Energy advances最新文献

The development of efficient catalysts for the cycloaddition of CO₂ with epoxides to produce cyclic carbonates (CCs) under mild reaction conditions remains a highly attractive research area. This study presents a trimethyl ammonium-rich pillar[5]arene (N(Me)₃⁺-P5) macrocycle as a promising heterogeneous catalyst for this reaction. The catalyst design ensures a complementary dual-function mechanism to facilitate the catalytic process. The ammonium groups activate the epoxides, and the bromide ions act as nucleophiles to initiate the ring opening. Optimized reaction conditions using 0.7 mol% catalyst loading and a CO₂ balloon at 80 °C, resulted in high CC yields, particularly with sterically unhindered epoxides. Furthermore, N(Me)₃⁺-P5 can be reused for at least five catalytic cycles, demonstrating its potential for sustainable applications.

Carbon capture and utilization technologies are considered crucial in reducing carbon dioxide levels in the atmosphere and mitigating climate change. One of the most promising utilization options is the catalytic hydrogenation of the captured carbon dioxide to methanol. However, this reaction requires large energy-consuming recycles due to the limitation of the chemical equilibrium. To shift the chemical equilibrium and increase per-pass conversion, membrane reactors that remove the produced water from the reaction zone can be applied. A sophisticated CFD model of the membrane reactor with a NaA zeolite membrane is developed, to identify key constructive and operating parameters. The model implements the Maxwell–Stefan approach for permeation that considers the complex behavior of pervaporating water–alcohol mixtures through microporous zeolite membranes. In a full-factorial design of experiment, two general categories of parameters (ratio between reaction and permeation, permeation driving force) that influence conversion and yield in membrane reactors are identified that need to be optimized in construction and operation. In the most promising configuration, the application of the membrane reactor results in an increased CO₂ conversion of 20.6% and a 16.0% enhanced methanol yield compared to an equivalent conventional reactor. With the findings of this study, key parameters for the general optimization of the construction and operation of membrane reactors for industrial applications are identified.

Correction for ‘Evaluation of redox pairs for low-grade heat energy harvesting with a thermally regenerative cycle’ by José Tomás Bórquez Maldifassi et al., Energy Adv., 2024, 3, 2877–2886, https://doi.org/10.1039/D4YA00368C.

As part of the rapidly advancing field of energy technologies, solar energy-driven studies using nanomaterials have gained significant attention. In this context, designing dye-sensitized solar cells (DSSCs) with nanostructured titania (TiO₂) and its composites is a key focus in material selection. This study investigated the synthesis and photovoltaic performance of TiO₂ nanoparticles (NPs) and their composites with ZnO nanorods (NRs), synthesized via a one-step ex situ approach. The fabricated devices were evaluated using a metal-free SK3 dye (D–π–A carbazole) and a Co²⁺/Co³⁺-based polymer gel electrolyte. Structural properties were analyzed using Rietveld refinement, alongside other physicochemical characteristics. Notably, the TiO₂/ZnO nanocomposite (TZ-3 NCs) with 30 wt% ZnO NRs in the photoanode demonstrated a significant improvement in solar energy-conversion efficiency (η) of 4.3%, which was 1.8 times higher than that of the TiO₂/SK3 NC-based photoanode (2.38%). This enhancement was attributed to the reduced charge-transfer resistance, improved donor density, and increased surface area, facilitating efficient charge transport. Additionally, the study explored the stability of the TZ-3/SK3 NC-based photoanode using time series analysis, a statistical tool that can contribute to understanding its long-term performance.

Correction for ‘Additive manufacturing of highly conductive carbon nanotube architectures towards 3D-printed carbon-based flexible thermoelectric generators’ by Christos K. Mytafides et al., Energy Adv., 2024, 3, 1642–1652, https://doi.org/10.1039/D4YA00182F.

Conventional lithium-ion batteries (LIBs) have become widely used in small and large applications, but the use of toxic and flammable liquid electrolytes can lead to safety issues and reduced cell performance. New generation solid-state lithium batteries (SSBs) have the potential to replace LIBs due to their safety and potentially high energy density (>450 W h kg⁻¹). The solid electrolyte (SE) is a crucial component in solid-state batteries. Among the available options, sulfide- and halide-based solid electrolytes stand out as promising candidates due to their high ionic conductivity and ease of processing. They are among the most prominent topics in solid electrolyte research for solid-state batteries. Despite their advantages like good compatibility with high-voltage cathodes and easy manufacturing, solid electrolytes still face issues of degradation of the Li metal/solid electrolyte interface. This is due to the formation of side reaction products at the interface, which inhibits lithium transport across it. The primary issue stems from the poor chemical and electrochemical stability of sulfide- and halide-based solid electrolytes when in contact with lithium metal. In this study, we have demonstrated that the composite electrolytes (Li₃YCl₄Br₂:Li₆PS₅Cl) comprising halide and argyrodite can prevent the formation of unfavorable interactions between the solid electrolyte and the Li metal anode. The Li/Li-symmetric cells employing the Li₃YCl₄Br₂:Li₆PS₅Cl electrolytes exhibited enhanced cycle life and high critical current density (CCD) from C/20 to C/2, compared to the symmetric cells utilizing only Li₃YCl₄Br₂ or Li₆PS₅Cl electrolyte. Furthermore, the Li/Li₃YCl₄Br₂/NCM half-cells demonstrated high initial coulombic efficiency and extended cycle life compared to half-cells utilizing traditional halide and argyrodite electrolytes. The approach described here offers a pathway to enhance halide-based solid-state batteries, providing a relatively simple and effective strategy.

Carbon mineralization offers the potential to durably store gigatonne-scale CO₂ emissions, with mining waste representing an especially promising feedstock due to its relatively small particle size, global availability, and opportunities for decarbonizing the mining sector. Despite significant research into the scale and potential of this technology, there remains a lack of techno-economic analyses (TEAs) that comprehensively capture the full-process costs of indirect carbonation using a pH-swing approach. This approach enables both CO₂ storage in carbonates, potentially usable to decarbonize concrete, and the extraction of critical minerals, incorporating the costs and revenues of coupling these processes. To address this gap, we developed a Class IV TEA tailored to estimate the costs and life cycle assessment (LCA) of combining critical mineral extraction and carbon mineralization in mining wastes. The model evaluates scenarios for various waste types (i.e.., legacy asbestos waste, aggregate quarry tailings, platinum group metal tailings) under different extraction conditions (acid type, temperature, strength) and carbonation parameters. Additionally, sensitivity analyses explore the effects of reactor design, internal acid–base recycling, and other factors on process costs and carbon efficiency. Our findings show carbon efficiencies of up to 95%, depending on process design. Acid–base recycling is critical for cost-effective and carbon-negative operations: without recycling, process costs exceed $3000 per tCO₂ and yield a carbon efficiency of −280%, while internal acid regeneration reduces costs to $500–800 per tCO₂ with carbon efficiencies ranging from 41–72%. Process costs vary by waste type and process conditions, ranging from $800–1800 per tCO₂ (assuming 10% reagent makeup), with the carbonate precipitation step contributing 34–78% of total costs. The TEA highlights that acid–base recycling is essential for scaling the pH-swing process on mine tailings and should be a research priority to enable gigatonne-scale CO₂ storage by mid-century. Additionally, selectively recovering critical minerals in wastes where magnesium and calcium are not exclusively leached could significantly offset capital costs.

High-efficiency solar cell architectures, including silicon heterojunction (SHJ) and perovskite/silicon tandems, rely heavily on the unique properties of transparent conducting oxides (TCOs). The push towards terawatt-scale PV manufacturing means it is increasingly desirable to develop indium-free TCOs to facilitate the upscaled manufacturing of high-efficiency cell designs. Aluminium-doped ZnO (AZO) deposited by atomic layer deposition (ALD) has emerged as a promising candidate due to its combination of optical transparency and electrical conductivity. In addition, AZO has also been shown to passivate the c-Si surface. The ability for one material to provide all three properties without requiring any indium is advantageous in single junction and tandem solar devices. Herein, we demonstrate exceptional silicon surface passivation using AZO/AlO_x stacks deposited with ALD, with a J₀ < 1 fA cm⁻² and corresponding implied open circuit voltage (iV_OC) of 740 mV. We provide a comprehensive analysis of the role of ALD precursor dosing to achieve optimised performance. A broad range of characterisation approaches were used to probe the structural, compositional, and chemical properties of AZO films. These indicated that the passivation properties are governed by a delicate interplay between the Zn and Al concentrations in the film, highlighting the importance of precise process control. Optical modelling in a single junction SHJ architecture indicates these AZO films are close in performance to high-mobility indium-containing TCOs. The insights provided by this work may help to further the case of indium-free TCOs, which is critical for upscaled production of high-efficiency solar cells.

Hybrid supercapacitors (HSCs), incorporating the benefits of batteries and supercapacitors (SCs), have drawn significant research attention. In this regard, metal oxides and metal–organic frameworks (MOFs) have emerged as standout contenders for electrode materials because of their varying oxidation states, redox-active nature and immensely high porosity along with large active site ratios. Here, we fabricated praseodymium sesquioxide (Pr₂O₃) in combination with C₁₈H₆Cu₃O₁₂ MOF and compared their composites in different weight ratios. Through three-electrode characterizations, the composite with the same weight ratio revealed a remarkable specific capacity of 2046 C g⁻¹, showing enhanced performance because of the proper utilization of C₁₈H₆Cu₃O₁₂ porosity and the chemical activity of Pr₂O₃. This composite (Pr₂O₃/C₁₈H₆Cu₃O₁₂) was subsequently combined with activated carbon in a hybrid device, and numerous electrochemical characterizations were further performed. Based on the outcomes, the device demonstrated a maximum specific capacity of 310 C g⁻¹, along with energy and power densities of 67 W h kg⁻¹ and 6114 W kg⁻¹, respectively, and a capacity retention of 98%. After careful evaluation of the device, two different models were applied to estimate the approximate capacitive and diffusive contributions of the device. These findings highlight the potential of the study for future usage in battery-supercapacitor systems.

Waste Tagetes erecta (Marigold) yellow-coloured flowers comprising carbonaceous biomass and organic pigment carotenoids are utilised for enhanced solar hydrogen generation through water splitting. The carbonaceous moiety of floral biomass, acting as a substrate is oxidised, makes uphill water splitting thermodynamically easier and improves the hydrogen production rate. Carotenoid, having visible light absorption and charge separation capability, acts as a photosensitizer when hybridised with semiconductors. A carotenoid–CdS nanohybrid photocatalyst exhibits an enhanced photocatalytic activity of 15 mmol g⁻¹ h⁻¹, almost three times that of pristine CdS (5 mmol g⁻¹ h⁻¹), when tested for hydrogen generation via water splitting under the full-band solar spectrum. The activity is further enhanced to 35 mmol g⁻¹ h⁻¹ (∼7 times that of pristine CdS) when the Tagetes erecta–CdS photocatalytic system is used for water splitting. An AQE of ∼17% is achieved using 420 nm of visible light.