A Replacement Reaction Enabled Interdigitated Metal/Solid Electrolyte Architecture for Battery Cycling at 20 mA cm-2 and 20 mAh cm-2
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Abstract Meeting end‐of‐century global warming targets requires aggressive action on multiple fronts. Recent reports note the futility of addressing mitigation goals without fully engaging the agricultural sector, yet no available assessments combine both nature‐based solutions (reforestation, grassland and wetland protection, and agricultural practice change) and cellulosic bioenergy for a single geographic region. Collectively, these solutions might offer a suite of climate, biodiversity, and other benefits greater than either alone. Nature‐based solutions are largely constrained by the duration of carbon accrual in soils and forest biomass; each of these carbon pools will eventually saturate. Bioenergy solutions can last indefinitely but carry significant environmental risk if carelessly deployed. We detail a simplified scenario for the United States that illustrates the benefits of combining approaches. We assign a portion of non‐forested former cropland to bioenergy sufficient to meet projected mid‐century transportation needs, with the remainder assigned to nature‐based solutions such as reforestation. Bottom‐up mitigation potentials for the aggregate contributions of crop, grazing, forest, and bioenergy lands are assessed by including in a Monte Carlo model conservative ranges for cost‐effective local mitigation capacities, together with ranges for (a) areal extents that avoid double counting and include realistic adoption rates and (b) the projected duration of different carbon sinks. The projected duration illustrates the net effect of eventually saturating soil carbon pools in the case of most strategies, and additionally saturating biomass carbon pools in the case of forest management. Results show a conservative end‐of‐century mitigation capacity of 110 (57–178) Gt CO 2 e for the U.S., ~50% higher than existing estimates that prioritize nature‐based or bioenergy solutions separately. Further research is needed to shrink uncertainties, but there is sufficient confidence in the general magnitude and direction of a combined approach to plan for deployment now.
Meeting end-of-century global warming targets requires aggressive action on multiple fronts. Recent reports note the futility of addressing mitigation goals without fully engaging the agricultural sector, yet no available assessments combine both nature-based solutions (reforestation, grassland and wetland protection, and agricultural practice change) and cellulosic bioenergy for a single geographic region. Collectively, these solutions might offer a suite of climate, biodiversity, and other benefits greater than either alone. Nature-based solutions are largely constrained by the duration of carbon accrual in soils and forest biomass; each of these carbon pools will eventually saturate. Bioenergy solutions can last indefinitely but carry significant environmental risk if carelessly deployed. We detail a simplified scenario for the U.S. that illustrates the benefits of combining approaches. We assign a portion of non-forested former cropland to bioenergy sufficient to meet projected mid-century transportation needs, with the remainder assigned to nature-based solutions such as reforestation. Bottom-up mitigation potentials for the aggregate contributions of crop, grazing, forest, and bioenergy lands are assessed by including in a Monte Carlo model conservative ranges for cost-effective local mitigation capacities, together with ranges for (a) areal extents that avoid double counting and include realistic adoption rates and (b) the projected duration of different carbon sinks. The projected duration illustrates the net effect of eventually saturating soil carbon pools in the case of most strategies, and additionally saturating biomass carbon pools in the case of reforestation. Results show a conservative end-of-century mitigation capacity of 110 (57 – 178) Gt CO2e for the U.S., ~50% higher than existing estimates that prioritize nature-based or bioenergy solutions separately. Further research is needed to shrink uncertainties but there is sufficient confidence in the general magnitude and direction of a combined approach to plan for deployment now.
Manganese dioxide (MnO 2 ) deposition/dissolution (Mn 2+ /MnO 2 ) chemistry, involving a two-electron-transfer process, holds promise for safe and eco-friendly large-scale energy storage. However, challenges like electrode/electrolyte interface environment fluctuations (H + and H 2 O activity), irreversible Mn degradation, and limited understanding of degradation mechanisms hinder the reversibility of the Mn 2+ /MnO 2 conversion. This study demonstrates a vanadyl/pervanadyl (VO 2+ /VO 2 + ) redox-mediated interface designed for high-energy Mn 2+ /MnO 2 batteries. Unlike flow systems, this work uncovers, for the first time, the mechanism of a static redox-mediated interface in regulating interfacial H + and H 2 O activities. Significantly, the VO 2+ /VO 2 + chemical redox mediation targets Mn 3+ intermediates, suppressing their hydrolysis and enabling 100% Mn 2+ /MnO 2 conversion. The redox-mediated interface enhances the Mn redox electron transfer process, achieving a stable ≈95% coulombic efficiency and ultrahigh capacity of 100 mAh cm −2 with an areal energy density of 111 mWh cm −2 , outperforming flow systems. The electrode also exhibits an average specific capacity of 593 mAh g −1 , approaching the theoretical limit of 616 mAh g −1 , and a specific energy density of 721 Wh kg −1 at high MnO 2 loadings (50–150 mg cm −2 ). Furthermore, the findings highlight the critical role of interfacial redox mediation in regulating H + and H 2 O activities and underscore the significance of interface dynamics.
All-solid-state Lithium batteries (ASSLBs) have gained widespread attention in recent years. However, their performance is still largely limited by the poor transport properties and stability of the solid-solid interfaces (SSIs). In this study, we report a new strategy for creating a reversible interface with good conductivity and self-adaptive mechanical properties for high-performance all-solid-state lithium batteries (ASSLBs). The interface is formed in situ from nanosized lithium iodide (LiI), a component of the solid-state electrolyte (SSE), which flows plastically along the SSE interfaces under high pressure due to its high ductility. Moreover, LiI segregates and enriches along the Li/SSE interfaces, reversibly enhancing Li plating/stripping due to its lithophilicity and high ionic conductivity. This dynamic LiI interface enables stable operation of metallic Li anode (>1000 h) at high current densities and elevated temperatures, and long-term cycling of all-solid-state Li-sulfur batteries (>250 cycles) with high sulfur utilization rate (>1400 mAh g-1) and areal capacity (>2 mAh cm-2). This study reveals a unique role of LiI in building robust SSIs and provides new insights into the design of novel SSEs and interfaces for high-performance ASSLBs.