ACS Applied Energy Materials

Journal: ACS Applied Energy Materials

Abbreviation

ACS Appl. Energy Mater.

Publisher

American Chemical Society

ISSN

2574-0962

Show all metadata

Search Results

Publications 1 - 10 of 39

Unveiling Solid-State Electrochemical Oxidation of LiBH₄ and Li₂B₁₂H₁₂ for High-Voltage All-Solid-State Batteries
Asakura, Ryo; Lodziana, Zbigniew; Grissa, Rabeb; et al. (2025)
ACS Applied Energy Materials
Hydridoborates are an emerging class of solid electrolytes that offer high ionic conductivity, low density, solution processability, compatibility with metallic anodes, and high oxidative stability. Notably, certain Li⁺ or Na⁺ solid electrolytes, consisting of two different cage-like closo-hydridoborate anion species, are compatible with 4 V-class cathodes by forming a sufficiently ion-conductive, passivating interphase. However, the nature of their electrochemical decomposition products and their dependence on electrochemical potentials remain unclear. In this combined theoretical and experimental study, we demonstrate the solid-state electrochemical oxidation of LiBH₄ to Li₂B₁₂H₁₂ above 2.0 V vs Li⁺/Li and provide evidence for the successive oxidation of closo-[B₁₂H₁₂]²⁻ anions to larger H-interconnected closo-clusters. This supports the observed trend that larger clusters formed via oxidation are stabilized at higher electrochemical potentials. Notably, the oxidation process from LiBH₄ toLi₂B₁₂H₁₂ proceeds through the formation of a highly conductive [BH₄]⁻–[B₁₂H₁₂]²⁻ mixed phase, indicating the potential for in situ formation of mixed-anion hydridoborates directly within all-solid-state cells. These insights into solid-state electrochemical decomposition at the solid-solid interfaces are transferable to other hydridoborate systems, regardless of cation species or anion structures, contributing to developing cathode design strategies for high-voltage all-solid-state batteries.
Evaluation of Dip-And-Pull Ambient Pressure X-ray Photoelectron Spectroscopy for Investigating Oxygen Evolution Reaction Electrocatalysts
Aegerter, Dino; Fabbri, Emiliana; Novotny, Zbynek; et al. (2025)
ACS Applied Energy Materials
In situ investigations of solid–liquid interfaces are crucial for gaining a fundamental understanding of electrocatalytic processes. Dip-and-pull ambient pressure X-ray photoelectron spectroscopy (APXPS) enables such investigations by analyzing an electrocatalyst surface (solid) through the covering electrolyte layer (liquid) with an applied electrochemical potential. This stable solid–liquid interface is created by vertically “dipping” and then “pulling” an electrode from a bulk electrolyte solution. The resulting electrolyte layer has a decreasing thickness toward the upper electrode, allowing in situ probing of the electrocatalyst surface in this upper region. However, detecting representative electrocatalyst surface changes remains challenging with dip-and-pull APXPS. To address the challenge, this study experimentally evaluates electrochemical and spectroscopic aspects of dip-and-pull APXPS by investigating thin films of Ni_1–xFe_xO_yoxygen evolution reaction (OER) electrocatalysts. Here, two technical limitations are revealed: (1) missing Faradaic reactions (i.e., redox and OER) in the electrocatalyst surface probing region and (2) low spectroscopic surface-sensitivity with the typically used tender X-rays. Limitation (1) is discovered with a modified electrode design that enables OER activity measurements, indicating limited ionic conductance along the vertically thinning electrolyte layer. This strongly suppresses the studied Faradaic reactions and hinders operando investigations of OER electrocatalyst thin films in the upper electrode region, where their surfaces are probed. To minimize limitations (1) and (2), the findings suggest changing electrochemical potential only when the electrode is completely dipped in the bulk electrolyte to enhance surface modifications and using lower energetic photons at higher flux to improve the surface-sensitivity. Moreover, cyclic voltammetry is presented as an electrochemical conditioning method to maximize the spectroscopic detectability of OER electrocatalyst surface changes. Overall, this dip-and-pull APXPS evaluation provides fundamental insights and suggestions that will further improve the technique for investigating OER electrocatalysts.
Performance Comparison of Transition Metal (Cr, Mn, Fe, Co, Ni, Cu)-Fluoride Conversion Cathodes in Thin-Film Solid-State Batteries
Casella , Joel; Morzy, Jedrzej Krzysztof; Mocanu , Felix C.; et al. (2025)
ACS Applied Energy Materials
Transition metal fluorides (TMFs) are promising alternatives for Li battery cathode active materials as they can show specific capacities up to 619 mAh/g for CrF3, compared to 272 mAh/g for LiNi0.8Mn0.1Co0.1O2, a commonly used intercalation cathode. TMFs are intrinsically difficult to study due to their incompatibility with typical liquid electrolytes and the need for conductive additives to ensure sufficient utilization. In this work, thin-film solid-state devices are used to compare six transition metals mixed with LiF in a 1.1:2 TM/LiF ratio (where TM = Cr, Mn, Fe, Co, Ni, or Cu) without the influence of additive and electrolyte interactions. C/10 delithiated capacities of 540, 113, 402, 407, 566, and 143 mAh/g are shown for (Cr, Mn, Fe, Co, Ni, Cu)-LiF cathodes, respectively. Chromium fluoride consistently outperforms the other cathodes up to 8C (190/219 mAh/g, lithiated/delithiated). Differences between the behavior of the TM-LiF cathodes are explored using electrochemical characterization and atomistic simulations. The choice of TM has a significant impact on cathode performance, which is likely to be connected to their distinct chemical natures, changing the thermodynamics and pathway of the conversion reaction.
Silver Bismuth Iodides for Photovoltaic Applications: Insights from Ab Initio Calculations and Experimental Analysis
Mladenović, Marko; Jahanbakhshi, Farzaneh; Im, Jeong-Hyeok; et al. (2025)
ACS Applied Energy Materials
Hybrid organic-inorganic perovskite solar cells (PSCs) present a leading thin-film photovoltaic technology with superior solar-to-electric power conversion efficiencies. The most effective compositions, however, contain lead cations, which are toxic and pose environmental hazards. One of the alternatives to lead-based perovskite materials is silver bismuth halide analogues. Here, we present a comprehensive investigation of different silver bismuth iodide compositions by means of density functional theory calculations (DFT) as well as X-ray diffraction, scanning and transmission electron microscopy, X-ray photoelectron spectroscopy, and photoluminescence spectroscopy measurements. Through our combined experimental and theoretical study, we have discovered that silver bismuth iodides possess several intrinsic limitations, such as limited charge transport and localized electronic states, owing to the presence of vacant sites. Such limitations result in moderate solar cell efficiencies, significantly lower than those of lead halide perovskites. However, we suggest the possibility of increasing efficiencies by adding BiCl3 to the precursor solution, yielding one of the highest efficiencies reported for this class of compounds to date. This highlights the potential of compositional engineering for these lead-free solar cell materials.
All-Nanofiber-Based Ultralight Stretchable Triboelectric Nanogenerator for Self-Powered Wearable Electronics
Zhao, Shuyu; Wang, Jiaona; Du, Xinyu; et al. (2018)
ACS Applied Energy Materials
A Quasi-Solid-State Polymer Lithium-Metal Battery with Minimal Excess Lithium, Ultrathin Separator, and High-Mass Loading NMC811 Cathode
Homann, Gerrit; Wang, Qing; Liu, Sufu; et al. (2024)
ACS Applied Energy Materials
Solid-state batteries with lithium metal anodes are considered the next major technology leap with respect to today’s lithium-ion batteries, as they promise a significant increase in energy density. Expectations for solid-state batteries from the automotive and aviation sectors are high, but their implementation in industrial production remains challenging. Here, we report a solid-state lithium–metal battery enabled by a polymer electrolyte consisting of a poly(DMADAFSI) cationic polymer and LiFSI in Pyr₁₃FSI as plasticizer. The polymer electrolyte is infiltrated and solidified in the pores of a commercial LiNi₀.₈Mn₀.₁Co₀.₁O₂ (NMC811) cathode with up to 2.8 mAh cm⁻² nominal areal capacity and in the pores of a 25 μm thin commercial polypropylene separator. Cathode and separator are finally laminated into a cell in combination with a commercial 20 μm thin lithium metal anode. Our demonstration of a solid-state polymer battery cycling at full nominal capacity employing exclusively commercially available components available at industrial scale represents a critical step forward toward the commercialization of a competitive all-solid-state battery technology.
An Organic Cathode Based Dual-Ion Aqueous Zinc Battery Enabled by a Cellulose Membrane
Glatz, Hadrien; Lizundia, Erlantz; Pacifico, Fiona; et al. (2019)
ACS Applied Energy Materials
Li4–xGe1–xPxO4, a Potential Solid-State Electrolyte for All-Oxide Microbatteries
Gilardi, Elisa; Materzanini, Giuliana; Kahle, Leonid; et al. (2020)
ACS Applied Energy Materials
Solid-state electrolytes for Li-ion batteries are attracting growing interest as they allow building safer batteries, also using lithium-metal anodes. Here, we studied a compound in the lithium superionic conductor (LISICON) family, i.e., Li4−xGe1−xPxO4 (LGPO). Thin films were deposited via pulsed laser deposition, and their electrical properties were compared to those of ceramic pellets. A detailed characterization of their microstructures shows that thin films can be deposited fully crystalline at higher temperatures but also partially amorphous at room temperature. The conductivity is not strongly influenced by the presence of grain boundaries, exposure to air, or lithium deficiencies. First-principles molecular dynamics simulations were employed to calculate the lithium-ion diffusion profile and the conductivity at various temperatures of the ideal LGPO crystal. Simulations give the upper limit of conductivity for a defect-free crystal, which is in the range of 10−2 S cm−1 at 300 °C. The ease of thin-film fabrication and room-temperature Li-ion conductivity in the range of a few μS cm−1 make LGPO very appealing electrolyte material for thin-film all-solid-state all-oxide microbatteries. © 2020 American Chemical Society
Influence of Carbon Material Properties on Activity and Stability of the Negative Electrode in Vanadium Redox Flow Batteries: A Model Electrode Study
Taylor, Susan M.; Pătru, Alexandra; Perego, Daniele; et al. (2018)
ACS Applied Energy Materials
SWCNT-Encapsulated Phosphorus-Grafted Stearyl Alcohol as a Flame-Retardant Phase-Change Material with Superior Thermal Properties
Li, Jun; Chen, Renjie; Luo, Yong; et al. (2022)
ACS Applied Energy Materials
Organic phase-change materials (OPCMs) are one of the most preferred media for thermal energy storage (TES) applications but are troubled by their low thermal conductivity, leakage, and flammability problems. Herein, stearyl alcohol (SAL), as an OPCM, was first chemically bonded with phosphorus oxychloride (POCl3) to reduce its flammability and then encapsulated in a single-wall carbon nanotube (SWCNT) skeleton to address the low thermal conductivity and leakage issue, obtaining a flame-retardant form-stable phase-change material film (PCMF). As a result, a promising heat storage capacity (191.3 kJ/kg) and superior thermal stability of the modified SAL were achieved as evaluated via differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA) testing. Then, microscale combustion calorimetry (MCC) testing was carried out, showing that the peak of the heat release rate (PHRR) and total heat release (THR) of the modified SAL were, respectively, reduced by 24.4% and 24.3% compared to bare SAL. After encapsulating the modified SAL into the SWCNT skeleton, the PHRR and THR values of the as-prepared PCMF can be further reduced because of the synergistic effect between the phosphorus group and the SWCNT skeleton, while the electrical and thermal conductivity of the PCMF were significantly improved, simultaneously. In addition, the obtained PCMF presented excellent light-to-thermal conversion and thermal energy storage performance. Thus, the strategy presented in this work provides a general method to extend the OPCMs application with superior flame-retardant properties.

Publications 1 - 10 of 39

Journal: ACS Applied Energy Materials

Abbreviation

Publisher

Journal Volumes

ISSN

Description

Filters

Search Results