Browsing by Author "Chen, Jinhang"

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    Battery metal recycling by flash Joule heating
    (AAAS, 2023) Chen, Weiyin; Chen, Jinhang; Bets, Ksenia V.; Salvatierra, Rodrigo V.; Wyss, Kevin M.; Gao, Guanhui; Choi, Chi Hun; Deng, Bing; Wang, Xin; Li, John Tianci; Kittrell, Carter; La, Nghi; Eddy, Lucas; Scotland, Phelecia; Cheng, Yi; Xu, Shichen; Li, Bowen; Tomson, Mason B.; Han, Yimo; Yakobson, Boris I.; Tour, James M.; Welch Institute for Advanced Materials; NanoCarbon Center; Applied Physics Program; Smalley-Curl Institute
    The staggering accumulation of end-of-life lithium-ion batteries (LIBs) and the growing scarcity of battery metal sources have triggered an urgent call for an effective recycling strategy. However, it is challenging to reclaim these metals with both high efficiency and low environmental footprint. We use here a pulsed dc flash Joule heating (FJH) strategy that heats the black mass, the combined anode and cathode, to >2100 kelvin within seconds, leading to ~1000-fold increase in subsequent leaching kinetics. There are high recovery yields of all the battery metals, regardless of their chemistries, using even diluted acids like 0.01 M HCl, thereby lessening the secondary waste stream. The ultrafast high temperature achieves thermal decomposition of the passivated solid electrolyte interphase and valence state reduction of the hard-to-dissolve metal compounds while mitigating diffusional loss of volatile metals. Life cycle analysis versus present recycling methods shows that FJH significantly reduces the environmental footprint of spent LIB processing while turning it into an economically attractive process.
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    Construction and Regeneration of Solid-State Lithium Batteries by Rapid Joule Heating
    (2024-05-02) Chen, Jinhang; Tour, James Mitchell
    Solid-state batteries, with their superior safety and energy density, are promising candidates to replace current lithium-ion batteries with organic liquid electrolytes. Polymer- and oxide-based solid electrolytes are particularly attractive for their low cost in fabrication and stability in air and under high voltages. The thesis discusses the modifications of solid electrolytes, cathode materials, and their interface. Robust and intimate interfaces are designed and constructed for high electrical and ionic conductivity in solid-state batteries. Chapter 1 investigates the design of a polymer electrolyte incorporating a carbon-based redox mediator, tailed for use in Li-O2 and Li-air batteries. The modified electrolyte tolerates the parasitic LiO2 species, yielding reduced overpotential during cycling and extended cycling life. The underlying mechanism of superoxide dismutase mimetic behavior was studied. The work provides insights into the rational design and modification of polymer-based electrolytes. Chapter 2 explores the interfacial properties between an oxide-based solid electrolyte and common cathode materials. It details the construction of a thin, conductive interphase between lithium aluminum titanium phosphate and lithium cobalt oxide, achieved through a rapid sintering method surpassing traditional furnace sintering capabilities. The enhanced battery performance highlights the crucial role of reaction kinetics in developing an effective cathode-solid electrolyte interface. Chapter 3 presents a general method for applying a carbon coating to cathode materials using rapid Joule heating. This facile post-treatment technique allows for introducing heteroatoms, selectively enhancing the formation of inorganic components in the cathode-electrolyte interphase. This approach offers a practical way to engineer the interphase composition and improve its electrical and ionic conductivity. Chapter 4 explores the thermal-resistant battery design that can be regenerated through rapid Joule heating. The capacity loss due to mechanical failure is mitigated during the thermal treatment. The method proposes a potential solution to reduce the energy cost of oxide-based solid-state batteries, benefiting the circular economy and enhancing energy efficiency. Chapter 5 describes the synthesis of boron nitride nanomaterials through the rapid Joule heating method. The selectivity towards boron nitride nanotubes is tuned in the catalytic growth process, which provides critical insights into the mechanism of rapid materials synthesis techniques. This thesis advances our understanding of the interphase construction in solid-state batteries.
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    Electrothermal mineralization of per- and polyfluoroalkyl substances for soil remediation
    (Springer Nature, 2024) Cheng, Yi; Deng, Bing; Scotland, Phelecia; Eddy, Lucas; Hassan, Arman; Wang, Bo; Silva, Karla J.; Li, Bowen; Wyss, Kevin M.; Ucak-Astarlioglu, Mine G.; Chen, Jinhang; Liu, Qiming; Si, Tengda; Xu, Shichen; Gao, Xiaodong; JeBailey, Khalil; Jana, Debadrita; Torres, Mark Albert; Wong, Michael S.; Yakobson, Boris I.; Griggs, Christopher; McCary, Matthew A.; Zhao, Yufeng; Tour, James M.
    Per- and polyfluoroalkyl substances (PFAS) are persistent and bioaccumulative pollutants that can easily accumulate in soil, posing a threat to environment and human health. Current PFAS degradation processes often suffer from low efficiency, high energy and water consumption, or lack of generality. Here, we develop a rapid electrothermal mineralization (REM) process to remediate PFAS-contaminated soil. With environmentally compatible biochar as the conductive additive, the soil temperature increases to >1000 °C within seconds by current pulse input, converting PFAS to calcium fluoride with inherent calcium compounds in soil. This process is applicable for remediating various PFAS contaminants in soil, with high removal efficiencies ( >99%) and mineralization ratios ( >90%). While retaining soil particle size, composition, water infiltration rate, and cation exchange capacity, REM facilitates an increase of exchangeable nutrient supply and arthropod survival in soil, rendering it superior to the time-consuming calcination approach that severely degrades soil properties. REM is scaled up to remediate soil at two kilograms per batch and promising for large-scale, on-site soil remediation. Life-cycle assessment and techno-economic analysis demonstrate REM as an environmentally friendly and economic process, with a significant reduction of energy consumption, greenhouse gas emission, water consumption, and operation cost, when compared to existing soil remediation practices.
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    High-surface-area corundum nanoparticles by resistive hotspot-induced phase transformation
    (Springer Nature, 2022) Deng, Bing; Advincula, Paul A.; Luong, Duy Xuan; Zhou, Jingan; Zhang, Boyu; Wang, Zhe; McHugh, Emily A.; Chen, Jinhang; Carter, Robert A.; Kittrell, Carter; Lou, Jun; Zhao, Yuji; Yakobson, Boris I.; Zhao, Yufeng; Tour, James M.; Smalley-Curl Institute; NanoCarbon Center; Welch Institute for Advanced Materials
    High-surface-area α-Al2O3 nanoparticles are used in high-strength ceramics and stable catalyst supports. The production of α-Al2O3 by phase transformation from γ-Al2O3 is hampered by a high activation energy barrier, which usually requires extended high-temperature annealing (~1500 K, > 10 h) and suffers from aggregation. Here, we report the synthesis of dehydrated α-Al2O3 nanoparticles (phase purity ~100%, particle size ~23 nm, surface area ~65 m2 g−1) by a pulsed direct current Joule heating of γ-Al2O3. The phase transformation is completed at a reduced bulk temperature and duration (~573 K, < 1 s) via an intermediate δʹ-Al2O3 phase. Numerical simulations reveal the resistive hotspot-induced local heating in the pulsed current process enables the rapid transformation. Theoretical calculations show the topotactic transition (from γ- to δʹ- to α-Al2O3) is driven by their surface energy differences. The α-Al2O3 nanoparticles are sintered to nanograined ceramics with hardness superior to commercial alumina and approaching that of sapphire.
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    Nondestructive flash cathode recycling
    (Springer Nature, 2024) Chen, Weiyin; Cheng, Yi; Chen, Jinhang; Bets, Ksenia V.; Salvatierra, Rodrigo V.; Ge, Chang; Li, John Tianci; Luong, Duy Xuan; Kittrell, Carter; Wang, Zicheng; McHugh, Emily A.; Gao, Guanhui; Deng, Bing; Han, Yimo; Yakobson, Boris I.; Tour, James M.; Applied Physics Program;Smalley-Curl Institute;NanoCarbon Center;Rice Advanced Materials Institute
    Effective recycling of end-of-life Li-ion batteries (LIBs) is essential due to continuous accumulation of battery waste and gradual depletion of battery metal resources. The present closed-loop solutions include destructive conversion to metal compounds, by destroying the entire three-dimensional morphology of the cathode through continuous thermal treatment or harsh wet extraction methods, and direct regeneration by lithium replenishment. Here, we report a solvent- and water-free flash Joule heating (FJH) method combined with magnetic separation to restore fresh cathodes from waste cathodes, followed by solid-state relithiation. The entire process is called flash recycling. This FJH method exhibits the merits of milliseconds of duration and high battery metal recovery yields of ~98%. After FJH, the cathodes reveal intact core structures with hierarchical features, implying the feasibility of their reconstituting into new cathodes. Relithiated cathodes are further used in LIBs, and show good electrochemical performance, comparable to new commercial counterparts. Life-cycle-analysis highlights that flash recycling has higher environmental and economic benefits over traditional destructive recycling processes.