Current inorganic solid electrolyte membranes generally suffer thick thickness of hundreds micrometers as well as low ionic conductivity,which limits the energy density and cycle life of all-solid-state lithium batter...Current inorganic solid electrolyte membranes generally suffer thick thickness of hundreds micrometers as well as low ionic conductivity,which limits the energy density and cycle life of all-solid-state lithium batteries.In this work,wet coating is employed to fabricate the Li_(6)PS_(5)Cl solid electrolyte thin membrane.The interaction among solvents containing different functional groups with the Li_(6)PS_(5)Cl electrolyte was explored.A new polymeric binder is synthesized by polymerization of dimethyl aminoethyl methacrylate(DMAEMA),polyethylene glycol diacrylate(PEGDA),and lithium bis(trifluoromethanesulfonyl)imide(LiTFSI),showing excellent stability to Li_(6)PS_(5)Cl solid electrolyte particles and high tensile strength of 1.46 MPa.Thus,a 40-μm-thick freestanding Li_(6)PS_(5)Cl membrane with 90 wt%Li_(6)PS_(5)Cl content is realized through in situ photo-polymerization,possessing a relatively high room temperature ionic conductivity of 1.23 mS cm^(−1).Moreover,the all-solid-state battery-based Li_(6)PS_(5)Cl membrane exhibits superior cycling stability after 1,000 cycles with a capacity retention of 76.92%at 0.2 C under 60℃.When the mass load of the active material LiCoO_(2) increases to 15.2 mg cm^(−2),the all-solid-state cell still delivers a high initial discharge capacity of 123.0 mAh g^(−1)(1.87 mAh cm^(−2))with a capacity retention rate of 89.93%after 200 cycles.展开更多
Ultrathin zeolite membranes are of paramount importance in accelerating gas transport during membrane separation,and lowering down their membrane thicknesses to submicron scale is deemed to be very challenging.Herein,...Ultrathin zeolite membranes are of paramount importance in accelerating gas transport during membrane separation,and lowering down their membrane thicknesses to submicron scale is deemed to be very challenging.Herein,we develop an advanced approach of surface gel conversion for synthesis of submicron-thick pure silica MFI(silicalite-1)zeolite membranes.Viscous gel is prepared by finely adjusting the precursor composition,enabling its reduced wettability.The unfavorable wetting of the support surface can effectively prevent gel penetration into alumina support voids.Aided by the seeds,the surface gel is directly and fully crystallized into an MFI zeolite membrane with minimal water steam.A membrane with a thickness of 500 nm is successfully acquired and it is free of visible cracks.Additionally,the as-synthesized membranes exhibit rapid and selective separation of hexane isomers by virtue of unprecedentedly high n-hexane permeance of 24.5×10^−7 mol m^−2 s^−1 Pa^−1 and impressive separation factors of 13.3-22.6 for n-hexane over its isomers.This developed approach is of practical interest for sustainable synthesis of high-quality zeolite membranes.展开更多
基金supported by the National Key R&D Program of China(grant no.2022YFB3807700)National Natural Science Foundation of China(grant nos.22309194 and 52372244)+4 种基金Ningbo S&T Innovation 2025 Major Special Programme(grant nos.2021Z122 and 2023Z106)Zhejiang Provincial Key R&D Program of China(grant no.2022C01072)Jiangsu Provincial S&T Innovation Special Programme for carbon peak and carbon neutrality(grant no.BE2022007)Baima Lake Laboratory Joint Funds of the Zhejiang Provincial Natural Science Foundation of China(LBMHD24E020001)Youth Innovation Promotion Association CAS(Y2021080).
文摘Current inorganic solid electrolyte membranes generally suffer thick thickness of hundreds micrometers as well as low ionic conductivity,which limits the energy density and cycle life of all-solid-state lithium batteries.In this work,wet coating is employed to fabricate the Li_(6)PS_(5)Cl solid electrolyte thin membrane.The interaction among solvents containing different functional groups with the Li_(6)PS_(5)Cl electrolyte was explored.A new polymeric binder is synthesized by polymerization of dimethyl aminoethyl methacrylate(DMAEMA),polyethylene glycol diacrylate(PEGDA),and lithium bis(trifluoromethanesulfonyl)imide(LiTFSI),showing excellent stability to Li_(6)PS_(5)Cl solid electrolyte particles and high tensile strength of 1.46 MPa.Thus,a 40-μm-thick freestanding Li_(6)PS_(5)Cl membrane with 90 wt%Li_(6)PS_(5)Cl content is realized through in situ photo-polymerization,possessing a relatively high room temperature ionic conductivity of 1.23 mS cm^(−1).Moreover,the all-solid-state battery-based Li_(6)PS_(5)Cl membrane exhibits superior cycling stability after 1,000 cycles with a capacity retention of 76.92%at 0.2 C under 60℃.When the mass load of the active material LiCoO_(2) increases to 15.2 mg cm^(−2),the all-solid-state cell still delivers a high initial discharge capacity of 123.0 mAh g^(−1)(1.87 mAh cm^(−2))with a capacity retention rate of 89.93%after 200 cycles.
基金the National Natural Science Foundation of China(21531003,21501024 and 21971035)Jilin Scientific and Technological Development Program(20170101198JC and 20190103017JH)+2 种基金Jilin Education Office(JJKH20180015KJ)“111”Program(B18012)open projects from the State Key Laboratory of Inorganic Synthesis&Preparative Chemistry and State Key Laboratory of Heavy Oil Processing(2018-8,SKLOP201902003)。
文摘Ultrathin zeolite membranes are of paramount importance in accelerating gas transport during membrane separation,and lowering down their membrane thicknesses to submicron scale is deemed to be very challenging.Herein,we develop an advanced approach of surface gel conversion for synthesis of submicron-thick pure silica MFI(silicalite-1)zeolite membranes.Viscous gel is prepared by finely adjusting the precursor composition,enabling its reduced wettability.The unfavorable wetting of the support surface can effectively prevent gel penetration into alumina support voids.Aided by the seeds,the surface gel is directly and fully crystallized into an MFI zeolite membrane with minimal water steam.A membrane with a thickness of 500 nm is successfully acquired and it is free of visible cracks.Additionally,the as-synthesized membranes exhibit rapid and selective separation of hexane isomers by virtue of unprecedentedly high n-hexane permeance of 24.5×10^−7 mol m^−2 s^−1 Pa^−1 and impressive separation factors of 13.3-22.6 for n-hexane over its isomers.This developed approach is of practical interest for sustainable synthesis of high-quality zeolite membranes.
