Electron/ion-conductive flexible copolymer PEDOT-PDMS (poly(3,4-ethylenedioxythiophene)-poly(dimethylsiloxane)) was successfully developed, which not only effectively optimizes high-voltage NaLiFePO4F cathode through dripping on electrode surface but also improves high-capacity Si anode through in-situ polymerization on the surface of Si particles. Theoretical calculation and experiments indicate that π-π conjugated structure in PEDOT-PDMS molecular chains easily interacts with PF6– anions, providing electron transfer pathways and preventing HF production. Moreover, Li ions transfer through Si-O in the amorphous phase of the copolymer, and its Young’s modulus at rupture is 1.17±0.10 MPa. The in-situ TEM results directly confirm that the polymer layer provides conducting pathways and buffers the stress induced by lithiation. With the NaLiFePO4F coated cathode, the cells show good cycle stability (~100% of capacity retention after 500 cycles) and high chemical diffusion coefficient of lithium-ions (1.89×10–9 cm2·s–1 and 1.20×10–9 cm2·s–1). In the case of coated Si anode, a capacity of 1512 mAh·g–1 is retained after 1000 cycles at 0.5 C with a capacity retention of 69.8% in terms of the highest specific capacity around the 160th cycle. This work opens a new avenue for the simultaneous optimization of cathode and anode with a functional polymer.
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Zinc-ion hybrid supercapacitors (ZHSCs) have been widely considered as promising candidates for flexible electrochemical energy storage devices. The key challenge is to develop hydrogel electrolytes with high hydrophilicity, anti-freezing, bending resistance, and stable interface with electrodes. This study reported a hydrogel electrolyte system that can meet the above functions, in which the zincophilic and negatively charged SO3−, migratable Na+, abundant hydrophilic functional groups, gum xanthan, and porous architecture could effectively promote the electrochemical performance of ZHSCs. ZHSCs with such hydrogel electrolytes not only exhibited good low-temperature performance but also showed excellent bending resistance ability. A high specific capacitance could be kept after a long air-working lifespan over 10,000 cycles under a wide operation voltage of 1.85 V at −10 ℃. Furthermore, flexible ZHSCs could maintain the capacitance retention of 93.18% even after continuous 500 bends at an angle of 180°. The designed hydrogel electrolytes could be also used for other electrochemical energy storage devices with anti-freezing and bending resistance by changing electrolyte salt.
Since lithium sulfur (Li-S) energy storage devices are anticipated to power portable gadgets and electric vehicles owing to their high energy density (2600 Wh·kg–1); nevertheless, their usefulness is constrained by sluggish sulfur reaction kinetics and soluble lithium polysulfide (LPS) shuttling effects. High electrically conductive bifunctional electrocatalysts are urgently needed for Li-S batteries, and high-entropy oxide (HEO) is one of the most promising electrocatalysts. In this work, we synthesize titanium-containing high entropy oxide (Ti-HEO) (TiFeNiCoMg)O with enhanced electrical conductivity through calcining metal-organic frameworks (MOF) templates at modest temperatures. The resulting single-phase Ti-HEO with high conductivity could facilitate chemical immobilization and rapid bidirectional conversion of LPS. As a result, the Ti-HEO/S/KB cathode (with 70 wt.% of sulfur) achieves an initial discharge capacity as high as ~1375 mAh·g–1 at 0.1 C, and a low-capacity fade rate of 0.056% per cycle over 1000 cycles at 0.5 C. With increased sulfur loading (~5.0 mg·cm–2), the typical Li-S cell delivered a high initial discharge capacity of ~607 mAh·g–1 at 0.2 C and showcased good cycling stability. This work provides better insight into the synthesis of catalytic Ti-containing HEOs with enhanced electrical conductivity, which are effective in simultaneously enhancing the LPS-conversion kinetics and reducing the LPS shuttling effect.
Although VB-Group transition metal disulfides (TMDs) VS2 nanomaterials with specific electronic properties and multiphase microstructures have shown fascinating potential in the field of electromagnetic wave (EMW) absorption, the efficient utilization of VS2 is limited by the technical bottleneck of its narrow effective absorption bandwidth (EAB) which is attributed to environmental instability and a deficient electromagnetic (EM) loss mechanism. In order to fully exploit the maximal utilization values of VS2 nanomaterials for EMW absorption through mitigating the chemical instability and optimizing the EM parameters, biomass-based glucose derived carbon (GDC) like sugar-coating has been decorated on the surface of stacked VS2 nanosheets via a facile hydrothermal method, followed by high-temperature carbonization. As a result, the modulation of doping amount of glucose injection solution (Glucose) could effectively manipulate the encapsulation degree of GDC coating on VS2 nanosheets, further implementing the EM response mechanisms of the VS2/GDC hybrids (coupling effect of conductive loss, interfacial polarization, relaxation, dipole polarization, defect engineering and multiple reflections and absorptions) through regulating the conductivity and constructing multi-interface heterostructures, as reflected by the enhanced EMW absorption performance to a great extent. The minimum reflection loss (Rmin) of VS2/GDC hybrids could reach −52.8 dB with a thickness of 2.7 mm at 12.2 GHz. Surprisingly, compared with pristine VS2, the EAB of the VS2/GDC hybrids increased from 2.0 to 5.7 GHz, while their environmental stability was effectively enhanced by virtue of GDC doping. Obviously, this work provides a promising candidate to realize frequency band tunability of EMW absorbers with exceptional performance and environmental stability.