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Rendering Redox Reactions of Cathodes in Li-Ion Capacitors Enabled by Lanthanides.

ABSTRACT: Capacitors allow extremely fast charge and discharge operations, which is a challenge faced by recent metal-ion batteries despite having highly improved energy densities. Thus, combined type electric energy storage devices that can integrate high energy density and high power density with high potentials, can overcome the shortcomings of the current metal-ion batteries and capacitors. However, the limited capacities of cathode materials owing to the barren redox reactions are regarded as an obstacle for the development of future high-performance hybrid metal-ion capacitors. In this study, we demonstrate the redox-reaction-rendering effect of the much overlooked lanthanide elements when used as the cathode of lithium-ion capacitors using the mesoporous carbon (MC) as a matrix material. Consequently, these lanthanide elements can effectively enrich the redox reaction, thus improving the capacity of the matrix materials by more than two times. Typically, the Gd-elemental decoration of MC surprisingly enhances the capacity by almost two times as compared with the underacted MC. Furthermore, the La nanoparticles (NPs) decoration depicts the same behavior. Evident redox peaks were formed on the original rectangular cyclic voltammetry (CV) curves. This study provides the first example of embedding lanthanide elements on matrix materials to enrich the desired redox reactions for improving the electrochemical performances.

SUBMITTER: Zhang K

PROVIDER: S-EPMC6990622 | biostudies-literature | 2020 Jan

REPOSITORIES: biostudies-literature

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Rendering Redox Reactions of Cathodes in Li-Ion Capacitors Enabled by Lanthanides.

Zhang Kaiqiang K Lee Tae Hyung TH Khalilzadeh Mohammad A MA Varma Rajender S RS Choi Ji-Won JW Jang Ho Won HW Shokouhimehr Mohammadreza M

ACS omega 20200115 3

Capacitors allow extremely fast charge and discharge operations, which is a challenge faced by recent metal-ion batteries despite having highly improved energy densities. Thus, combined type electric energy storage devices that can integrate high energy density and high power density with high potentials, can overcome the shortcomings of the current metal-ion batteries and capacitors. However, the limited capacities of cathode materials owing to the barren redox reactions are regarded as an obst ...[more]

PMID: 32010838

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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

Rendering Redox Reactions of Cathodes in Li-Ion Capacitors Enabled by Lanthanides.

Publications

Rendering Redox Reactions of Cathodes in Li-Ion Capacitors Enabled by Lanthanides.

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