Transition metal sulfides have demonstrated excellent heavy metal detoxification in previous studies. However, the activity of their S-functional sites is usually not maximized because they are not precisely regulated. Herein, we report a new short-term cathodic tuned CuS crystals (C-tuned CuS) distortion strategy, ultrafast detoxicating over 95% Cr(VI) in 1 min，its detoxification rate was elevated by five orders of magnitude times compared to the untuned one. The high Cr(VI) detoxification performance is mainly attributed to the layered sulfur atoms tuning within series of cathodic potential shown by In-situ Raman. Besides, the four-tuning stages of C-tuned CuS lattice distortion based on the variation of Raman peak height and redshift changes was investigated by density functional theory (DFT) calculations, showing that the S-S bonds was stretched under cathodic tuning, extending from 2.106 to 2.345 Å. The stretched S-S bonds with enhanced polarity and electron activity prevailed the formation of transient Cr-S bonds with Cr(VI), favoring the direct electron transfer without O mediation, thus reducing the Cr(VI) reduction energy barrier. Cathodic tuning CuS crystal distortion, a “Plug and Play” strategy, show a new electron-level microscopic insights into wastewater reduction techniques development.
Multivalent cation batteries are attracting increasing attention in energy-storage applications, but reversible storage of highly polarizing multivalent cations is a major difficulty for the electrode materials. In the present study, charge-delocalizing Mo3S13 cluster-based materials (crystalline (NH4)2Mo3S13 and amorphous MoSx) are designed and investigated as cathodes for rechargeable magnesium batteries. Both of the cathodes show high magnesium storage capacities (296 and 302 mAh g–1 at 100 mA g–1) and superior rate performances (76 and 80 mAh g–1 at 15 A g–1). A high area loading of 3.0 mg cm–2 could be achieved. These performances are of the highest level compared with those of reported magnesium storage materials. Further mechanism study and theoretical computation demonstrate the magnesium storage active sites are the bridging disulfur groups of the Mo3S13 cluster. The valence state of bridging disulfur decreases/increases largely during magnesiation/demagnesiation along with breaking/formation of the sulfur–sulfur bond, which makes the Mg-association/dissociation highly reversible. The sulfur–sulfur bond breaking and formation provides high reversible capacities. Prominently, the valence state increase and sulfur–sulfur bond formation of the bridging disulfur during charge weakens the bonding with Mg2+, significantly assisting the magnesium dissociation. The present study not only develops high-performance magnesium storage cathode materials but also demonstrates the importance of constructing favorable magnesium storage active sites in the high-performance cathode materials design. The findings presented herein are of great significance for the development of electrode materials for the storage of multivalent cations.
Gan Cheng,Yujie Peng,Peigao Duan,Enze Li,Chao Lv,Xin Wang,Fangqin Cheng
Coal remains a primary global energy source, however, the continued exploitation has positioned high-sulfur coal as a critical concern, with its desulfurization remaining a significant technical challenge worldwide. In this study, fine high-sulfur samples were selected for investigation, and a series of flotation and electrochemical methods were employed for desulfurization. The results indicate that both sulfur and ash contents of high-sulfur coal decrease with decreasing particle size. The desulfurization efficiencies for different methods are as follows: 31.04% for flotation, 32.15% for grinding-flotation, 41.08% for electrochemistry, 42.04% for ultrasonic-electrochemistry, 49.51% for electrochemical-flotation, and 51.23% for ultrasonic-electrochemistry-grinding-flotation. Flotation effectively removes most of the inorganic sulfur content, while electrolysis can remove both inorganic sulfur and a portion of organic sulfur content. Grinding facilitates the liberation of sulfur inclusions in coal, while ultrasonic treatment aids in detaching gangue minerals from the coal surface, thereby accelerating the electrochemical reactions. Simulation results show that the C-S bond in coal is more resistant to dissociation than the S-S bond. The oxidation efficacy varies across different crystal planes, with the {111} plane exhibiting the most optimal electrochemical oxidation performance. Furthermore, molecular dynamics simulations indicate that both the collector and electrolytic oxidation affect sulfur migration within the coal matrix.
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