in AlCl_(3)are broken down after coordinating of Al^(3+)by ligand DMSO,and Cl^(-)in the resulting compound is weakly bound to complexions[Al(DMSO)_(6)]^(3+),which may facilitate Cl^(-)migration.By partial replacement of Cl^(-)with PF_(6)^(-),the room-temperature ionic conductivity of as-prepared electrolyte is increased by one order of magnitude from 2.172×10^(-5)S cm^(-1)to 2.012×10^(-4)S cm^(-1).When they are assembled with Ag(anode)/Ag-AgCl(cathode)electrode system,reversible electrochemical redox reactions occur on both sides,demonstrating its potential for solid-state chloride ion batteries.The strategy by weakening the bonding interaction using organic ligands between Cl^(-)and central metallic ions may provide new ideas for developing solid chloride-ion conductors.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.22278101,22068010,22168016,and 52365044)the Natural Science Foundation of Hainan Province(Grant Nos.2019RC142 and 519QN176)the Finance Science and Technology Project of Hainan Province(Grant No.ZDYF2020009).
文摘Novel and promising chloride ion batteries(CIBs)that can operate at room temperature have attracted great attentions,due to the sustainable chloride-containing resources and high theoretical energy density.To achieve the superior electrochemical properties of CIBs,the structure design of electrode materials is essential.Herein,2D NiAl-layered double hydroxide(NiAl-LDH)nanoarrays derived from Al2O3 are in-situ grafted to graphene(G)by atomic layer deposition(ALD)and hydrothermal method.The achieved NiAl-LDH@G hybrids with 2D NiAl-LDH arrays grown perpendicularly on graphene surface,can efficiently prevent the stacking of LDHs and enlarge specific surface area to provide more active sites.The NiAl-LDH@G cathode exhibits a maximum discharge capacity of 223.3 mA h g^(-1)and an excellent reversible capacity of 107 mA h g^(-1)over 500 cycles at 100 mA g^(-1)with a high coulombic efficiency around 96%,whereas pure NiAl-LDH has a discharge capacity of only 48.8 mA h g^(-1)and a coulombic efficiency(CE)of about 78%.More importantly,the NiAl-LDH@G electrode has a stable voltage at 1.9 V and an outstanding discharge capacity of higher than 72 mA h g^(-1)after 120 days.Additionally,XRD,XPS,and EDS have been employed to unveil the electrochemical reaction and Cl-storage mechanism of the NiAlLDH@G cathode in CIBs.This work opens a facile and reasonable way for improving electrochemical performance at anion-type rechargeable batteries in terms of cathode material design and mechanism interpretation.
基金supported by the Czech Science Foundation(GACR No.2016124J)supported by the grant of Specific university researchgrant No.A2_FCHT_2022_056
文摘The growing demand for substitutes of lithium chemistries in battery leads to a surge in budding novel anion-based electrochemical energy storage,where the chloride ion batteries(CIBs)take over the role.The application of CIBs is limited by the dissolution and side reaction of chloride-based electrode materials in a liquid electrolyte.On the flipside,its solid-state electrolytes are scarcely reported due to the challenge in realizing fast Cl^(-)conductivity.The present study reports[Al(DMSO)_(6)]Cl_(3),a solid-state metal-organic material,allows chloride ion transfer.The strong Al-Cl bonds in AlCl_(3)are broken down after coordinating of Al^(3+)by ligand DMSO,and Cl^(-)in the resulting compound is weakly bound to complexions[Al(DMSO)_(6)]^(3+),which may facilitate Cl^(-)migration.By partial replacement of Cl^(-)with PF_(6)^(-),the room-temperature ionic conductivity of as-prepared electrolyte is increased by one order of magnitude from 2.172×10^(-5)S cm^(-1)to 2.012×10^(-4)S cm^(-1).When they are assembled with Ag(anode)/Ag-AgCl(cathode)electrode system,reversible electrochemical redox reactions occur on both sides,demonstrating its potential for solid-state chloride ion batteries.The strategy by weakening the bonding interaction using organic ligands between Cl^(-)and central metallic ions may provide new ideas for developing solid chloride-ion conductors.