ACS Energy Letters 最新文献

Degradation of halide perovskites under a humid atmosphere is the major challenge preventing widespread commercial deployment of this material class. Here it is shown that strain engineering via alkali metal chloride treatment at the FAPbI₃/SnO₂ interface effectively improves moisture-related stability. CsCl and KCl treatments reduce microstrain at the perovskite surface and slow the α- to δ-phase transformation. Alkali metal treatments with LiCl, NaCl, and RbCl led to an increase in microstrain and faster degradation. The compressive strain at the perovskite surface was the smallest for CsCl and was linked to improved stability. First-principles density functional theory calculations confirm the preferential formation of alkali defects at interstitial positions at the perovskite surface. Particularly CsCl and KCl treatments lead to a release of compressive strain at the perovskite surface and local structural distortions that may favor passivation of surface defects. In contrast, the room-temperature dynamics of Li interstitials result in an overall expansion of lattice volume, which may be linked to more facile lattice degradation.

Aqueous proton batteries (APBs) have attracted increasing attention due to their high-power capability and low-temperature tolerance. Electrode materials remain a bottleneck and have restricted the further development of APBs. Here, we report H⁺/PO₄^3– reverse dual-ion batteries (RDIBs) with a Sb anode functioning as PO₄^3– host and a Turnbull blue analogue (TBA) or tetrachloro-p-benzoquinone (TCBQ) cathode as H⁺ host. The Sb anode reversibly accommodates PO₄^3– via the equation Sb + PO₄^3– – 3e^– ↔ SbPO₄ at −0.2–0 V vs Ag/AgCl and delivers a specific capacity of 686 mAh/g. Pairing with a TBA cathode, the resultant TBA|Sb RDIB exhibits acceptable cycling stability and rate capability even under a positive/negative (P/N) mass ratio of 7. Another TCBQ|Sb RDIB features a flat voltage platform and operation competence at −30 °C. Our work enriches anion hosts for high-capacity DIBs and offers a configuration solution to the practicality of H⁺-deficient electrodes in proton-based energy storage devices.

Constructing low-dimensionality/three-dimensionality (LD/3D) perovskite heterointerfaces is a well-established strategy to enhance the perovskite photovoltaic performance. Here, we introduce a solvent-orthogonality approach to precisely tailor the structure and dimensionality of LD perovskites within LD/3D perovskite heterointerfaces, thereby optimizing interfacial energetics. In this approach, LD perovskite precursors, comprising both organic and inorganic components, are dissolved in a mixed acetonitrile and 1,2-dimethoxyethaane solvent system and deposited onto a 3D perovskite layer with minimal impact on the substrate. Unlike traditional cation-exchange methods that focus solely on organic components, our strategy enables the growth of dimensionally tailored LD stacks (1D, 2D, and quasi-2D configurations), forming effective LD/3D heterointerfaces. This optimization improves carrier kinetics at the perovskite-charge transport layer, resulting in an n-i-p device efficiency of 25.14% and solar modules (18 cm² active area) with 22.61% efficiency. Our solvent-orthogonality strategy presents a promising method for engineering perovskite heterointerfaces in various photovoltaic applications.

In pursuing advanced clean energy storage technologies, all-solid-state Li metal batteries (ASSMBs) emerge as promising alternatives to conventional organic liquid electrolyte-based batteries due to their reduced flammability risks, increased energy densities, extended lifespan, and design flexibility. Here, we estimate lithium requirements per unit of energy, cathode loading, and the amount of electrolyte required at a single-layer cell level ASSMB utilizing garnet-type, NASICON-type, and sulfide solid electrolytes and LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811), LiCoO₂, and LiFePO₄ cathodes for Li metal anode and in situ anode configurations. To enable advanced batteries suitable for long-range and fast-charging electric vehicles, the electrodes (anode and cathode) must achieve a practical areal capacity of at least 7 mAh cm^–2 and support rapid charging rates of 4C (15 min). Furthermore, we also present the key requirements for mechanical properties and strategic design considerations in ASSMB architecture to effectively address the challenges posed by the volume expansion of the electrodes.

Low-temperature CO₂ electrolysis is a promising approach for defossilizing the production of commodity chemicals. However, state-of-the-art electrolyzers often suffer from low stability due to salt precipitation and electrode flooding. One strategy to increase the stability is pulsed operation of the electrolyzer, i.e. repeated application of low potentials (resting period). However, the water management of this operation mode is poorly understood. This work presents the first quantitative operando analysis of the water management in a CO₂ electrolyzer under application relevant operation conditions via high-resolution neutron imaging (<6 μm). Within 100 h of operation at 400 mA cm^–2, pulsed operation shows a significant stabilization of voltage and selectivity (1.8 mV h^–1 and −0.002% h^–1) compared to constant current operation (2.9 mV h^–1 and −0.11% h^–1). During the resting period, pulsed operation introduces 2.2 μL cm^–2 of additional water to the cathode, which facilitates the removal of salt precipitates and mitigates uncontrolled electrode flooding.

The surface spin configuration of catalysts is crucial for spin-dependent catalysis, as electrochemical reactions predominantly occur at the solid–liquid interface. This configuration influences reaction efficiency by altering the spin states of intermediates. Thus, identifying the surface spin configuration is essential for understanding the mechanisms affecting catalytic activity. This work designs multidomain and single-domain Fe₇S₈ nanosheets through thickness control. Under a 200 mT magnetic field, the multidomain sample transitions to a single-domain state, while the surface spin configuration of the single-domain sample remains unchanged, as observed via magnetic force microscopy. Electrochemical tests show that a saturated magnetic field of 200 mT reduces the overpotential of the multidomain sample from 306 to 240 mV at 10 mA cm^–2, while the single-domain sample maintains an overpotential of 257 mV. These results demonstrate that spin disorder at magnetic domain walls limits spin selectivity during the OER, suggesting strategies for developing innovative spin-selective catalysts.