Angew Chem Int Ed Engl
December 2024
In Li-O batteries (LOBs), the electron transfer between triplet O and singlet LiO possesses a spin-dependent character but is still neglected, while the spin-conserved electron transfer without losing phase information should guarantee fast kinetics and reduced energy barriers. Here, we provide a paradigm of spin-selective catalysis for LOB that the ferromagnetic quantum spin exchange interactions between Pt and Fe atoms in fully-exposed PtFe clusters filter directional e-spins for spin-conserved electron transfer at Fe-Fe sites. The kinetics of O/LiO redox reaction is markedly accelerated as predicted by theoretical calculations, showing dramatically decreased relaxation time of the rate determining step for more than one order of magnitude, compared with the Fe clusters without spin-selective behavior.
View Article and Find Full Text PDFThe application of lithium metal anode in all-solid-state batteries has the potential to achieve both high energy density and safety performance. However, the presence of serious dendrite issues hinders this potential. Here, the ion transport pathways and orientation of dendrite growth are regulated by utilizing the differences of ionic conductivity in heterogeneous electrolytes.
View Article and Find Full Text PDFThe traditional working principle within lithium-ion batteries relies on Li shuttling between the cathode and anode, namely the rocking-chair mechanism. A single working ion constrains the possibilities for battery design and the selection of electrode materials, while realizing multiple working ions offers the potential to break through the fundamental principles of traditional battery construction. Accordingly, it is necessary to develop dual-ion conductors to enable the migration of multiple working ions.
View Article and Find Full Text PDFLi-O battery (LOB) is a promising "beyond Li-ion" technology with ultrahigh theoretical energy density (3457 Wh kg ), while currently impeded by the sluggish cathodic kinetics of the reversible gas-solid reaction between O and Li O . Despite many catalysts are developed for accelerating the conversion process, the lack of design guidance for achieving high performance makes catalysts exploring aleatory. The Sabatier principle is an acknowledged theory connecting the scaling relationship with heterogeneous catalytic activity, providing a tradeoff strategy for the topmost performance.
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