Conditioning-free electrolytes with high reversibility of Mg plating/stripping are of vital importance for the commercialization of the superior rechargeable magnesium batteries(RMBs).In the present work,a non-nucleop...Conditioning-free electrolytes with high reversibility of Mg plating/stripping are of vital importance for the commercialization of the superior rechargeable magnesium batteries(RMBs).In the present work,a non-nucleophilic electrolyte(denoted as MLCH)based on all-inorganic salts of MgCl_(2),LiCl and CrCl_(3) for RMBs is prepared by a straightforward one-step reaction.As a result,the MLCH electrolyte shows the noticeable performance of high ionic conductivity(3.40 mS cm^(−1)),low overpotential(∼46 mV vs Mg/Mg^(2+)),high Coulombic efficiency(∼93%),high anodic stability(SS,∼2.56 V vs Mg/Mg^(2+))and long-term(more than 500 h)cycling stability,especially the conditioning-free characteristic.The main equilibrium species in the MLCH electrolyte are confirmed to be the tetracoordinated anions of[LiCl2(THF)2]−and solvated dimers of[Mg_(2)(μ-Cl)3(THF)6]+.The addition of LiCl can assist the dissolution of MgCl_(2) and activation of the electrode/electrolyte interface,resulting in a superior Mg plating/stripping efficiency.The synergistic effect of LiCl,CrCl_(3),a small amount of HpMS and the absence of polymerization THF enable the conditioning-free characteristic of the MLCH electrolyte.Moreover,the MLCH electrolyte exhibits decent compatibility with the cathodic materials of CuS.The Mg/CuS full cell using the MLCH electrolyte presents a discharge specific capacity of 215 mAh g^(−1)at 0.1 C and the capacity can retain∼72%after 40 cycles.Notably,the MLCH electrolyte has other superiorities such as the broad sources of materials,low-cost and easy-preparation,leading to the potential prospect of commercial application.展开更多
Rechargeable magnesium batteries are attractive candidates for energy storage due to their high theoretical specific capacities,free of dendrite formation and natural abundance of magnesium.However,the development of ...Rechargeable magnesium batteries are attractive candidates for energy storage due to their high theoretical specific capacities,free of dendrite formation and natural abundance of magnesium.However,the development of magnesium secondary batteries is severely limited by the lack of high-performance cathode materials and the incompatibility of electrode materials with electrolytes.Herein,we report the application of CuS nanoflower cathode material based on the conversion reaction mechanism for highly reversible magnesium batteries with boosted electrochemical performances by adjusting the compatibility between the cathode and electrolyte.By applying non-nucleophilic electrolytes based on magnesium bis(hexamethyldisilazide)and magnesium chloride dissolved in the mixed solvent of tetrahydrofuran and N-butyl-N-methyl-piperidinium bis((trifluoromethyl)sulfonyl)imide(Mg(HMDS)_(2)-MgCl_(2)/THF-PP14TFSI)or magnesium bis(trifluoromethanesulfonyl)imide,magnesium chloride and aluminium chloride dissolved in dimethoxyethane(Mg(TFSI)2-MgCl_(2)-AlCl_(3)/DME),the magnesium batteries with CuS nanoflower cathode exhibit a high discharge capacity of~207 mAh·g^(–1)at 100 mA·g^(–1)and a long life span of 1,000 cycles at 500 mA·g^(–1).This work suggests that the rational regulation of compatibility between electrode and electrolyte plays a very important role in improving the performance of multi-valent ion secondary batteries.展开更多
Magnesium/sulfur battery(Mg/S)has recently received wide attention due to its high theoretical energy density(3,260 Wh/L)and low cost.To further improve its safety and flexibility,developing a polymer electrolyte that...Magnesium/sulfur battery(Mg/S)has recently received wide attention due to its high theoretical energy density(3,260 Wh/L)and low cost.To further improve its safety and flexibility,developing a polymer electrolyte that can be compatible with both electrophilic S and Mg is critical.Here,we report a magnesium chloride-(fluorinated tetraethylene glycolic)borate(MgCl-FTGB)based non-nucleophilic,gel-type polymer electrolyte for Mg/S battery via a facile synthetic method through commercially available reagents.This electrolyte coupled with glass fiber allows reversible Mg deposition/dissolution(100%coulombic efficiency)with low polarization(500μA/cm^2,300/300 mV),and shows a wide electrochemical window of 4.8 V(vs.Mg/Mg^2+).Mg/S battery assembled with this electrolyte can cycle over 50 times with a high specific discharge capacity retention of over 1,100 mAh/g.展开更多
基金supported by the Science and Technology Research Program of Chongqing Municipal Education Commission(Grant No.KJQN 202103202)the Doctoral Research Foundation of Chongqing Industry Polytechnic College(Grant No.2022GZYBSZK2-11).
文摘Conditioning-free electrolytes with high reversibility of Mg plating/stripping are of vital importance for the commercialization of the superior rechargeable magnesium batteries(RMBs).In the present work,a non-nucleophilic electrolyte(denoted as MLCH)based on all-inorganic salts of MgCl_(2),LiCl and CrCl_(3) for RMBs is prepared by a straightforward one-step reaction.As a result,the MLCH electrolyte shows the noticeable performance of high ionic conductivity(3.40 mS cm^(−1)),low overpotential(∼46 mV vs Mg/Mg^(2+)),high Coulombic efficiency(∼93%),high anodic stability(SS,∼2.56 V vs Mg/Mg^(2+))and long-term(more than 500 h)cycling stability,especially the conditioning-free characteristic.The main equilibrium species in the MLCH electrolyte are confirmed to be the tetracoordinated anions of[LiCl2(THF)2]−and solvated dimers of[Mg_(2)(μ-Cl)3(THF)6]+.The addition of LiCl can assist the dissolution of MgCl_(2) and activation of the electrode/electrolyte interface,resulting in a superior Mg plating/stripping efficiency.The synergistic effect of LiCl,CrCl_(3),a small amount of HpMS and the absence of polymerization THF enable the conditioning-free characteristic of the MLCH electrolyte.Moreover,the MLCH electrolyte exhibits decent compatibility with the cathodic materials of CuS.The Mg/CuS full cell using the MLCH electrolyte presents a discharge specific capacity of 215 mAh g^(−1)at 0.1 C and the capacity can retain∼72%after 40 cycles.Notably,the MLCH electrolyte has other superiorities such as the broad sources of materials,low-cost and easy-preparation,leading to the potential prospect of commercial application.
基金the National Key R&D Program of China(No.2017YFA0208200)the National Natural Science Foundation of China(Nos.22022505 and 21872069)+3 种基金the Fundamental Research Funds for the Central Universities(Nos.020514380266,020514380272,and 020514380274)the Scientific and Technological Innovation Special Fund for Carbon Peak and Carbon Neutrality of Jiangsu Province(BK20220008)the Nanjing International Collaboration Research Program(Nos.202201007 and 2022SX00000955)the 2021 Suzhou Gusu Leading Talents of Science and Technology Innovation and Entrepreneurship in Wujiang District(No.ZXL2021273).
文摘Rechargeable magnesium batteries are attractive candidates for energy storage due to their high theoretical specific capacities,free of dendrite formation and natural abundance of magnesium.However,the development of magnesium secondary batteries is severely limited by the lack of high-performance cathode materials and the incompatibility of electrode materials with electrolytes.Herein,we report the application of CuS nanoflower cathode material based on the conversion reaction mechanism for highly reversible magnesium batteries with boosted electrochemical performances by adjusting the compatibility between the cathode and electrolyte.By applying non-nucleophilic electrolytes based on magnesium bis(hexamethyldisilazide)and magnesium chloride dissolved in the mixed solvent of tetrahydrofuran and N-butyl-N-methyl-piperidinium bis((trifluoromethyl)sulfonyl)imide(Mg(HMDS)_(2)-MgCl_(2)/THF-PP14TFSI)or magnesium bis(trifluoromethanesulfonyl)imide,magnesium chloride and aluminium chloride dissolved in dimethoxyethane(Mg(TFSI)2-MgCl_(2)-AlCl_(3)/DME),the magnesium batteries with CuS nanoflower cathode exhibit a high discharge capacity of~207 mAh·g^(–1)at 100 mA·g^(–1)and a long life span of 1,000 cycles at 500 mA·g^(–1).This work suggests that the rational regulation of compatibility between electrode and electrolyte plays a very important role in improving the performance of multi-valent ion secondary batteries.
基金the National Natural Science Foundation of China(Nos.21433013 and NSFCU1832218)the National Key Research and Development Program of China(No.2016YFB0100100)+2 种基金the International Partnership Program of Chinese Academy of Sciences(Nos.121 E32KYSB20150004)the CAS-Queensland Collaborative Science Fund(No.121E32KYSB20160032)the Users with Excellence Project of Heifei Science Center CAS(No.2018HSC-UE005).
文摘Magnesium/sulfur battery(Mg/S)has recently received wide attention due to its high theoretical energy density(3,260 Wh/L)and low cost.To further improve its safety and flexibility,developing a polymer electrolyte that can be compatible with both electrophilic S and Mg is critical.Here,we report a magnesium chloride-(fluorinated tetraethylene glycolic)borate(MgCl-FTGB)based non-nucleophilic,gel-type polymer electrolyte for Mg/S battery via a facile synthetic method through commercially available reagents.This electrolyte coupled with glass fiber allows reversible Mg deposition/dissolution(100%coulombic efficiency)with low polarization(500μA/cm^2,300/300 mV),and shows a wide electrochemical window of 4.8 V(vs.Mg/Mg^2+).Mg/S battery assembled with this electrolyte can cycle over 50 times with a high specific discharge capacity retention of over 1,100 mAh/g.
