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Abstract This study presents a novel polymer‐in‐salt (PIS) zwitterionic polyurethane‐based solid polymer electrolyte (zPU‐SPE) that offers high ionic conductivity, strong interaction with electrodes, and excellent mechanical and electrochemical stabilities, making it promising for high‐performance all solid‐state lithium batteries (ASSLBs). The zPU‐SPE exhibits remarkable lithium‐ion (Li⁺) conductivity (3.7 × 10⁻⁴ S cm⁻¹at 25 °C), enabled by exceptionally high salt loading of up to 90 wt.% (12.6 molar ratio of Li salt to polymer unit) without phase separation. It addresses the limitations of conventional SPEs by combining high ionic conductivity with a Li⁺transference number of 0.44, achieved through the incorporation of zwitterionic groups that enhance ion dissociation and transport. The high surface energy (338.4 J m⁻²) and elasticity ensure excellent adhesion to Li anodes, reducing interfacial resistance and ensuring uniform Li⁺flux. When tested in Li||zPU||LiFePO₄ and Li||zPU||S/C cells, the zPU‐SPE demonstrated remarkable cycling stability, retaining 76% capacity after 2000 cycles with the LiFePO₄cathode, and achieving 84% capacity retention after 300 cycles with the S/C cathode. Molecular simulations and a range of experimental characterizations confirm the superior structural organization of the zPU matrix, contributing to its outstanding electrochemical performance. The findings strongly suggest that zPU‐SPE is a promising candidate for next‐generation ASSLBs. 

Abstract A gas‐phase approach to form Zn coordination sites on metal–organic frameworks (MOFs) by vapor‐phase infiltration (VPI) was developed. Compared to Zn sites synthesized by the solution‐phase method, VPI samples revealed approximately 2.8 % internal strain. Faradaic efficiency towards conversion of CO₂to CO was enhanced by up to a factor of four, and the initial potential was positively shifted by 200–300 mV. Using element‐specific X‐ray absorption spectroscopy, the local coordination environment of the Zn center was determined to have square‐pyramidal geometry with four Zn−N bonds in the equatorial plane and one Zn‐OH₂bond in the axial plane. The fine‐tuned internal strain was further supported by monitoring changes in XRD and UV/Visible absorption spectra across a range of infiltration cycles. The ability to use internal strain to increase catalytic activity of MOFs suggests that applying this strategy will enhance intrinsic catalytic capabilities of a variety of porous materials. 

Abstract A gas‐phase approach to form Zn coordination sites on metal–organic frameworks (MOFs) by vapor‐phase infiltration (VPI) was developed. Compared to Zn sites synthesized by the solution‐phase method, VPI samples revealed approximately 2.8 % internal strain. Faradaic efficiency towards conversion of CO₂to CO was enhanced by up to a factor of four, and the initial potential was positively shifted by 200–300 mV. Using element‐specific X‐ray absorption spectroscopy, the local coordination environment of the Zn center was determined to have square‐pyramidal geometry with four Zn−N bonds in the equatorial plane and one Zn‐OH₂bond in the axial plane. The fine‐tuned internal strain was further supported by monitoring changes in XRD and UV/Visible absorption spectra across a range of infiltration cycles. The ability to use internal strain to increase catalytic activity of MOFs suggests that applying this strategy will enhance intrinsic catalytic capabilities of a variety of porous materials.