Advanced Sustainable Systems最新文献

Piezocatalysis has emerged as a promising field of research that uses mechanical energy to drive a chemical change. There is growing evidence that piezocatalysts can perform challenging chemical conversions from organic transformations to water splitting. A key challenge to piezocatlaysis is mitigating the inherent high relative permittivity of a ferroelectric material. This high permittivity restricts the transfer of carriers required for a chemical reaction to occur and reduces the reaction rate. Here the concept of producing a co-catalyst system is taken to enhance carrier mobility increasing the observed reaction rate. The study highlights the importance of determining the sonochemical and piezocatalytic contributions to catalysis. The combination of a Pt metal co-catalyst with BaTiO₃ through a simple solid-state method led to a four fold increase in the rate of H₂ production compared to BaTiO₃ and sonochemical reactions in the absence of a catalyst. BaTiO₃/Pt is found to exhibit stable piezocatalytic performance over 12 h. Where there is a deviation from steady-state water splitting, it is shown that this is due to mechanical removal of Pt rather than a phase change in the catalyst system. This work confirms the additive benefits of hybrid materials for improving piezocatalytic processes.

Macroscopic 3D-controllable graphene (3D-CG) architectures not only retain the intrinsic properties of graphene sheets but also exhibit structural advantages for pollutant adsorption and energy storage. This paper proposes a novel hybrid powder-based additive manufacturing method to fabricate 3D biomass-derived laser-induced graphene (3D B-LIG) structures with customizable geometries and microporous features. This method utilizes two waste sources as feedstock precursors for sustainable graphene production: “black liquor” (sodium lignosulfonate, NaLS) and “white pollution” (polypropylene, PP). Employing a computer-aided design process, this method allows for the synchronous creation of various freeform macrostructures, with either identical or variable sections. To optimize the formability and processing efficiency of 3D B-LIG, systematic studies have been conducted. These studies establish the relationship between processing parameters and the resulting structures by controlling the laser parameters and the mixing ratio of NaLS and PP. By leveraging tunable microporous structures with a maximized specific surface area of 485.3 m² g⁻¹, 3D B-LIG demonstrates exceptional performance in pollutant adsorption (with a maximum adsorption capacity of 283.3 mg g⁻¹ for methylene blue) and energy storage (with a gravimetric specific capacitance value of 194.9 F g⁻¹).

Free-standing, highly transparent and flexible films are obtained from solvent casting of aqueous colloidal dispersions of surface-deacetylated chitin nanocrystals. The Young's modulus and the water absorption of the films is further modulated by the addition of three natural polyphenols, i.e., epigallocatechingallate, tannic acid and one lignosulfonate, which differ one another in terms of molecular weight, and overall amount of hydroxy, phenolic and catecholic functionalities. The polyphenolic molecules create an extensive network of hydrogen bonds with the nanocrystals, thus controlling interfacial interactions. Therefore, they act as crosslinkers exerting a reinforcing and structuring action and hampering water absorption. The films do not show dissolution in water upon 7 days of incubation at room temperature, and the release profiles of the polyphenols in aqueous media evidence hindered Fickian diffusion kinetics confirming the presence of interactions with the nanostructured matrix. Lastly, the developed films possess bioactive properties, as they show both radical scavenging and antimicrobial activity. These characteristics are enhanced by the phenolic and, most importantly, catecholic moieties present in tannins (and to a lesser extent in lignins), allowing to reach bactericidal effects as high as 99.99% against both Gram-positive and Gram-negative strains.

With a high theoretical gravimetric capacity of 3579 mAhg⁻¹, silicon (Si) has made a promising claim as an alternative to graphite (372 mAhg⁻¹) in lithium-ion battery (LIB) anodes as an active material. Unfortunately, inherent failure mechanisms (pulverization, delamination, promoting thick interphase formation, and non-conducting nature) of Si anodes have plagued their way toward commercialization. To stabilize Si anodes, this work reports the design, synthesis, and application of a conducting/crosslinked poly(BIAN) (P-BIAN) as a polymer binder for Si anodes. Theoretical evaluation of crosslinked P-BIAN and electrochemical characterization of anodic half-cells show that the crosslinked P-BIAN exhibits its versatility by a) administering mechanical robustness to stabilize Si particles, b) undergoing n-doping owing to the low-lying lowest unoccupied molecular orbital (LUMO) to tailor a thin solid-electrolyte interphase (SEI), and c) maintaining electrical conductivity. This inspired Si anodes to show a high reversible capacity of ≈2500 mAhg⁻¹ for over 1000 cycles with 99.1% capacity retention at 500 mAg⁻¹ current-rate.

This paper examines the chemical characteristics of four plant-derived bio-oils, including waste cooking oils, to address a research gap concerning their effects on the thermal stability and moisture susceptibility of asphalt. While bio-oils are known to soften asphalt, their specific impact on these properties is less understood. The study evaluates four different bio-oils (B1–B4) derived from various waste vegetable sources to determine their influence on asphalt performance. The findings indicate that bio-oils with higher purity and lower polyunsaturated fatty acid content offer better resistance to heat and UV-induced degradation. Bio-oils with lower iodine values also show improved resistance to moisture damage. Notably, bitumen composites containing bio-oil B2 do not negatively affect asphalt's moisture resistance, while others increase its moisture susceptibility. Tests with liquid anti-strip agents reveal that silanes and amine-based agents are the most effective at reducing moisture damage. These results underscore the importance of selecting bio-oils with low acid and iodine values, low polyunsaturated fatty acid content, and high purity for use in asphalt. This study supports sustainability and resource conservation by recommending bio-oils that preserve the durability of bio-modified asphalts.

The electrochemical reduction of nitrite (NO₂⁻) contaminants to ammonia (NH₃) is a sustainable and energy-saving strategy for NH₃ synthesis. However, this multi-electron reduction process requires an efficient electrocatalyst to overcome the kinetic barrier. Herein, the Pt₂Cu₁ nanooctahedrons are synthesized through a liquid-phase chemical reduction process. The synergistic effect of bimetallic Pt and Cu sites in the Pt₂Cu₁ nanooctahedrons is indispensable for accelerated NO₂⁻ hydrogenation, originating from the strong hydrogen-atoms adsorption capacity at Pt site and the strong NO₂⁻ adsorption capacity at Cu site. Specifically, the introduction of Pt sites can accelerate the accumulation of hydrogenated species on the catalyst surface, which promotes the formation of NH₃. In 0.5 m Na₂SO₄ solution, the Pt₂Cu₁ nanooctahedrons can reduce NO₂⁻ to NH₃ at a yield of 4.22 mg h⁻¹mg_cat⁻¹ and a Faraday efficiency of 95.5% at a potential of −0.14 V versus RHE. Meanwhile, the Pt₂Cu₁ nanooctahedrons also exhibit excellent activity for the sulfion oxidation reaction (SEOR). Using Pt₂Cu₁ nanooctahedrons as bifunctional electrocatalyst, a coupled electrolysis system combining the nitrite electrochemical reduction reaction (NO₂⁻ERR) with the SEOR requires only 0.3 V total voltage, enabling energy-saving electrochemical NH₃ production and collective value-added recovery of nitrite and sulfion waste.

Solid composite electrolytes (SCEs) have attracted serious attention for solid-state Li metal batteries. In particular, SCEs that incorporate inorganic sulfide into polymer electrolytes provide a feasible approach to address the air sensitivity and (electro)chemical instability of sulfides. Nevertheless, there is still little research on pairing sulfide-SCEs with high-voltage cathodes. In this work, reports on efforts to synthesize and compare SCEs that embedding sulfides (Li₇PS₆ and Li₃PS₄) into PVDF/HFP polymer using a strong polar solvent (DMF). Two sulfides show distinct behaviors when dispersed in the DMF solvent. The Li₇PS₆-SCE exhibits an ionic conductivity of 2.5 × 10⁻⁴ S cm⁻¹ at room temperature, higher than the Li₃PS₄-SCE (1.75 × 10⁻⁴ S cm⁻¹). Moreover, Li₇PS₆-SCE displays better electrochemical cycling performance in solid-state Li metal batteries with LiNi_1/3Mn_1/3Co_1/3O₂ (NMC 111) cathode.. When increasing upper cut-off voltages from 4.0 to 4.4 V, Li| Li₇PS₆-SCE |NMC111 cells deliver higher discharge capacities but exhibit worse cycling stability. Interface analysis using X-ray photoelectron spectroscopy (XPS) reveals the formation of LiF under a high voltage of 4.4 V, while t not present with 4.0 V. This work explores the synthesis of SCEs with different sulfides in a strong polar solvent and highlights the interface reactions between sulfide/PVDF-HFP SCEs with oxide cathodes.

Improving food preservation technologies is a key aspect in the struggle to reduce global food waste, and natural antimicrobial substances, such as essential oil (EO) components represent very promising food preserving agent. However, their intrinsic chemico-physical properties, such as the low melting point, low water solubility and high volatility, pose some practical difficulties in exploiting them for practical applications. Cocrystallization is used to stabilize liquid or volatile EO components providing them whit a crystalline environment, thus improving their potential application as antibacterial agents. Five EO active ingredients (THY = thymol, CAR = carvacrol, EUG = eugenol, CAD = trans-cinnamaldehyde, and VAN = o-vanillin) and two coformers (INA = Isonicotinamide, and HBA = 4-hydroxybenzoic acid) have been combined and the corresponding cocrystals have been studied for their potential inhibiting effect against four food spoilage bacteria (Bacillus thuringiensis, Enterobacter cloacae, Pseudomonas fluorescens, and Serratia marcescens). The structures of the five cocrystals have been used to derive structure-activity relationships in terms of release energy of the active ingredients form the crystalline environment, and a correlation has been derived with the Intermolecular Interaction Energies of the EO molecules.

Cerium-containing titania nano-octahedra (CeTNOh) are obtained by ultrasonication-hydrothermal synthesis of Ce-containing titanate nanowires (0.35, 0.46, and 0.70 Ce mol %) from commercial TiO2 (Degussa P25). CeTNOh are tested as photocatalysts to degrade a target pollutant (ciprofloxacin) under simulated solar light and at mild conditions. CeTNOh are anatase polymorphs with increasing crystallite size as Ce content increases. Hydrothermal treatments enhance the specific surface area (SSA) compared to P25, although Ce addition slightly reduces SSA while increasing crystallite size. Electron Microscopy confirms the morphology, although higher Ce levels hinder a full transformation. X-ray photoemission spectroscopy (XPS) shows the presence of Ce³⁺/Ce⁴⁺ redox pair, promoting electron mobility and Ti-Ce interactions. Optical and electronic spectroscopy reveals that Ce loading reduces the bandgap from 3.20 to 2.74 eV, extending light absorption into the visible range, thus enhancing the photocatalytic activity. The best sample, CeTNOh0.35, achieved 83% degradation of ciprofloxacin after 360 minutes under solar irradiation, with poor adsorption in the dark period. Higher Ce loadings negatively affect photoactivity by partially covering titania active sites. Reusability tests confirm the stability and efficiency of CeTNOh0.35 over three cycles, highlighting the importance of octahedral morphology in Ce-containing systems to boost the final photoactivity for water remediation.