Advanced Sustainable Systems最新文献

Nickel Nanoparticle Synthesis

Early-stage cost evaluation during catalyst development holds the potential to accelerate the commercialization and deployment of advanced catalytic materials for sustainable chemical processes. In article number 2300030, Frederick G. Baddour, Brittney E. Petel, and Kurt M. Van Allsburg, utilize CatCost, a free and publicly available estimation tool for the evaluation of catalyst manufacturing costs, to perform a cost-responsive optimization of the synthesis of nickel nanoparticles.

Molybdenum diselenide (MoSe₂), a 2D layered transition metal dichalcogenide, has garnered significant scientific research interest for its catalytic and electrocatalytic activities. Here, a straightforward hydrothermal procedure is used to synthesize MoSe₂ nanosheets (NSs) and focus on their adsorption capabilities and hydrogen evolution reaction (HER) activity. The MoSe₂ NSs which are synthesized by 12 h of hydrothermal treatment found to exhibit the highest adsorption capacity of 91.67 mg g⁻¹. The kinetics of the adsorption process have been found to follow the pseudo-second-order model, signifying chemisorption and multilayer adsorption as described by the Freundlich isotherm. The thermodynamic analysis further suggests that the adsorption proceeds by endothermic and spontaneous mechanisms. The self-cleaning property of the adsorbent is demonstrated by degrading the dye on the adsorbent-coated cotton fabric. The sample created using a 12 h hydrothermal method has been shown to have a minimal Tafel slope of 58 mV dec⁻¹. It also shows excellent HER activity at low over-potential and possesses long-term durability. The dual functionality of MoSe₂ NSs in both adsorption and electrocatalytic activity highlights their potential for application in environmental remediation and renewable energy production.

In the search for clean energy technologies, it is crucial to develop low-cost batteries with enhanced performance, and 2D materials are promising for electrode applications owing to their high surface area where fast ionic diffusion can occur. In this work, density functional theory calculations that demonstrate the great potential of recently synthesized 2D pyrite as a battery electrode are reported. An extensive analysis of its performance toward Li-ion batteries and post-lithium technologies (Na, K, Mg, Ca, Zn, Al), as well as how point defects can be leveraged to engineer its electronic properties are reported. First, the results explain that the main drawback of the unmodified material, namely its voltammetric peaks at high voltages, is due to the overly strong adsorption of lithium ions. Second, it is demonstrated that hydrogenation of the material leads to milder open-circuit voltages without compromising the capacity of the anode, and lowers the diffusion barrier to only 0.06eV for both Li and K ions. With a capacity as high as 1317 mAh g⁻¹ for Al-ion, hydrogenated monolayer pyrite is demonstrated to be a promising material for energy storage applications.

This study reports a visible light active Ba/Sc co-doped potassium niobate (KNbO₃) ferroelectric material for enhanced photocatalytic applications. Through 5% Ba and Sc co-doping in KNbO₃ (i.e., 0.95KNbO₃-0.05Ba(Nb_1/2Sc_1/2)O₃), the electronic band gap (E_g) is narrowed down to the visible range of the solar spectrum. The prepared samples are systematically examined by using X-ray diffraction and Raman spectroscopy, which confirms the successful incorporation of Ba and Sc ions into the KNbO₃ lattice. Scanning electron microscopy (SEM) and energy dispersive spectroscopy (EDS) analysis reveal particle morphology and chemical homogeneity of prepared samples. The UV–vis spectroscopy and ferroelectric PE-loop demonstrate enhanced optical absorption compared to host KNbO₃ while retaining ferroelectric behavior. The photoelectrochemical (PEC) measurements under visible light irradiation demonstrate a notable enhancement in the photocurrent for 0.95KNbO₃-0.05Ba(Nb_1/2Sc_1/2)O₃ (hereafter denoted by 5KBSNO) compared to undoped KNbO₃. Additionally, the 5KBSNO sample displays enhanced RhB dye degradation efficiency, reaching ≈50% compared to parent KNbO₃ (≈30%) under light irradiation. First-principles density functional theory (DFT) calculations are employed to understand the mechanism responsible for the reduced band gap. This study presents a promising material for developing advanced ferroelectric photocatalysts with tailored band structures for efficient solar energy harvesting for energy conversion and contamination remediation applications.

Driven by the advantages of hydrogen energy, such as environmental protection and high energy density, the market has an urgent demand for hydrogen energy. Currently, the primary methods for hydrogen production mainly include hydrogen generation from fossil fuels, industrial by-products, and water electrolysis. Seawater electrolysis for hydrogen production, due to its advantages of cleanliness, environmental protection, and ease of integration with renewable energy sources, is considered the most promising method for hydrogen production. However, seawater electrolysis faces challenges such as the reduction of hydrogen production efficiency due to impurities in seawater, as well as high costs associated with system construction and operation. Therefore, it is particularly necessary to summarize optimization strategies for seawater electrolysis for hydrogen production to promote the development of this field. In this review, the current situation of hydrogen production by seawater electrolysis is first reviewed. Subsequently, the challenges faced by seawater electrolysis for hydrogen production are categorized and summarized, and solutions to these challenges are discussed in detail. Following this, an overview of an in situ large-scale direct electrolysis hydrogen production system at sea is presented. Last but not least, suggestions and prospects for the development of seawater electrolysis for hydrogen production are provided.

In this work, sustainable Li-based battery separators are prepared starting from a waste material from the glass industry, viz. polyvinyl butyral (PVB) widely used as a sacrificial interlayer in high impact-resistant windows. First, polymeric membranes are prepared via the phase-inversion method using commercial PVB as the backbone and 4,4′-methylenebis(cyclohexylisocyanate) as a crosslinking agent. They are characterized from a physicochemical viewpoint by thermomechanical analysis, infrared spectroscopy, and scanning electron microscopy, and are successfully tested as separators in Li-metal cells with LP30 electrolyte. Electrical and electrochemical properties are evaluated by impedance spectroscopy and galvanostatic cycling, providing comparable results with commercial Celgard 25 µm monolayer microporous polypropylene separator. As a proof-of-concept, for the first time, recycled PVB-based polymer membranes from wasted car glasses are prepared, adjusting the synthesis protocol to account for the presence of plasticizers and contaminants. They show a dense elastomeric appearance and proved to be compatible with Li metal and stable upon 600 h of Li plating/stripping. The electrochemical window is compatible with the LiFePO₄ cathode, as demonstrated by prolonged galvanostatic cycling (250 cycles) in laboratory-scale cells. Preliminary results are highly encouraging and pave the way to developing novel separators for safe, low-cost, and sustainable energy storage devices.

Lithium hydroxide (LiOH) is rapidly becoming the main precursor for layered oxide cathodes used in lithium ion batteries. Current hydrometallurgical method for LiOH production uses substantial amounts of chemicals and creates wastes, leaving behind a negative environmental footprint. Electrodialysis is emerging as a more sustainable technology for LiOH production, effectively eliminating the conventional chemical addition step and its subsequent waste management. Additionally, hydrogen is generated as a by-product during the electrodialysis process. Various configurations of the electrodialysis cell have been employed to maximize the energy efficiency of the process and the purity of the LiOH product. Nonetheless, this review found that there is a lack of concerted effort in developing ion exchange membranes specific for LiOH production. Current membrane technologies are not tailored to LiOH production, with limited selectivity to lithium in relative to other monovalent cations, as well as relying heavily on harmful perfluoroalkyl (PFA)-based polymeric membranes. In this review, special attention is given to the state of the art in the testing and development of membranes, i.e., cation and anion exchange membranes, bipolar membranes, as well as novel membranes that are potentially low-cost, non-fluorinated, lithium-selective with high chemical stability and mechanical robustness.

Biocatalysis is a green and sustainable process for synthesizing chiral organic building blocks and active pharmaceutical ingredients (API). United Nations' Sustainable Development Goals 2030 advocates using green, sustainable, recyclable chemicals by industries to reduce environmental pollution. Pharmaceutical companies are adopting biocatalysis technologies for manufacturing chiral active pharmaceutical ingredients. The lipase-catalyzed kinetic and dynamic-kinetic resolution method is a pharmaceutically accepted process for manufacturing chiral API. This review describes the reported methods for synthesizing chiral API/KSM (Key Starting Material) molecules using lipase enzymes over the last ten years.

Highly porous carbon materials derived from renewable resources constitute a promising and sustainable strategy regarding the enhancement of CO₂ capture technologies. In this work, the valorization of Eucalyptus globulus wood, a forest invasive species present in European forests, is performed through its transformation in biochar. The deposition of nitrogen and different metals (aluminum, copper and chromium) onto biochar is performed, using the magnetron sputtering as a pioneering technique, to produce coated biochar nanoparticles with improved properties. The resultant modified biochar particles maintain a highly porous structure and present a remarkable CO₂ adsorption capacity (up to 4.80 mmol g⁻¹ for N@BC), which is attributed to the synergy of their large total surface area (527 m² g⁻¹) and microporosity (pore diameter = 21 Å), with a high content of nitrogen and oxygen heteroatom moieties (40.4% N, 11.4% O). Their application as heterogeneous bifunctional catalysts in CO₂ cycloaddition to epichlorohydrin is performed, in the absence of any solvent or co-catalyst, under moderate conditions (20 bar CO₂, 120 °C), leading to good conversions (up to 58% conversion) and excellent selectivity for cyclic carbonates. Cu-coated biochar is shown to be more stable than non-modified material, being recycled and reused along 4 consecutive runs without loss of catalytic activity or selectivity.

Sulfate radicals based advanced oxidation processes (SR-AOPs) have gained attention recently due to their high mineralization capability in environmental remediation. The high persulfate (PS) activation activity of cobalt-based semiconductors has epitomized them as preferred catalysts for SR-AOPs but shortcomings such as leaching, and loss of catalytic active sites limit their applicability. Herein, two different strategies are employed to minimize leaching and improve charge transportation and separation for efficient PS activation under visible light irradiation using LDH/CaCO₃/PS and Ba₂CoMnO₅/PS AOP systems synthesized by solid state method. LDH/CaCO₃/PS achieved 17.9% higher reaction rate than Ba₂CoMnO₅/PS for degradation of amoxicillin (AMX) with higher TOC mineralization efficacy. Despite SO₄^•− and OH^• existence and involvement in both systems, the degradation pathways mapped from QTOF-HPLC-MS data demonstrated formation of different pathways during AMX mineralization. This work demonstrates novel fabrication of brownmillerite double layered perovskite and insulator supported LDH for environmental pollution remediation.