Orbital Coupling of PbO<sub>7</sub> Node in Single-Crystal Metal-Organic Framework Enhances Li-O<sub>2</sub> Battery Electrocatalysis.
basic_science · Level V
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- Record sourced from PubMed, PMID 37942960.
- Also identified by DOI 10.1021/acs.nanolett.3c03576.
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Abstract
Optimizing the local coordination environment of metal centers in metal-organic frameworks (MOFs) is crucial <i>yet</i> challenging for regulating the overpotential of lithium-oxygen (Li-O<sub>2</sub>) batteries. Herein, we report the synthesis of a class of PbO<sub>7</sub> nodes in a single crystal MOF (naphthalene-lead-MOF, known as Na-Pb-MOF) to significantly enhance the kinetics of both discharge and charge processes. Compared to the PbO<sub>6</sub> node in the single-crystal tetramethoxy-lead-MOF (4OMe-Pb-MOF), the bond length between Pb and O in the PbO<sub>7</sub> node of Na-Pb-MOF increases, resulting in weaker Pb 5d-O 2p orbital coupling, which optimizes the adsorption interaction toward intermediates, and thereby promotes the rate-determining steps of both the reduction of LiO<sub>2</sub> to Li<sub>2</sub>O<sub>2</sub> and the oxidation of LiO<sub>2</sub> to O<sub>2</sub> for reducing the activation energy of the overall reaction. Consequently, Li-O<sub>2</sub> batteries based on Na-Pb-MOF electrocatalysts exhibit a low total charge-discharge overpotential of 0.52 V and an excellent cycle life of 140 cycles.