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null (Ed.)Optical and X-ray spectroscopy studies reveal the location and role of Fe 3+ sites incorporated through direct synthesis in NH 2 -MIL-125(Ti). Fe K-edge XAS analysis confirms its metal–oxo cluster node coordination while time-resolved optical and X-ray transient absorption studies disclose its role as an electron trap site, promoting long-lived photo-induced charge separation in the framework. Notably, XTA measurements show sustained electron reduction of the Fe sites into the microsecond time range. Comparison with an Fe-doped MOF generated through post-synthetic modification indicates that only the direct synthesis approach affords efficient Fe participation in the charge separated excited state.more » « less
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Abstract A major challenge in the pursuit of higher‐energy‐density lithium batteries for carbon‐neutral‐mobility is electrolyte compatibility with a lithium metal electrode. This study demonstrates the robust and stable nature of a
closo ‐borate based gel polymer electrolyte (GPE), which enables outstanding electrochemical stability and capacity retention upon extensive cycling. The GPE developed herein has an ionic conductivity of 7.3 × 10−4 S cm−2at room temperature and stability over a wide temperature range from −35 to 80 °C with a high lithium transference number ( = 0.51). Multinuclear nuclear magnetic resonance and Fourier transform infrared are used to understand the solvation environment and interaction between the GPE components. Density functional theory calculations are leveraged to gain additional insight into the coordination environment and support spectroscopic interpretations. The GPE is also established to be a suitable electrolyte for extended cycling with four different active electrode materials when paired with a lithium metal electrode. The GPE can also be incorporated into a flexible battery that is capable of being cut and still functional. The incorporation of acloso ‐borate into a gel polymer matrix represents a new direction for enhancing the electrochemical and physical properties of this class of materials.
