The amine-functionalized Christian-Albrechts-University-1 (CAU-1) metal-organic framework (MOF) possesses intrinsic structural features ideally suited for hydrogen (H2) separation, with pore apertures closely matching the molecular size of hydrogen, thereby enabling selective hydrogen transport via molecular sieving. The physicochemical and structural tailoring of CAU-1 holds immense potential for gas separation thin-film nanocomposite (TFN) membranes yet it remains largely unexplored. This work presents the first systematic investigation of CAU-1 incorporation confined within a thin PMMA selective layer supported on a polysulfone (PSF) substrate, elucidating its influence on the interfacial structure, gas transport pathways, and hydrogen separation performance of polymethyl methacrylate (PMMA)/CAU-1 TFN membranes. Morphological analyses revealed the successful formation of thin, dense, and defect-free TFN exhibiting excellent polymer-filler compatibility with no observable interfacial voids, while thermogravimetric analysis demonstrated excellent thermal stability up to 360 degrees C. The optimized PMMA/CAU0.5 membrane achieved an H2 permeability of 294.43 Barrer, with ideal selectivities of 4.91, 6.30 and 5.03 against carbon dioxide (CO2), nitrogen (N2), and methane (CH4), respectively, representing respective improvements of 11%, 42%, and 51% over pristine PMMA. Under mixed-gas conditions, the H2/CO2 separation factor surpassed the Robeson upper limit indicating the effective H2-selective transport properties. These findings highlight the pivotal role of CAU-1 in creating microporous, H2-selective transport pathways, demonstrating the potential of PMMA/CAU-1 TFN membranes for enhanced hydrogen purification.
Reliable thermal runaway risk monitoring during electric vehicle (EV) fast charging requires models that capture short electrical transients and long thermal dependencies under changing operating conditions. Existing predictors often emphasise temperature accuracy but provide limited mechanisms for converting multivariate prediction errors into hierarchical online decisions. This study develops a hierarchical monitoring framework that combines a Convolutional Neural Network (CNN), a Bidirectional Nested Long Short-Term Memory (BiNLSTM) network, and an Adaptive Gating Fusion Mechanism (AGFM). The CNN branch extracts local fluctuations, the BiNLSTM branch represents long-range thermal evolution, and AGFM adjusts their contributions according to operating conditions. An adaptive sliding window then converts temperature-prediction residuals into three hierarchical warning levels using empirically calibrated severity thresholds. The framework is evaluated using four-season real-world Lithium Iron Phosphate (LFP) fast-charging data and auxiliary Newman, Tiedemann, Gu, and Kim (NTGK) electrothermal simulations of Nickel Cobalt Manganese (NCM) modules. On the real-vehicle data, the model achieves MAEs of 0.0311-0.0484 degrees C across seasons and an R2 up to 0.9989. At the second warning level, accuracy, precision, and F1-score reach 92.73%, 83.33%, and 86.21%, respectively. In abnormal charging cases, the first warning level provides 19.70-34.25 s of intervention time before protective cutoff. These results demonstrate a computational route from multivariate battery-state prediction to hierarchical online monitoring for safer fast-charging operation.
Acidic deep eutectic solvents combined with electrocatalysis enables green and efficient lignin depolymerization into value-added chemicals through hydrogen-bond activation and radical-mediated selective bond cleavage. In particular, the dual-acid DES composed of choline chloride, lactic acid, and acetic acid provides synergistic enhancement of both acidity and the hydrogen-bond network, thereby promoting lignin dissolution and facilitating more efficient bond cleavage during electrocatalytic depolymerization. However, conventional metal electrodes often suffer from severe electrochemical corrosion in dual-acid DES systems, which limits their practical application. Here, we design a corrosion-resistant RuO2-SnO2/Ti heterojunction catalyst for electrocatalytic oxidation of lignin in a choline chloride-lactic-acetic acid DES. Using 4-benzyloxyphenol as a model compound, the catalyst achieved 97 % conversion and a 22 % benzoquinone yield within 3 h at 5 mA cm-2. Density functional theory (DFT) calculations reveal that selective C-O bond cleavage occurs on the heterojunction surface, elucidating the reaction pathway. When applied to alkali-extracted lignin , the system produced valuable aromatic aldehydes, including syringaldehyde (0.82 wt%) and vanillin (2.37 wt%). The generated aromatic products also show potential as renewable fuel-related chemicals and fuel precursors, further highlighting the relevance of this strategy to sustainable energy and biomass valorization. This work demonstrates a sustainable and efficient strategy for lignin valorization in electro-catalytic double-acidic DES media through the development of durable electrocatalysts.
Ammonia, as a zero-carbon fuel, co-firing with coal is an effective technological pathway for reducing CO(2)emissions, but the high NO(X)emission remains a critical issue. Considering the high specific heat capacity and high radiation of CO2, its application in ammonia-coal co-firing may be beneficial to the reduction of NO(X)and can mitigate the greenhouse effect. In this study, the influence of CO2-rich conditions on nitrogen oxidation during ammonia-coal co-firing was investigated by density functional theory (DFT) and the oxidation mechanism of ammonia-nitrogen and coal-nitrogen under CO2-rich conditions is clarified. Results show that the oxidation rate of ammonia-nitrogen is significantly accelerated under the CO2-rich atmosphere, promoting its conversion to NOX, whereas this atmosphere inhibits the conversion of coal-nitrogen to NO(X)at high temperatures (>1600 K). Kinetic analysis further reveals that the promotional effect of CO(2)on ammonia-nitrogen oxidation weakens with the increase in temperature, while its inhibitory effect on the ring-opening of pyridine-N six-membered rings in coal-nitrogen is enhanced after exceeding a certain critical temperature.
This work demonstrates the direct conversion of CO2 to aromatics using a NaFeCo/H-ZSM-5 multifunctional catalyst, highlighting how hydrothermal synthesis conditions of H-ZSM-5 (especially temperature and rotating rate) precisely tune the physicochemical properties of the acidic zeolite and the resulting aromatics synthesis performance. By varying the synthesis parameters, we flexibly control the Al location and the acid sites distribution in H-ZSM-5, which directly govern the aromatics selectivity. Multiple experimental and characterization results clarify that the synergy between Al location and Br & oslash;nsted/Lewis acid sites ratio collectively influence the selectivity of total aromatics, whereas the BTX (benzene, toluene, and xylene) fraction in total aromatics is dominated by the external surface acid sites of H-ZSM-5. Specifically, the increase of hydrothermal temperature optimizes the acid site density of zeolite, therefore boosting the space-time yield (STY) of aromatics and BTX by enhancing the driving force of the tandem process. For the rotating rate factor, a higher rotating rate enriches Al at channel intersections-a configuration that is more conducive to aromatics synthesis-leading to an aromatics selectivity of up to 48.5 %, while the increased external acidity promotes the formation of heavy aromatics. Therefore, optimized STY of BTX (19.5 mmol & sdot;g-1h- 1) is achieved at a moderate rotating rate of 5.6 r/min. This study establishes a clear structure-function relationship between the acidic property of H-ZSM-5 and aromatics synthesis performance, providing a strategic guideline for the rational design of H-ZSM-5 zeolites for CO2 hydrogenation toward value-added aromatics.
