Advanced Sustainable Systems最新文献

Synthesis of oxygenated MXene grafted MOFs structures and their enhanced characteristics have been found rare for supercapacitor applications. Herein, oxygenated MXene Mo₂CT_x (T_x = ─O, ─OH) and oxygenated MXene Mo₂CT_x nanosheets grafted CoBDC nanorods are synthesized successfully. Synergetically, oxygenated MXene Mo₂CT_x nanosheets grafted CoBDC nanorods exhibited the enhanced electrical conductivity of 12.90 µS cm⁻¹, specific surface of 70.20 m² g⁻¹ and pore diameter of 7.82 nm due to a good grafting of nanorods and nanosheets. Owing to enhanced characteristics, oxygenated MXene Mo₂CT_x nanosheets grafted CoBDC nanorods showed a strong redox reaction and exhibited a good specific capacitance of 1295.51 F g⁻¹, energy density of 54.43 W h Kg⁻¹ and power density of 3856.23 W Kg⁻¹, which is greater than pristine MXene Mo₂CT_x nanosheets and CoBDC nanorods. Oxygenated MXene Mo₂CT_x nanosheets grafted CoBDC nanorods retained a specific capacitance of 90.70%. An asymmetric system consisting of oxygenated MXene Mo₂CT_x nanosheets, grafted CoBDC nanorods, and activated carbon showed a potential window of 1.2 V, and energy and power densities are found as 17.68 W h Kg⁻¹ and 4105.92 W Kg⁻¹, respectively. Hence, it can be concluded that oxygenated MXene Mo₂CT_x nanosheets grafted CoBDC nanorods exhibited a good characteristics for supercapacitor applications.

Intensive agriculture and industrialization have caused soil contamination, deterioration, and reduced productivity, threatening agricultural sustainability. Petroleum hydrocarbons (PHCs) from natural and human-made sources have caused significant soil pollution and health hazards, prompting advanced research. However, due to cost and practical limitations, existing approaches have fallen short in effectively restoring soil health and productivity. Recent advancements in nanotechnology offer promising opportunities to enhance soil quality indicators, increase crop yield, and ensure environmental sustainability. Nanotechnology has gained attention in agriculture for developing sustainable technologies and strategies for environmental remediation. By utilizing nanomaterials, nanotechnology enables the creation of improved materials and products, particularly for remediation. Emerging approaches, like combining nanomaterials with biological processes, are recognized as effective for removing contaminants. Integrating nanomaterials with microorganisms enhances their functionality and promotes plant nutrient availability, thereby improving soil health. Nano-enhanced bioremediation is a successful method for addressing PHC contamination, enhancing the absorption and breakdown of pollutants, and reducing their accumulation and dispersion. This paper explores the role of nanomaterials in augmenting rhizoremediation of PHC-polluted soils. It examines the rhizosphere involvement in bioremediation and highlights the potential of nanotechnology in improving soil health. The interactions between nanomaterials and microbes are discussed, along with their mechanisms and applications.

Electrocatalytic CO₂ reduction reaction (CO₂RR) in acidic media attracts significant attention due to its ability to circumvent the low carbon utilization efficiency and system instability associated with carbonate formation in traditional alkaline/neutral systems. However, although high proton concentrations in acidic environments inhibit carbonate generation, they simultaneously intensify hydrogen evolution reaction (HER) competition and compromise the adsorption stability of key intermediates, thereby severely restricting CO₂ reduction selectivity and efficiency. Thus, it is a great challenge to effectively suppress HER and accelerate acidic CO₂RR. This review commences with an overview of recent progress in acidic CO₂ electrolysis, addressing the fundamental limitations hindering the use of acidic electrolytes. It subsequently systematically examines advanced strategies to overcome these challenges, encompassing the regulation of the electrolyte microenvironment, the role of alkali cations, surface and interface functionalization, nanoconfinement structural design, and the exploitation of novel electrolyzers. The conclusion proffers insights into emerging challenges and future research directions. It is anticipated that this timely endeavor could galvanize research efforts to mitigate CO₂ crossover, catalyze novel insights for resolving the “alkalinity problem”, and propel CO₂RR into a more sustainable and viable technology.

Lithium-sulfur (Li-S) batteries exhibit substantial potential as next-generation energy storage devices due to their high theoretical capacity (1675 mAh g⁻¹), low cost, and environmental friendliness. However, the practical application is hindered by the insulating nature of sulfur/lithium sulfide (Li₂S) and the polysulfide shuttle effect. Herein, hollow-structured Co-CoP (Co-CoP@HNC)and intercalated is successfully fabricated it into the interlayer spacing of 2D MXene(MX) nanosheets (Co-CoP@MX) to modify the separator for Li-S batteries. The Co-CoP@HNC intercalation expands the MX interlayer spacing, facilitating lithium ions (Li⁺) transport, while the polar Co-CoP@HNC acts as a catalytic center to accelerate polysulfide conversion. In addition, the built-in electric field (BIEF) between Co and CoP drives the directional transfer of adsorbed polysulfides from the CoP (strong adsorption) to the Co (high catalytic activity), thereby accelerating their conversion. Therefore, the battery with the Co-CoP@MX modified separator exhibits an initial capacity of 1356.77 mAh g⁻¹ at 0.2 C, maintains 979.77 mAh g⁻¹ at 1 C with a minimal capacity decay rate of 0.078% per cycle in 500 cycles, and achieves a high initial capacity of 751.08 mAh g⁻¹ under high sulfur loading of 8.36 mg cm⁻².

The global push for climate neutrality and circularity has intensified interest in converting plastic waste into valuable chemical feedstocks. This study examines the techno-economic feasibility of producing syngas from post-consumer plastic waste (PCPW) via chemical looping partial oxidation (CLPO) and compares it to more established syngas production techniques, namely dry reforming of methane (DRM) and gasification of PCPW. Process simulations are conducted in Aspen Plus, targeting a syngas stoichiometric number (SN) of 2.0, which is ideal for downstream Fischer–Tropsch synthesis. The CLPO process, conceptualized in a dual fluidized bed reactor setup, is modeled using literature data and compared to DRM and gasification in terms of capital and operational expenditures (CAPEX and OPEX). A detailed separation train is designed to meet severe syngas purity requirements, accounting for typical impurities present in process feedstocks. Results show that, although CLPO offers flexibility and avoids direct air separation, it suffers from high CAPEX and OPEX, leading to a significantly higher levelized cost of syngas (LCOS) of 616 € t⁻¹, compared to 503 and 494 € t⁻¹ for the DRM and gasification benchmarks, respectively. Sensitivity analyses highlight syngas selling price and reactor CAPEX as key economic drivers.

For the first time, the immobilization of Lewis base molecular catalysts is demonstrated on lignocellulosic bamboo shavings for synthetic applications, focusing on the valorization of CO₂ and its derivatives. Two types of catalysts are immobilized on bamboo shavings: covalent functionalization using isocyanate chemistry is employed to prepare Bamboo supported Hexaethylenedicarbamate ethyl methyl imidazolium iodide [Bamboo@HMEMIM][I], while a silane-based approach is applied to obtain Bamboo supported 1,5,7-Triazabicyclo[4.4.0]dec-5-ene [Bamboo@TBD]. Both materials are fully characterized through elemental analysis, FT-IR, TGA, and Scanning Electron Microscopy (SEM). The first catalyst, [Bamboo@HMEMIM][I], promoted the cycloaddition of CO₂ with epoxide, achieving 100% conversion and complete selectivity toward cyclic carbonates under optimized conditions (2.8 mol% catalyst, 10 bar CO₂, at 70 °C for 16 h). This catalyst also demonstrates good recyclability, showing a decrease in activity only after four consecutive cycles (74% yield in the fourth cycle, 61% in the fifth). The reaction scope demonstrates its broad applicability for other epoxides (Y = 86−100%). The second catalyst is applied to the synthesis of glycerol carbonate through cycloaddition between dimethyl carbonate (DMC) and glycerol. Optimized conditions (5 mol% catalyst, 10:1 DMC:glycerol ratio, at 100 °C for 16 h) achieves 100% conversion and 69% selectivity for glycerol carbonate. In this case the degradation of catalysts by Phanerochaete chrysosporium is investigated.

Lithium-ion batteries (LIBs) are pivotal energy storage technologies for achieving a low-carbon future. However, the exponential growth in global demand for LIBs has triggered dual crises: resource scarcity in battery production and environmental pollution caused by spent batteries. Developing green and sustainable recycling strategies for LIBs is therefore critical to addressing these challenges. Hydrometallurgy has emerged as a research focus due to its advantages in high leaching efficiency, high product purity, and low energy consumption. This review systematically summarizes recent advances in hydrometallurgical recycling technologies for spent LIBs. Key approaches cover reagent-assisted leaching (including reducing agent-assisted leaching, deep eutectic solvents (DES), oxidizing agent-assisted leaching); field-assisted leaching (including ultrasound, microwave, and electrochemistry); catalytic-assisted leaching (including photocatalysis, contact-electro-catalysis, and photothermal catalysis), and others (like supercritical fluid, mechanochemistry). In particular, the principles and challenges of catalytic leaching are discussed in depth, offering a roadmap for future industrial applications. By providing a comprehensive theoretical framework and practical insights, this review aims to advance hydrometallurgical recycling toward higher efficiency, sustainability, and environmental compatibility, thereby supporting the transition to a circular economy.

The booming industry of wearable electronics, IoT devices, and self-powered sensor networks is in critical need of sustainable and efficient mechanical energy harvesting devices. Among the new materials, lead-free perovskites have garnered significant interest due to their potential to address the environmental and toxicity issues associated with traditional lead-based systems, while offering good energy conversion and multifunctionality. This review discusses the state-of-the-art of lead-free perovskite materials in piezoelectric nanogenerators, triboelectric nanogenerators, as well as hybrid devices that use both of these working principles. Specific topics of interest cover material classes and synthesis routes, material properties and characterization, as well as energy harvester developments and their functionalization in various application fields. This review examines the device performance of various perovskite systems and identifies the most effective materials and evaluates their suitability for flexible, stretchable, and wearable applications. Challenges such as stability over long periods of time, scalability in processing, and enhancement of performance are severely discussed with suggestions for future studies. The study highlights lead-free perovskites as a game-changer to fabricate green and next-generation self-powered energy devices.

The development of highly active hydrogen evolution electrocatalysts is key to overcoming bottlenecks in hydrogen energy industrialization and advancing the hydrogen economy from laboratory research to large-scale application. However, Pt-based catalysts are confronted with challenges such as high cost and poor stability. Here, EDM-Co-MOF@Pt-Pd catalyst is synthesized via a simple two-step method utilizing Co-MOF as a sacrificial template. The in situ decomposed Co-MOF releases Co²⁺ and dimethylimidazole ligands into the solution. Under the action of cathode voltage, Pt and Pd are induced to preferentially nucleate at the defect sites on the surface of nickel foam through spontaneous substitution reactions, effectively improving the dispersion of Pt and Pd nanoparticles. Meanwhile, the d-band centers of Pt and Pd shift down, optimizing their adsorption of reaction intermediates. Under the combined effect of these two aspects, the HER overpotential of this catalyst at 10 mA cm⁻² is only 16 mV, which is superior to the existing noble metal catalysts. Moreover, after running for 120 h, the HER overpotential only increases by 11 mV, proving that the catalytic activity and stability have been significantly improved. It overcomes the tendency of traditional precious metal catalysts to aggregate and deactivate, resulting in superior stability and significant potential.

Single-atom Fe─N─C (Fe₁-N-C) materials represent advanced oxygen reduction reaction (ORR) catalysts in base, but insufficient oxygen evolution reaction (OER) performance severely limit their applications in rechargeable Zn─air batteries (ZABs). Herein, ultrasmall Fe cluster liganded Fe-N₄ sites (Fe_nc/Fe₁-N-C) are encapsulated within N-doped carbon hollow nanosheets through ZIF phase conversion and subsequent pyrolysis. The synergistic interplay between Fe clusters and closely surrounding Fe-N₄ active sites can collectively modulate the electronic structures and optimize adsorption energetics of reaction intermediates. Such Fe_nc/Fe₁-N-C hybrid catalysts not only exhibit excellent ORR properties but also deliver remarkable activities for low-potential iodide oxidation reaction (IOR), which can replace the high-potential and destructive OER to improve the energy efficiency and cyclability of ZABs. As a result, the Fe_nc/Fe₁-N-C hollow nanosheets achieve remarkable ORR performance with a high half-wave potential of 0.931 V versus reversible hydrogen electrode (RHE). When coupled with the IOR during charging process, the Fe_nc/Fe₁-N-C based hybrid battery exhibits an unprecedented charge/discharge voltage gap of only 0.51 V and sustains ultrastable cycling up to 450 h. Theoretical calculations reveal that the Fe cluster ligands can drive delocalization of the Fe d_z² orbitals of Fe-N₄ active sites to optimize the desorption step of the intermediates, thereby optimizing oxygen intermediate adsorption energetics.