ACS Sustainable Chemistry & Engineering最新文献

Replacing the sluggish anodic oxygen evolution reaction (OER) with the value-added ethylene glycol oxidation reaction (EGOR) is a promising strategy for energy-efficient hydrogen production. However, achieving high Faradaic efficiency (FE) and selectivity, while elucidating the complex reaction kinetics and mass transport mechanisms coupled with the hydrogen evolution reaction (HER), remains challenging. Herein, a Mo-doped NiCo₂O₄ electrocatalyst, synthesized via a CTAB-assisted method, achieves >98% FE and >98% selectivity for ethylene glycol (EG) electrooxidation to formic acid (FA) at 100 mA/cm² in a three-electrode half-cell configuration. Density functional theory (DFT) reveals that Mo doping optimizes the electronic structure, thereby lowering the rate-determining step (RDS) energy barrier for selective FA production. An asymmetric flow field anion exchange membrane (AEM) flow electrolyzer was designed to overcome mass transport limitations, enabling a 143 mV reduction in cell voltage compared to conventional water electrolysis and stable operation over 30 h. In situ electrochemical impedance spectroscopy (EIS) with the distribution of relaxation times (DRT) quantitatively decouples ion transport, charge transfer, and mass transfer resistances under operational conditions. Systematic optimization of current density, flow rate, and EG concentration demonstrated synergistic regulation of kinetics and mass transport. This work provides a high-performance system for the co-production of green hydrogen and valuable chemicals and establishes a universal diagnostic framework for optimizing hybrid electrolysis systems.

Developing novel and sustainable processes for the production of bioplastics is crucial to addressing and mitigating the environmental challenges caused by the overconsumption of synthetic plastics. The old-fashioned linear “make-take-waste” consumption models are not environmentally sustainable and need to be transformed to circular systems to preserve natural resources. Therefore, in this study, we successfully recycled regenerated cellulose films into films and textile fibers via the Ioncell process. Films produced from dissolving pulp–ionic liquid (IL) solutions (cycle 0) were redissolved in ionic liquid to form recycled films and fibers within cycle 1. This process was repeated to showcase the recyclability of the cellulose within 2 recycling cycles. In both cycles, thin and highly transparent films have been produced that maintained the strength of the original films but improved the elongation at break (230–235 MPa, 10–13%). The fibers exhibit tenacities and elongations at break comparable to standard Ioncell fibers from virgin pulp (51.3–53.7 cN/tex, 9.2–11.6%). Additionally, a demonstration fabric was knitted from fibers of cycle 1. Overall, the results display the recyclability of the cellulosic films into high-quality products without any loss of quality.

Lithium iron phosphate batteries are widely adopted because of their cost-effectiveness. However, the large-scale recycling of these batteries is constrained by the economic and safety challenges posed by existing recycling technologies. Here, a sustainable and universal strategy based on low-temperature aqueous relithiation is proposed for LFP regeneration utilizing hydroxylamine sulfate as a mediator. The enhanced reductive environment created by hydroxylamine sulfate significantly lowers the Li⁺ migration energy barrier to lithium vacancies and enhances the repair of Fe_Li antisite defects at a reduced temperature of 40 °C, simplifying the operational process substantially. By combination with a short annealing step, the Li loss and structural degradation in LFP are effectively mitigated, enabling further restoration of electrochemical performance. Notably, the results of in situ X-ray diffraction (XRD) during the lithiation process reveal that the final step of complete lattice repair is a critical factor in controlling the lithium replenishment process. Furthermore, this process exhibits integration, sustainability, and universality, thereby overcoming the barriers to transitioning direct recycling from lab-scale to industrial applications.