Green Chemistry最新文献

Rechargeable aluminum-ion batteries (AIBs) are promising candidates for next-generation energy storage, yet their practical deployment is hampered by the intrinsic limitations of conventional ionic liquid (IL) electrolytes, such as high viscosity, corrosivity, and moisture sensitivity. This review focuses on the core role of IL electrolyte design in enabling highly reversible aluminum metal anodes. First, the fundamental requirements and working mechanisms of ILs are systematically elucidated. Furthermore, recent optimization strategies are critically summarized and discussed in terms of four aspects: (1) cation-anion pair engineering to regulate active aluminum species, tailor physicochemical properties, and reduce reliance on costly imidazolium-based components, (2) functional additives to enhance ion transport and regulate solid electrolyte interphase (SEI) formation, (3) deep eutectic solvent formulations as potentially lower-cost and more sustainable alternatives, and (4) gel and quasi-solid-state architecture construction to improve safety and mechanical strength. Finally, the performance-sustainability trade-offs of current IL electrolyte systems are discussed, and design guidelines are provided for developing safer and more sustainable electrolytes with high ionic conductivity, wide electrochemical windows, and robust interfacial compatibility. These advancements are expected to facilitate the realization of highly reversible aluminum metal anodes and high-energy-density AIBs, thereby propelling the development of next-generation aluminum-based energy storage technologies.

Poly(butyl cyanoacrylate) microbubbles (PBCA MB) are clinically investigated ultrasound-responsive materials whose formation is governed by surfactant-mediated interfacial templating. Here, we used a chemically diverse panel of 14 commercially designated greener non-ionic surfactants to clarify how surfactant chemistry governs PBCA MB formation and performance. By combining physicochemical analysis, dissipative particle dynamics simulations, microscopy, drug-loading experiments, and acoustic characterization, we determined how the architecture of the hydrophobic moiety, PEG chain length, and hydrophilic-lipophilic balance shape MB yield, shell composition, morphology, and function. The hydrophobic tail structure primarily influenced MB yield, while increasing PEG chain length shifted the morphology toward asymmetric particles. Surfactant incorporation into PBCA MB shells depended on surfactant hydrophilic-lipophilic balance, and dissipative particle dynamics simulations indicated preferential surfactant enrichment at the polymer-water interface. Brij O20 and Ecosurf SA-9 increased drug loading by 6.2- and 4.8-fold relative to conventional Triton X-100-generated MB, while acoustic performance could be tuned toward either greater stability or stronger non-linear, disruption-prone behavior. Together, these findings clarify the role of surfactant chemistry in PBCA MB synthesis and promote surfactant design as a practical route to tailor MB morphology, shell composition, drug loading, and acoustic performance.

Co-electrolysis of CO₂ (CO₂E) and water enables the production of syngas for sustainable aviation fuels (SAF) that are compliant with European RFNBO (renewable fuels of non-biological origin) regulations. However, a mismatch exists between the intermittent renewable electricity supply and the continuous operation of the downstream Fischer-Tropsch plants. To address this, we developed a two-stage linear optimization model to optimize the operation of a 540 MW electrolysis plant, alongside the sizing and operation of the connected renewable generation, battery storage, and syngas storage. Applying this model to a Dutch case study, we explored grid integration with an electrolyzer across future scenarios with global warming potentials (GWPs) ranging between 35 and 370 g CO₂-eq per kWh. For generation, the preferred renewable mix is onshore wind combined with PV. When grid mix electricity consumption is restricted, the electrolyzer has an optimal capacity factor of 78% but requires a battery of comparable capacity to the electrolyzer and multi-kilotonne syngas storage to ensure continuous output. Crucially, we found that producing RFNBO-compliant syngas for SAF is impossible with the 2025 Dutch grid mix. Even at a reduced grid intensity of 205 g CO₂-eq per kWh, RFNBO compliance limits grid consumption to just 1% of grid mix electricity per hour. This results in a levelized cost of 2350 EUR₂₀₁₉ per tonne syngas. Unrestricted grid electricity consumption becomes feasible when emissions drop below 36 g CO₂-eq per kWh, reducing production costs by 43% (1344 EUR₂₀₁₉ per tonne syngas). Consequently, we demonstrate that grid composition intensity is a bottleneck for the short-term economic viability and regulatory compliance of CO₂E-based SAF in the Netherlands.

Xylochemicals, bio-based platform molecules isolated from wood-based waste streams, have been of particular interest to those in the paints and coatings industry seeking to increase bio-based content in their products. This tutorial review provides an introduction to the area, and covers recent advances across three key platforms: furfural and 5-hydroxymethylfurfural, vanillin, and cardanol derivatives, as well as an overview of other lignocellulosic platform molecules currently under investigation.

Fully recyclable waterborne acetal thermosets were synthesized via the condensation of sorbitol and glutaraldehyde, utilizing oxalic acid as a green and in situ decomposable catalyst. Via a simple one-pot polycondensation in water the catalyst-free densely crosslinked networks are formed, combining high mechanical performance (tensile strength >90 MPa), stiffness (Young's modulus 3.3 GPa), and excellent thermal and solvent stability. While the materials remain fully stable under neutral conditions, the acetal linkages enable complete depolymerization under acidic environments, producing a homogeneous solution that can be recondensed into new thermosets with properties indistinguishable from the original, thus achieving true closed-loop recycling. The resins also exhibit outstanding compatibility with glass and carbon fibers, enabling the fabrication of high-performance, recyclable composites from which pristine fibers can be recovered. Together, these results establish waterborne, bio-based acetal chemistry as a scalable and sustainable platform for high-performance thermosets and fiber composites, offering a practical and circular route toward next-generation materials design.

Chemical recycling of plastic waste will play a key role in both decoupling the plastics economy from fossil feedstocks and addressing growing global plastic pollution. Real-world plastic waste streams, however, are complex and heterogeneous, which presents a serious challenge to established chemical recycling methods. Here, we present a series of zinc complexes that show high activity for the chemical recycling of poly(lactic acid) (PLA), bisphenol A polycarbonate (BPA-PC), and poly(ethylene terephthalate) (PET). Crucially, the most active of these catalysts is capable of selectively deconstructing a mixed feed of these polymers in succession with selectivity governed by careful modulation of reaction temperature. This sequential approach allows for the products of each reaction to be isolated in high yields without the need for complex separations. Further, high activity is demonstrated for the direct depolymerization of PLA to lactide. This work demonstrates the feasibility of sequential chemical recycling of mixed plastic waste as a tool for a more circular plastics economy.

Benzyl ethers are among the most robust and indispensable protecting groups in the synthesis of complex natural products and pharmaceuticals, providing effective neutralization of the reactive hydroxy group in phenols and alcohols. However, their cleavage necessitates the use of expensive catalysts, hazardous conditions, or excessive organic additives. Herein, we report a catalyst-free, photoinduced debenzylation protocol of phenolic and aliphatic ethers. By leveraging in situ generated solvent-anions as the reductant, the protocol achieves chemoselective debenzylation in the presence of alkenes, amides, carbamates, alcohols, and boronic esters in high yields under mild conditions. This strategy circumvents the need for costly hydrogenation catalysts or toxic reagents, providing a sustainable and economically viable alternative for debenzylation.