Sustainable Energy & Fuels最新文献

The energy transition, alongside sufficiency measures, demands massive electrification supported by low-carbon electricity. However, carbon-based molecules will remain vital, especially in sectors like long-distance transport (aviation and shipping) and chemicals. Biogenic, atmospheric, or recycled carbon sources offer key alternatives to fossil fuels in the shift toward a circular carbon economy, aligning with sustainability goals like the Renewable Energy Directive (RED III). Based on 183 case studies, this work analyzes thermochemical conversion processes for fuel production, using lignocellulosic biomass, CO₂, and low-carbon hydrogen from electrolysis. Nine biofuel, e-fuel, and e-biofuel processes are evaluated, producing liquid hydrocarbons, synthetic natural gas, or methanol. Material and energy balances, determined using ProSimPlus®, compare carbon conversion and energy efficiency. Economic analysis estimates investment and production costs for industrial-scale units, while greenhouse gas (GHG) assessment considers different electricity mixes and biomass supply chains. The results show that substituting biomass with hydrogen improves carbon conversion: from 35–40% for biofuels to 65–70% for e-biofuels, and up to 80–85% for e-fuels with carbon capture. Hybrid energy sources boost energy efficiency for e-biofuels (61.3%) compared to biofuels (50.3%). However, using electricity (100 € per MWh) raises production costs, which are heavily dependent on electricity price assumptions. Aligning e-fuel and e-biofuel production with RED III requires a largely decarbonized electricity mix, while more comprehensive emission assessments are necessary for biofuels and e-biofuels, considering potential land-use impacts of massive biomass production.

A novel sustainable synthesis strategy for producing a range of structurally distinct zeolites, specifically Zeolite 4A, Zeolite 13X, and Zeolite Y, is presented. This method avoids organic templates (commonly used for many high-silica zeolites such as ZSM-5, Beta, or high-silica Y) and directly produces Zeolite 4A, Zeolite 13X, and Zeolite Y from natural bentonite clay without the need for synthetic silica or alumina sources and thus offers a much more environmentally-benign production strategy than existing commercial synthetic routes. By systematically tuning alkaline fusion conditions and hydrothermal crystallization parameters, selective zeolite phase formation is achieved: lower fusion temperatures and NaOH/clay ratios favor the formation of LTA-type Zeolite 4A, while higher values promote the formation of FAU-type Zeolite 13X and Zeolite Y. The synthesized zeolites demonstrated structural characteristics and adsorption performance comparable to their commercial counterparts. Zeolite 13X exhibited the highest CO₂ adsorption capacity, attributed to its elevated microporosity and sodium content, while Zeolite Y showed enhanced hydrothermal stability and reduced water affinity, resulting from its higher Si/Al ratio and lower cation density. Water vapor adsorption isotherms and repeated cycling tests revealed clear differences in hydrothermal stability between the synthesized zeolites. A cradle-to-gate life cycle assessment (LCA), performed for Zeolite 13X as a representative product, revealed a ∼90% reduction in global warming potential (2.48 vs. 24.25 kg CO₂ eq. per kg), over 95% lower cumulative energy demand, and significantly decreased ecotoxicity and human toxicity indicators when compared to conventional chemical synthesis. Additionally, cost-oriented economic analysis showed that the clay-based synthesis route reduces the production cost of Zeolite 13X by approximately 33% compared to conventional chemical synthesis. Overall, this work provides a mechanistically informed, environmentally friendly framework for the phase-selective synthesis of industrially relevant zeolites from natural clay.

Graphitic Carbon Nitride (GCN) has garnered significant attention in recent decades as a potential candidate for various photocatalytic activities due to its ability to respond to visible light and its broad range of potential applications. Despite its high chemical stability, suitable band gap, rapid accessibility and unique layered structure, GCN suffers from several limitations, including fast recombination rate, carrier separation of charge and partial visible light absorption, that make it unsuitable for further applications. Researchers are focused on tuning the electronic structure of GCN by altering its morphology via interaction with other highly conducting materials or by doping at its structural defects. This review presents the elaborate history of the introduction of GCN, provides an overview of the structure and morphological properties of GCN, and focuses on the variety of synthesis techniques of GCN composites using chemical and biological methods. Finally, the photocatalytic applications of GCN composites for both environmental and energy applications are discussed. Environmental applications include water remediation, adsorption of waste materials, disinfection and removal. Energy applications involve water splitting, CO₂ reduction and H₂O₂ production. Alternative applications like organic transformation reactions are also briefly discussed in this review.

Vacancy and strain engineering have been identified as effective approaches for modulating the oxygen evolution reaction (OER) activity of electrocatalysts. Applying external fields like magnetic and light fields to electrocatalysts is also a potential approach to enhance the OER activity. However, the influence of the dual magnetic and light fields on the OER performance of electrocatalysts subjected to both vacancy and strain engineering remains unexplored. Herein, we rationally prepared epitaxial single-crystal LaNiO₃ (LNO) thin films as model electrocatalysts on LaAlO₃ (LAO) substrates under different oxygen pressures via pulsed laser deposition (PLD), obtaining LNO thin films with compressive strain and tunable oxygen contents. It is found that a volcano-shaped relationship exists between the OER activity and the oxygen content. This relationship originates from the synergistic modulation of both the Ni²⁺/Ni³⁺ ratio and the d-band center position in the LNO thin films. Furthermore, the LNO thin films exhibit a higher OER activity under dual magnetic and light fields compared to those under no external fields, irrespective of their oxygen content. The enhanced OER activity under dual magnetic and light fields primarily stems from the generation of photogenerated electron–hole pairs and the formation of triplet-state oxygen species, collectively reducing the energy barrier for the OER process.

The transition from pilot-scale to grid-scale hydrogen production via water electrolysis requires electrocatalysts that simultaneously exhibit high activity, durability, and scalability. Here, we report a hierarchically engineered two-dimensional (2D–2D) hybrid catalyst comprising NiMo-layered double hydroxide (NiMo-LDH) nanoflowers hydrothermally grown on highly exfoliated MXene nanosheets supported by a porous nickel foam. Scanning electron microscopy reveals an interwoven architecture in which NiMo-LDH nanoflowers are intricately anchored within delaminated MXene layers, effectively suppressing nanosheet restacking and maximizing active site exposure while facilitating rapid gas diffusion. The negatively charged surface terminations of MXene further enhance intrinsic activity by modulating interfacial electronic coupling and optimizing water molecule adsorption on NiMo-LDH. Benefiting from this synergistic design, the NiMo-LDH/MXene hybrid electrocatalyst achieves low overpotentials of 266 mV and 290 mV versus the reversible hydrogen electrode (RHE) at 50 mA cm⁻² for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively. At higher operational scales, the electrode delivers 200 mA cm⁻² at an overpotential of 373 mV for the HER and 320 mV for the OER, underscoring its capability for delivering industrially relevant current densities. The catalyst also exhibits robust long-term durability, sustaining stable operation for nearly 90 h and maintaining highly stable and low potentials of 3.24 V and 4.28 V at industrially relevant current densities of 300 and 1000 mA cm⁻², respectively. High faradaic efficiencies of ∼94% for the HER and ∼80% for the OER are simultaneously attained under alkaline conditions. This work highlights the rational integration of layered double hydroxides with conductive 2D materials as an effective route to enhance charge transfer, structural stability, and electrocatalytic efficiency, thereby offering a promising platform for next-generation water-splitting systems aimed at large-scale renewable hydrogen production.

Achieving high power conversion efficiency (PCE) remains a major challenge in the development of organic solar cells (OSCs). While non-fullerene acceptors (NFAs) have demonstrated significant progress, innovative molecular strategies are still required to overcome limitations in spectral coverage, charge transport, and interfacial energetics. Here, we propose a dipyran-centered molecular design approach and introduce seven novel asymmetric A–D–π–A NFAs, systematically engineered through terminal-acceptor modifications. Density functional theory (DFT) and time-dependent DFT (TD-DFT) methods have been adopted in both gas and solvent phases to evaluate their electronic, optical, and photovoltaic (PV) properties. Among the designed molecules, DP1 exhibits the narrowest HOMO–LUMO gap (E_g = 1.85 eV) and the lowest exciton binding energy (E_b = 0.30 eV), favoring efficient exciton dissociation. DP2 shows the most red shifted absorption (λ_max = 888 nm) along with the lowest electron reorganization energy (λ_e = 0.0040 eV), ensuring broad solar spectrum utilization and efficient charge transport. DP5 demonstrates the highest light harvesting efficiency (LHE = 0.999462) and strong oscillator strength (f = 3.269), while also achieving the highest fill factor (FF = 99.1%), indicating robust photon absorption and charge collection. DP7 delivers the highest open circuit voltage (V_oc = 1.71 V) with a strong fill factor (FF = 92.3%), providing excellent voltage headroom. Additionally, DP3 exhibits the largest dipole moment (11.417 D in solvent), which enhances intramolecular charge transfer (ICT) and polarity driven separation. Compared to the reference molecule R, all designed NFAs exhibit reduced E_g, red shifted λ_max, stronger ICT, and improved charge mobilities. Overall, this work highlights dipyran-based asymmetric NFAs as strong candidates for next generation OSCs and provides a theoretical framework for guiding the rational design of high efficiency PV materials.

This study investigated aluminum oxide (Al₂O₃) surface coatings on lithium nickel manganese cobalt oxide (NMC811) cathodes using a wet chemical process based on ethanol-dissolved aluminum ethoxide (Al(OEt)₃). Three coating concentrations, 1, 2, and 3 wt% Al precursor relative to the NMC811 mass, were synthesized and referred to as NMC811@AlO-1, NMC811@AlO-2, and NMC811@AlO-3, respectively. The workflow encompassed structural and surface characterizations of the coated samples, followed by electrochemical evaluation in half- and full-cell configurations. FTIR confirmed Al–O bond formation, while XRD and Raman spectroscopy verified that the NMC811 lattice structure remained unchanged after coating. Furthermore, transmission electron microscopy (TEM) and energy-dispersive X-ray spectroscopy (TEM-EDX) confirmed the successful deposition of the Al₂O₃ layer. Time-of-flight secondary ion mass spectrometry (ToF-SIMS) analysis revealed Al³⁺ ion diffusion into the grain interiors, indicating a potential impact on the electrochemical performance of the electrodes. Electrochemical tests showed that all the coated samples exhibited improved stability, with NMC811@AlO-3 (3 wt% coating) achieving the best capacity retention in half cells. In the second phase, full cells were formed using pre-lithiated graphite, graphene, and graphene oxide (GO) anodes, for which pre-lithiation conditions were optimized. Among all combinations, the NMC811@AlO-3/GO full cell demonstrated the highest initial discharge capacity (183 mAh g⁻¹) and the best cycling retention (80.1% after 250 cycles at C/2). These results suggest that a 3 wt% Al₂O₃ coating, combined with a GO anode, provides the most promising pathway toward high-performance full-cell systems.

A global imperative to meet net-zero targets by 2050 places immense pressure on the transport sector, a major contributor to greenhouse gas emissions. Low-carbon liquid fuels (LCLFs) offer a scalable solution for difficult to electrify or hydrogen-powered transport modes, such as heavy-duty freight, aviation, and shipping, due to their high energy density requirements and extended asset life. As “drop-in” replacements, LCLFs leverage diverse bio-based or synthetic feedstocks that are compatible with existing infrastructure, to minimise disruption and capital expenditure. This perspective examines the challenges inherent in scaling LCLF supply chains sustainably and cost-effectively. These include inelastic demand in heavy transport, constraints in feedstock availability and uneven refining capacity, and supply-side complexities like fragmented policy, inconsistent lifecycle emissions accounting, and stringent certification standards that limit blending. In assessing the readiness for LCLF among industries and countries we propose key aspects to unlock the potential of LCLF opportunities. We argue that scaling LCLF supply is a central driver for decarbonisation, requiring coordinated investment across all sustainable carbon sources, harmonised policy, and enhanced investment certainty. This integrated approach is essential to harness LCLFs' full potential for a resilient, low-carbon energy future.

Li-ion diffusion, intercalation, and de-intercalation are key challenges in lithium metal fluorosulfate for the evolution of the electrochemical properties of LIBs. Here, we addressed a novel and viable protocol for the evolution of the Li-ion migration and electrochemical properties of lithium metal fluorosulfate using first-principles calculations. The electronic properties of lithium metal fluorosulfate disclosed the band-gap tuning through Cr, Mn, and Ni substitution. The diffusion of Li ions from one octahedral position to another, following the one-dimensional pathway along the c-axis, was disclosed by the charge density and distribution analysis. The investigation of thermal properties unveiled the intercalation and deintercalation, which elaborated the chemical energy, structural changes, and spontaneous behavior. The Li/LFCS half-cell electrochemical properties predicted an average operating voltage of 4.99 V, and the oxidation and reduction potentials of Li/LFCS were 2.2 V and 1.95 V, respectively. The volumetric energy and power densities of the Li/LFCS half-cell were 1.15 W h cm⁻³ and 1.15 W cm⁻³, respectively. The gravimetric energy and power densities of the Li/LFCS half-cell were 3.109 kW h kg⁻¹ and 3.109 kW kg⁻¹, respectively. The theoretical capacity of Li/FCS was 220.3 mA h g⁻¹. The average voltage of the C₆/LFCS full-cell was 4.31 V. The calculated energy and power densities of C₆/LFCS were 3.109 kW h kg⁻¹ and 3.109 kW kg⁻¹, respectively.

The persistent challenges in designing lightweight, reversible hydrogen storage materials are addressed by utilizing a density functional approach and ab initio molecular dynamics (AIMD) analysis of newly proposed Li₃CX (X = S and Se) monolayers. The pristine monolayers exhibit robust thermodynamic stability, and upon the sequential adsorption of a maximum of six hydrogen (H₂) molecules, they achieve significant gravimetric storage capacities of 15.67 wt% for Li₃CS and 9.80 wt% for Li₃CSe. The average adsorption energy (0.22 eV) of the H₂ molecule lies within the ideal range of cyclable physisorption, facilitating reliable hydrogen uptake and release under room temperature. Desorption temperatures decrease predictably with surface coverage, reaching 281 K for 6H₂@Li₃CS and 346 K for 6H₂@Li₃CSe, indicative of low-energy release potential. These results underscore the practical viability of the Li₃CX monolayers as a high-capacity, thermally stable, and structurally resilient hydrogen storage medium for next-generation clean energy technologies. Our investigations provide valuable insights for experimentalists exploring two-dimensional monolayers with practical hydrogen storage capabilities.