ChemSusChem最新文献

2,5-Bis(hydroxymethyl)furan (BHMF) is a promising intermediate for the synthesis of pharmaceuticals and crown ethers, whereas achieving a high reaction rate in the hydrogenation of 5-hydroxymethylfurfural (5-HMF) to form BHMF remains challenge. In this work, a series of Cu/CeO₂–x catalysts (x denotes H, Air, Ar) were synthesized by calcination under different atmospheres (10% H₂/Ar, Air, Ar) and evaluated for the 5-HMF hydrogenation to BHMF. Cu/CeO₂–Ar exhibited a superior reaction rate of 26.8 mmol·g_cat⁻¹·h⁻¹ and BHMF yield of 99.1% under the condition (180°C, 5 h, 1 MPa H₂), significantly outperforming Cu/CeO₂–H and Cu/CeO₂–Air. The characterizations reveal that the calcination in the oxygen-deficient argon atmosphere led to high Cu dispersion and minimized Cu particle size in the Cu/CeO₂–Ar. These properties resulted in the abundant Cu⁺–O_V–Ce³⁺ sites and increased Cu⁰ number. In situ Fourier transform infrared spectroscopy analysis elucidates the distinct roles of these active sites. Cu⁺ sites are responsible for perpendicular adsorption of the 5-HMF carbonyl group, and Cu⁰ sites drive efficient H₂ dissociation. In contrast, the O_V–Ce³⁺ sites do not adsorb 5-HMF and H₂. The close synergy between numerous Cu⁰ sites and abundant Cu⁺ sites in the Cu/CeO₂–Ar accelerates the process of 5-HMF hydrogenation to BHMF.

The development of air-stable non-noble metal catalysts with high efficiency for hydrogen production from ammonia borane (AB) is crucial for advancing the hydrogen economy. In this work, Prussian blue analogs-derived air-stable Cu_xNi_y@NC/SiO₂ catalysts have been synthesized by a facile precipitation and thermal decomposition method. The optimized Cu₁Ni₆@NC/SiO₂ exhibits the best hydrogen production performance at room temperature, being 5 times more active than Cu₁Ni₆@NC and superior to other Cu_xNi_y@NC/SiO₂ catalysts. Beyond the reactivity, Cu₁Ni₆@NC/SiO₂ exhibits outstanding durability and antioxidant properties, maintaining its catalytic activity unchanged even after 6 months of air exposure. Characterization tools indicated that the enhanced performance and durability of the Cu₁Ni₆@NC/SiO₂ catalyst originated from a combination of the synergistic effect of Ni–Cu alloying and the core–shell structure. Moreover, Cu₁Ni₆@NC/SiO₂ also exhibits high efficiency and excellent recyclability toward the hydrogenation of adiponitrile and 2-methylglutaronitrile at ambient conditions on coupling with AB dehydrogenation. This research not only provides a simple strategy for the construction of air-stable non-noble metal catalysts for AB hydrolysis, but also offers a promising way for the design of heterogeneous non-noble metal catalysts with excellent oxygen resistance for industrial applications.

The growing energy shortages and environmental damage make it urgent to activate chemical reactions under mild conditions, reducing energy consumption and improving efficiency. Mechanocatalysis, with its advantages of simplicity, scalability, and sustainability, has demonstrated exceptional performance in many key heterogeneous catalytic reactions and surpassed traditional catalytic methods. It possesses significant potential for future applications and development. In this review, recent advances in the field of mechanocatalysis for energy and environmental applications are systematically summarized. Meanwhile, insights into the design of effective mechanical catalysts and the mechanocatalytic reactions, especially those with gaseous reactants, are highlighted and discussed in detail. Lastly, challenges and future perspectives in the mechanocatalysis are described to guide its broader application in the field of catalysis.

The growing transition from fossil fuels to renewable energy sources such as wind and solar requires efficient stationary energy storage systems to ensure grid stability. Among emerging technologies, redox flow batteries (RFBs) offer a promising solution due to their unique decoupling of energy and power capacities, allowing flexible system design. Recent advances in organic RFBs (ORFBs) have highlighted redox-active organic molecules as sustainable alternatives to conventional vanadium-based systems, addressing issues of cost and corrosivity. In particular, nitroxide radicals such as tetramethylpiperidinyloxyl (TEMPO) derivatives have demonstrated high reversibility and fast kinetics in aqueous systems, though the stability of their oxidized N-oxoammonium form remains a challenge for long-term storage. Isoindoline-based nitroxides offer potential for enhanced stability but have been limited by complex and low-yield synthetic routes. Herein, we present a convenient metal-catalyzed [2 + 2 + 2] intermolecular cycloaddition strategy for the synthesis of isoindoline-based nitroxides and their aza analogs, including two new candidates, TC-TMIO and PPO. Electrochemical characterization reveals that PPO, a cationic 2,3-dihydropyrrolo[3,4-c]pyridinium nitroxide, exhibits an oxidation potential 220 mV higher than the benchmark 4-TMA-TEMPO and achieves solubility exceeding 3 M in 1 M NaCl aqueous solution. Preliminary stability assessments of the PPO and RFB testing using a methyl viologen/PPO system demonstrate its potential as a high-performance, sustainable posolyte for aqueous ORFBs.

Membrane electrode assembly (MEA) systems hold promise as a technology capable of achieving high stability and current density for electrochemical CO₂ reduction (ECR). The fabrication techniques, including the selection of MEA components, the defined technological route, and the activation process, determine both the normal operation of the system and the proper performance of catalysis. Besides, the mass transfer of ions and water within the membrane directly impacts the local microenvironment, ultimately leading to variations in product distribution. In this article, we elucidate the characteristics and functionalities of each component within the MEA electrolyzers. Additionally, the fabrication techniques and activation processes of MEA are emphasized for their practical production. Besides, the developments and challenges of MEA for ECR are concluded, along with proposed solutions. Finally, we concentrate on the ions transport and water management within MEA, which directly impacts the availability of MEA electrolyzers and the distribution of products for ECR.

Polyethylene terephthalate (PET), despite its extensive use, presents serious environmental concerns due to inefficient recycling and inevitable downcycling. In this work, a sustainable one-reactor upcycling strategy is developed to directly convert waste PET into functional metal–organic frameworks (MOFs). Using a biocompatible betaine catalyst and adopting a single-reactionvessel strategy, this integrated process substantially improves reaction efficiency and scalability. The strategy is further extended to other polyester plastics, such as polylactic acid (PLA), enabling the synthesis of six MOFs (Zn-BDC, Ca-BDC, Ni-BDC, Co-BDC, Zn-LA, and Ca-LA) with excellent crystallinity and tunable morphologies. When incorporated into polyvinylidene fluoride (PVDF) composite films, the PET-derived Zn-BDC exhibits superior passive radiative-cooling performance compared with conventional MOF-5 composites, achieving high solar reflectance (≈94.4%) and mid-infrared emissivity (≈95.5%), which lead to an average temperature reduction of 9.3°C below ambient conditions. Overall, this streamlined and scalable upcycling route provides an economically viable bridge between sustainable plastic-waste valorization and next-generation energy-saving materials.

Thermosetting polymers feature highly cross-linked networks that are fundamentally distinct from those of thermoplastics. Even with similar cross-linking point, their three-dimensional architecture imposes significant mass transfer barriers and necessitates harsh, energy-intensive degradation conditions. Overcoming these limitations to achieve efficient and low-energy recycling of epoxy thermosets remains a major challenge. To address this challenge, this article developed a cosolvent-enhanced diethylenetriamine (DETA) catalytic system that enables rapid and efficient degradation under mild conditions. This approach achieved complete decomposition within 30 min at 60°C, significantly reducing time and energy consumption compared to conventional methods. The cosolvents accelerate degradation by disrupting the resin morphology to enhance mass transport and activating the amine catalyst through hydrogen-bonding interactions. This article provides a practical and sustainable pathway for recycling of thermosetting polymers, highlighting the potential of solvent-catalyst synergy in promoting circular polymer economies.

Solid electrolytes (SEs) have attracted considerable attention in applications such as energy storage systems and electrical devices due to their intrinsic safety and high energy density. Among them, layered oxide-based SEs exhibit high stability, reasonable ionic conductivity, and lower sintering temperatures compared with other oxide-based SEs. Nevertheless, the demand for higher ionic conductivity and lower synthesis temperatures still persists. To address these challenges, this work explores a substitution strategy for Na₂Zn₂TeO₆ (NZTO), which shows the highest ionic conductivity among layered oxide SEs. Iron (Fe³⁺), one of the most earth-abundant elements, is employed to partially substitute Zn²⁺ in NZTO to enhance both stability and performance. This approach successfully improves ionic conductivity and lowers sintering temperature. Specifically, the ionic conductivity increases significantly from 0.469 mS/cm in pristine NZTO to 0.850 mS/cm at 25°C with 0.1 Fe substitution, and a pure P2 NZTO phase is obtained at 750°C, compared with 900°C for pristine NZTO. Furthermore, a 12.9% capacity enhancement and improved stability are achieved when fabricating a solid-state cell with 0.1 Fe³⁺-substituted NZTO compared with pristine NZTO, confirming its potential for applicability in all-solid-state batteries.

The Cover Feature illustrates the bisguanidine organocatalyst-driven recycling of common polyesters, polylactide (PLA), polyethylene terephthalate (PET), and polycaprolactone (PCL). Three catalysts were evaluated in their ability to depolymerize PLA, with the most active demonstrating remarkable versatility and robustness in cascade recycling of polymer mixes and the valorization of post-consumer PET waste, thus highlighting a sustainable pathway toward a circular plastics economy. More information can be found in the Research Article by S. Herres-Pawlis and co-workers (DOI: 10.1002/cssc.202502062).

The Cover Feature illustrates a Li—Co dual-doped gadolinium-doped ceria (GDC) electrolyte that enables fast O²⁻ ion transport and low-temperature densification below 1000 °C. The schematic highlights enhanced grain connectivity, oxygen vacancy–assisted conduction, and their application in metal-supported solid oxide electrolysis cells for efficient hydrogen production. More information can be found in the Research Article by B. Amini-Horri and co-workers (DOI: 10.1002/cssc.202501679).