ACS Applied Energy Materials最新文献

High-entropy alloy aerogels (HEAAs) have emerged as promising catalysts that combine multimetallic synergy and surface unsaturated sites for renewable energy conversion, yet the development of efficient and low-cost HEAAs remains challenging. In this study, for the first time, Cu-rich CuBiInZnPd HEAAs were prepared as efficient electrocatalysts for the carbon dioxide reduction reaction (CO₂RR). Compared with low-entropy counterparts such as CuPd metallic aerogels (MAs) and Cu MAs, the CuBiInZnPd HEAAs possess a higher Faradaic efficiency for formate of 94.7% at −1.0 V versus the reversible hydrogen electrode during the CO₂RR. Moreover, CuBiInZnPd HEAAs demonstrate excellent operational stability, maintaining nearly constant current density over 20 h. Mechanism research indicates that the multimetallic synergy and surface unsaturated sites in CuBiInZnPd HEAAs influence the surface electronic structure of Cu and the adsorption of reaction intermediates, consistent with the observed CO₂RR performance. This work provides a new approach for the functionalization of HEAAs and offers new ideas for the design of low-cost CO₂RR electrocatalysts.

The limited thermal stability of organic solar cells has hampered their commercialization. Therefore, it is crucial to gain in-depth insight into the underlying causes of thermal device instability and to develop practical approaches to reduce its impact. In this study, we examine thermal degradation processes of the donor/acceptor system PBDB-T-2F:BTP-4F (alias PM6:Y6) in bulk heterojunction polymer/nonfullerene acceptor (NFA) solar cells, considered as a state-of-the-art system of the organic photovoltaics (OPV) technology. More specifically, this study investigates the effects of varying postproduction annealing temperatures on the performance of solar cells and locally resolves the thermally induced impact on these solar cells using a set of advanced imaging techniques, including photoluminescence imaging (PLI), electroluminescence imaging (ELI), and light beam-induced current (LBIC) measurements.

The electrochemical reduction of CO₂ is typically investigated under pure CO₂ feeds, but practical deployment must address more complex and dilute sources such as flue gases. Here, we studied Cu/Cu₂O electrodes decorated with tin (Sn) synthesized using a scalable electrodeposition method and post-treatments under both pure CO₂ and reactive nitrogen oxide-containing simulated flue gas, toward formic acid synthesis. Raman spectroscopy and Atomic Force Microscopy analyses revealed that flue gas exposure induces heterogeneous restructuring of the electrode with surface roughening, surface carbonate formation, and localized redeposition processes. Optimal catalyst performance under pure CO₂ was achieved with intermediate Sn coverage of 3 min electrodeposition, delivering Faradaic efficiencies of 80% and production rates of 370 μmol cm^–2 h^–1. Sn-modified Cu₂O electrodes also exhibited high selectivity toward formic acid under acidic gas containing simulated flue gas, reaching Faradaic efficiencies of 90% albeit at production rates of 113 μmol cm^–2 h^–1, despite a 10-fold reduced CO₂ partial pressure. These results demonstrate that interfacial Sn–Cu structures enabled selective CO₂RR even under challenging feed conditions, pointing out both the opportunities and limitations of translating laboratory-scale catalysts to realistic gas streams.

Gelatin is a promising biomass material for supercapacitors. In this article, carboxymethyl cellulose (CMC) and gelatin are used as raw materials to form soluble composite condensates as precursors for carbon electrodes as well as gel electrolytes. By an environmentally friendly method, N, O, and P multidoped three-dimensional porous carbon named CMC-GL-700 with a large specific surface area of 613.62 m² g^–1 and a pore volume of 0.3672 cm³ g^–1 is obtained. Due to these advantages, the porous carbon electrode delivers a large specific capacitance of 340 F g^–1 at 1 A g^–1 and good cycle stability with 92.5% capacity retention after 10000 cycles. Moreover, all CMC-GL-based quasi-solid-state supercapacitors, made with CMC-GL-700 as an electrode and CMC/GL hydrogel as a gel electrolyte, exhibit a high energy density of 39.16 Wh kg^–1 at a power density of 414.64 W kg^–1.

Ruthenium-based electrocatalysts have emerged as a promising alternative to iridium when it comes to the oxygen evolution reaction (OER), particularly in proton exchange membrane water electrolyzers (PEMWE). Although Ru-based catalysts exhibit superior intrinsic activity, their widespread adoption is hindered by stability challenges under acidic operating conditions, necessitating strategies to mitigate dissolution and degradation. This review offers an in-depth examination of Ru-based catalysts, highlighting the critical role of support materials in determining their catalytic activity, electronic conductivity, and long-term stability. The discussion is systematically organized according to the type of support material, each offering distinct advantages and limitations. Reported experimental studies are compiled and critically analyzed to highlight representative advances in synthesis strategies and corresponding electrochemical performance, with emphasis on catalytic activity and durability. By consolidating recent progress and performance benchmarks, this review provides a coherent overview of the current landscape of Ru-based OER electrocatalysts. Finally, future research directions are proposed to accelerate the development of robust, high-performance Ru-based catalysts capable of replacing iridium in large-scale PEM water electrolysis applications. By bridging insights across materials design, synthesis, and electrochemical evaluation, this review aims to guide the rational development of next-generation Ru-based electrocatalysts that combine high activity, stability, and scalability for sustainable hydrogen production.

Poly(vinylidene fluoride) (PVDF)-based composite solid-state electrolytes (CSEs) have high application value in the field of solid-state electrolytes due to their high dielectric constant, excellent electrochemical stability, and thermal stability. However, compatibility issues between the polymer matrix and inorganic filler have hindered the development of CSEs. Furthermore, PVDF is prone to dehydrofluorination in alkaline environments, which exacerbates the agglomeration of inorganic filler and decreases the electrolyte’s overall performance. Herein, a controlled treatment of the surface of inorganic ceramic filler Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO) is carried out by an appropriate amount of introducing acetic acid (HAc), thereby efficiently removing Li₂CO₃ from the surface of LLZTO and precisely adjusting the pH of the electrolyte slurry. Moreover, the distribution of LLZTO in the polymer matrix is significantly improved, enhancing the mechanical strength of the electrolyte membrane and optimizing the Li⁺ transport path. The optimized CSEs exhibit high room-temperature ionic conductivity of 0.577 mS·cm^–1 and enhance compatibility with the lithium metal anode. The lithium symmetric battery can be stably cycled at 0.1 mA·cm^–2 for 1750 h. The LiFePO₄∥Li full battery exhibits good stability at 1C, with an initial specific discharge capacity of 138.4 mAh·g^–1 and a capacity retention of 94.9% after 200 cycles and 70.6% after 500 cycles. This study provides a simple and effective solution to optimize the preparation process and improve the overall performance of CSEs.

Anode-free lithium metal batteries (AFLMBs) are considered promising technologies for future storage applications, capable of achieving superior energy density in a streamlined cell design. Yet, their practical realization remains clouded by persistent challenges, including formation of lithium dendrites and limited cycling durability. Herein, we introduce a composite nanofiber separator composed of polyimide (PI) interwoven with garnet-type Li_6.75La₃Zr_1.75Ta_0.25O₁₂ (LLZTO) fillers, fabricated via a one-step electrospinning method and subsequently underwent thermal imidization. The fabricated PI/LLZTO membrane forms a robust, three-dimensional fibrous network with well-distributed LLZTO particles. This architecture significantly improves both electrolyte uptake and mechanical strength, while forming a channel for continuous ion conduction that encourages uniform Li⁺ flux, one of the key factors in suppressing dendrite formation. The separator delivers high ionic conductivity, reaching 3.16 mS cm^–1 with a measured Li⁺ transference number of 0.76. In Li symmetric cells, it enables remarkably stable cycling over 2900 h with an ultralow overpotential (∼0.007 V). When deployed in Cu||NMC622 AFLMB full cells, it delivers smooth and dendrite-suppressed lithium deposition behavior, with a first-cycle discharge capacity of 181 mAh g^–1 and retaining 40% capacity after completing 100 charge–discharge cycles. In comparison, the commercial polypropylene separator retains 10% only. This work demonstrates how functional separator design, particularly anchored ceramic–polymer synergy, can unlock pathways toward stable, high-performance AFLMBs.

Sodium-ion batteries (SIBs) are emerging as cost-effective and sustainable candidates for large-scale energy storage due to the natural abundance and low cost of sodium. However, conventional graphite anodes are intrinsically unsuitable for SIBs because Na ion intercalation is thermodynamically unfavorable, motivating the exploration of alternative anode materials. Inspired by the recent experimental realization of the biphenylene network (BPN), encourages to explore its low-dimensional analogues as potential anode materials for alkali-ion batteries. In this study, we therefore rationally design and investigate biphenylene concentric nanorings (BPNCRs), a zero-dimensional (0D) derivative of BPN, as a potential anode material for SIBs using first-principles density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations. The BPNCR anode exhibits a high theoretical capacity of 483 mAhg^–1 and energy density of 1236 mWhg^–1, which can be further enhanced by increasing the inter-ring separation. The average open-circuit voltage is 0.15 V under vacuum and becomes significantly higher (0.76 V) under electrolyte-screened conditions, which is beneficial for practical operation. Charge analysis reveals significant electron transfer from Na to the carbon framework, indicating strong Na–C interaction and also all Na atoms are charged, thereby reducing the possibility of Na plating. BPNCRs also exhibit excellent mechanical stability, with slight volume expansion (∼1.06%) during sodiation and a low Na-ion diffusion barrier (<0.22 eV), ensuring fast ion transport. The electrolyte effect is examined using an implicit solvation model with ethylene carbonate, which further stabilizes Na adsorption. AIMD simulations at 300 K yield a high Na diffusion coefficient of 3.57 × 10^–5 cm² s^–1, indicating fast Na ion diffusion kinetics. Furthermore, a three-dimensional bulk assembly of sodiated BPNCRs is modeled and found to be structurally stable, providing a practical pathway toward bulk electrode realization. Overall, these results highlight BPNCRs as a promising confined carbon anode platform and provide insights into structure-driven design principles for high-performance SIB anodes.

Natural evolution has led to long-term interactions between biology and the environment, with many excellent functions and perfect structures existing in nature. Inspired by the vertebral column structure, we developed a buffer-engineered nucleation strategy for inserting a buffer component into adjacent perovskite grains. This strategy synchronously tailors the perovskite crystallization of perovskite films and improves the flexibility of inverted perovskite solar cells. The rigid and high-quality perovskite grains that efficiently absorb photons correspond to the vertebrae of vertebrates, whereas fullerene, as a flexible buffer, can serve as an intervertebral disk to interconnect neighboring vertebra-like grains. In addition to functioning as a buffer to enhance the flexibility of the film, the fullerene inserted between the perovskite grains was also employed to passivate the uncoordinated lead ions in the perovskite and promote interfacial contacts, enhancing the efficiency of charge extraction at the interface. As a result, the power conversion efficiency of a methylammonium-based flexible perovskite solar cell, fabricated on a flexible polyethylene terephthalate substrate, was significantly enhanced from the pristine device’s value of 14.58% to 18.21%. Moreover, the FPSCs successfully survived a harsh dynamic mechanical bending test owing to the reasonable inspiration from the vertebral column. This strategy could prove highly beneficial for future FPSC fabrication processes because of the significant enhancement in the elasticity and flexural strength of the perovskite films at the nanoscale, as well as the effective passivation of defects achieved by the embedded materials.

We study the charge and spin-dependent thermoelectric response of a ferromagnetic helical system irradiated by arbitrarily polarized light using a tight-binding framework and the Floquet–Bloch formalism. Transport properties for individual spin channels are determined by employing the nonequilibrium Green’s function technique, while phonon thermal conductance is evaluated using a mass-spring model with different lead materials. The findings reveal that light irradiation induces spin–split transmission features, suppresses thermal conductance, and yields favorable spin thermopower and figure of merit (FOM). The spin FOM consistently outperforms its charge counterpart under various light conditions. Moreover, long-range hopping is shown to enhance the spin thermoelectric performance, suggesting a promising strategy for efficient energy conversion in related ferromagnetic systems.