Zhibin Zhou

Single Lithium‐Ion Conducting Polymer Electrolytes Based on a Super‐Delocalized Polyanion

A novel single lithium-ion (Li-ion) conducting polymer electrolyte is presented that is composed of the lithium salt of a polyanion, poly[(4-styrenesulfonyl)(trifluoromethyl(S-trifluoromethylsulfonylimino)sulfonyl)imide] (PSsTFSI(-)), and high-molecular-weight poly(ethylene oxide) (PEO). The neat LiPSsTFSI ionomer displays a low glass-transition temperature (44.3 °C; that is, strongly plasticizing effect). The complex of LiPSsTFSI/PEO exhibits a high Li-ion transference number (tLi (+) =0.91) and is thermally stable up to 300 °C. Meanwhile, it exhibits a Li-ion conductivity as high as 1.35×10(-4)  S cm(-1) at 90 °C, which is comparable to that for the classic ambipolar LiTFSI/PEO SPEs at the same temperature. These outstanding properties of the LiPSsTFSI/PEO blended polymer electrolyte would make it promising as solid polymer electrolytes for Li batteries.

A ceramic/polymer composite solid electrolyte for sodium batteries

Achieving high ionic conductivity in solid electrolytes and reducing the interfacial resistance between solid electrolytes and electrode materials are considered to be one of the biggest challenges in developing solid-state batteries. The integration of the high ionic conductivity of inorganic ceramics and the flexibility of organic polymers was attempted to yield a solvent-free ceramic/polymer composite solid electrolyte for Na batteries for the first time. The composite solid electrolytes exhibit a Na+ ion conductivity as high as 2.4 mS cm−1 at 80 °C. Meanwhile, this composite membrane is thermally stable up to 150 °C and maintains the flexibility of polymer electrolytes. The solid-state Na3V2(PO4)3/CPE/Na battery using this ceramic/polymer composite electrolyte exhibits an initial reversible capacity of 106.1 mA h g−1 and excellent cycle performance with negligible capacity loss over 120 cycles.

Novel Concentrated Li[(FSO2)(n-C4F9SO2)N]-Based Ether Electrolyte for Superior Stability of Metallic Lithium Anode

Lithium (fluorosulfonyl)(n-nonafluorobutanesulfonyl)imide [Li[(FSO2)(n-C4F9SO2)N] (LiFNFSI)] is investigated as a conducting salt, which can form a relatively stable solid-electrolyte-interphase film in concentrated ether electrolyte to achieve favorable protection for lithium metal anodes. Li|Cu and Li|Li cells with concentrated LiFNFSI-based electrolyte have been demonstrated to display high average Coulombic efficiency (≈97%) and excellent cycling stability (over 1,000 h) of metallic lithium anodes, compared to concentrated lithium bis(trifluoromethanesulfonyl)imide [Li[N(SO2CF3)2] (LiTFSI)]-based electrolyte. The morphologies and compositions of the lithium-metal anode surface are also comparatively analyzed by scanning electron microscopy and X-ray photoelectron spectroscopy, respectively. Moreover, superior electrochemical performance in the concentrated LiFNFSI-based electrolyte for Li|LiFePO4 cells is also presented herein. These results indicate that concentrated LiFNFSI-based electrolyte is a promising candidate for metallic lithium rechargeable batteries.

Lithium Bis(fluorosulfonyl)imide/Poly(ethylene oxide) Polymer Electrolyte for All Solid-State Li–S Cell

Solid polymer electrolytes (SPEs) comprising lithium bis(fluorosulfonyl)imide (Li[N(SO2F)2], LiFSI) and poly(ethylene oxide) (PEO) have been studied as electrolyte material and binder for the Li-S polymer cell. The LiFSI-based Li-S all solid polymer cell can deliver high specific discharge capacity of 800 mAh gsulfur-1 (i.e., 320 mAh gcathode-1), high areal capacity of 0.5 mAh cm-2, and relatively good rate capability. The cycling performances of Li-S polymer cell with LiFSI are significantly improved compared with those with conventional LiTFSI (Li[N(SO2CF3)2]) salt in the polymer membrane due to the improved stability of the Li anode/electrolyte interphases formed in the LiFSI-based SPEs. These results suggest that the LiFSI-based SPEs are attractive electrolyte materials for solid-state Li-S batteries.

Impact of the functional group in the polyanion of single lithium-ion conducting polymer electrolytes on the stability of lithium metal electrodes

A novel single lithium-ion (Li-ion) conducting polymer electrolyte composed of lithium poly[(4-styrenesulfonyl)(fluorosulfonyl)imide] (LiPSFSI) and poly(ethylene oxide) (PEO) exhibits a high Li-ion transference number (tLi+ = 0.90) and sufficient electrochemical stability for use in Li batteries. The ionic conductivities of the LiPSFSI/PEO blended polymer electrolytes are higher than those of the lithium poly(4-styrenesulfonate) (LiPSS)/PEO electrolyte and are comparable to those of the lithium poly[(4-styrenesulfonyl)(trifluoromethanesulfonyl)imide] (LiPSTFSI)/PEO electrolyte in the temperature range of 25–90 °C. More importantly, the complex of LiPSFSI/PEO exhibits excellent interfacial compatibility with the Li metal electrode compared to both those of the LiPSS/PEO and LiPSTFSI/PEO electrolytes.

Concentrated dual-salt electrolytes for improving the cycling stability of lithium metal anodes*

Lithium (Li) metal is an ideal anode material for rechargeable Li batteries, due to its high theoretical specific capacity (3860 mAh/g), low density (0.534 g/cm3), and low negative electrochemical potential (−3.040 V vs. standard hydrogen electrode). In this work, the concentrated electrolytes with dual salts, composed of Li[N(SO2F)2] (LiFSI) and Li[N(SO2CF3)2] (LiTFSI) were studied. In this dual-salt system, the capacity retention can even be maintained at 95.7% after 100 cycles in Li|LiFePO4 cells. A Li|Li cell can be cycled at 0.5 mA/cm2 for more than 600 h, and a Li|Cu cell can be cycled at 0.5 mA/cm2 for more than 200 cycles with a high average Coulombi efficiency of 99%. These results show that the concentrated dual-salt electrolytes exhibit superior electrochemical performance and would be a promising candidate for application in rechargeable Li batteries.

A new Na[(FSO2)(n-C4F9SO2)N]-based polymer electrolyte for solid-state sodium batteries

To improve the safety of sodium (Na) batteries, we first report a new solid polymer electrolyte (SPE), composed of sodium (fluorosulfonyl)(n-nonafluorobutanesulfonyl)imide (Na[(FSO2)(n-C4F9SO2)N], NaFNFSI) and poly(ethylene oxide) (PEO), which is prepared by a facile solution-casting method. The NaFNFSI/PEO (EO/Na+ = 15) blended polymer electrolyte exhibits a relatively high ionic conductivity of 3.36 × 10−4 S cm−1 at 80 °C, sufficient thermal stability (>300 °C) and anodic electrochemical stability (≈4.87 V vs. Na+/Na) for application in solid-state Na batteries. Most importantly, the NaFNFSI-based SPE can not only deliver excellent chemical and electrochemical stability with Na metal, but can also display good cycling and current-rate performances for the Na|SPE|NaCu1/9Ni2/9Fe1/3Mn1/3O2 cell. All of these outstanding properties would make the NaFNFSI-based SPE promising as a candidate for application in solid-state Na batteries.