Dataset Information

Origin and Acceleration of Insoluble Li₂ S₂ -Li₂ S Reduction Catalysis in Ferromagnetic Atoms-based Lithium-Sulfur Battery Cathodes.

ABSTRACT: Accelerating insoluble Li₂ S₂ -Li₂ S reduction catalysis to mitigate the shuttle effect has emerged as an innovative paradigm for high-efficient lithium-sulfur battery cathodes, such as single-atom catalysts by offering high-density active sites to realize in situ reaction with solid Li₂ S₂ . However, the profound origin of diverse single-atom species on solid-solid sulfur reduction catalysis and modulation principles remains ambiguous. Here we disclose the fundamental origin of Li₂ S₂ -Li₂ S reduction catalysis in ferromagnetic elements-based single-atom materials to be from their spin density and magnetic moments. The experimental and theoretical studies disclose that the Fe-N₄ -based cathodes exhibit the fastest deposition kinetics of Li₂ S (226 mAh g^-1 ) and the lowest thermodynamic energy barriers (0.56 eV). We believe that the accelerated Li₂ S₂ -Li₂ S reduction catalysis enabled via spin polarization of ferromagnetic atoms provides practical opportunities towards long-life batteries.

SUBMITTER: Yan R

PROVIDER: S-EPMC10107143 | biostudies-literature | 2023 Jan

REPOSITORIES: biostudies-literature

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Publications

Origin and Acceleration of Insoluble Li2 S2 -Li2 S Reduction Catalysis in Ferromagnetic Atoms-based Lithium-Sulfur Battery Cathodes.

Yan Rui R Zhao Zhenyang Z Cheng Menghao M Yang Zhao Z Cheng Chong C Liu Xikui X Yin Bo B Li Shuang S

Angewandte Chemie (International ed. in English) 20221201 1

Accelerating insoluble Li2 S2 -Li2 S reduction catalysis to mitigate the shuttle effect has emerged as an innovative paradigm for high-efficient lithium-sulfur battery cathodes, such as single-atom catalysts by offering high-density active sites to realize in situ reaction with solid Li2 S2 . However, the profound origin of diverse single-atom species on solid-solid sulfur reduction catalysis and modulation principles remains ambiguous. Here ...[more]

PMID: 36321878

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Project description:Metallic contaminants pose a significant challenge to the viability of directly recycling Li-ion batteries. To date, few strategies exist to selectively remove metallic impurities from mixtures of shredded end-of-life material (black mass; BM) without concurrently damaging the structure and electrochemical performance of the target active material. We herein present tailored methods to selectively ionize two major contaminants—Al and Cu—while retaining a representative cathode (LiNi0.33Mn0.33Co0.33O2; NMC-111) intact. This BM purification process is conducted at moderate temperatures in a KOH-based solution matrix. We rationally evaluate approaches to increase both the kinetic corrosion rate and the thermodynamic solubility of Al0 and Cu0, and evaluate the impact of these treatment conditions on the structure, chemistry, and electrochemical performance of NMC. Specifically, we explore the impacts of chloride-based salts, a strong chelating agent, elevated temperature, and sonication on the rate and extent of contaminant corrosion, while concurrently evaluating the effects on NMC. The reported BM purification process is then demonstrated on samples of “simulated BM” containing a practically relevant 1 wt% concentration of Al or Cu. Increasing the kinetic energy of the purifying solution matrix through elevated temperature and sonication accelerates the corrosion of metallic Al and Cu, such that ∼100% corrosion of 75 μm Al and Cu particles is achieved within 2.5 hr. Further, we determine that effective mass transport of ionized species critically impacts the efficacy of Cu corrosion, and that saturated Cl– hinders rather than accelerates Cu corrosion by increasing solution viscosity and introducing competitive pathways for Cu surface passivation. The purification conditions do not induce bulk structural damage to NMC, and electrochemical capacity is maintained in half-cell format. Testing in full cells suggests that a limited quantity of residual surface species are present after treatment, which initially disrupt electrochemical behavior at the graphite anode but are subsequently consumed. Process demonstration on simulated BM suggests that contaminated samples—which prior to treatment show catastrophic electrochemical performance—can be recovered to pristine electrochemical capacity. The reported BM purification method offers a compelling and commercially viable solution to address contamination, particularly in the “fine” fraction of BM where contaminant sizes are on the same order of magnitude as NMC and where traditional separation approaches are unfeasible. Thus, this optimized BM purification technique offers a pathway towards viable direct recycling of BM feedstocks that would otherwise be unusable.

Dataset Information

Origin and Acceleration of Insoluble Li₂ S₂ -Li₂ S Reduction Catalysis in Ferromagnetic Atoms-based Lithium-Sulfur Battery Cathodes.

Publications

Origin and Acceleration of Insoluble Li<sub>2</sub> S<sub>2</sub> -Li<sub>2</sub> S Reduction Catalysis in Ferromagnetic Atoms-based Lithium-Sulfur Battery Cathodes.

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