Sulfur hexafluoride (SF6), the strongest greenhouse gas, has great challenges in degradation because of its stable structure, posing significant environmental concerns. Photocatalysis offers an environmentally friendly, low-energy solution, but the fluoride deposition on catalysts reduces their activity, thus limiting their large-scale application. To prevent catalyst fluoride poisoning, we report a thin-layer graphitic carbon nitride (CN) material loaded with MoOx (CNM) that resists fluoride deposition for long-term SF6 degradation. By combining molecular structure design and nanostructure regulation, we construct a photocatalyst with enhanced charge carrier mobility and reduced transport distances. We find that the CNM exhibits a high specific surface area, increased contact between reactants and active sites, and efficient electron–hole separation due to the Mo-N bonds, achieving an SF6 degradation efficiency of 1.73 mmol/g after one day due to the prolonged catalytic durability of the catalyst, which is eight times higher than pristine g-C3N4 (0.21 mmol/g). We demonstrate the potential of CNMs for low-energy, high-efficiency SF6 degradation, offering a new approach to mitigate the environmental impact of this potent greenhouse gas. We envision that this study will inspire further research into advanced photocatalytic materials for environmental remediation, contributing to global efforts in combating climate change.
Halogen‐mediated electrosynthesis is a sustainable strategy for organic synthesis under mild conditions. Yet achieving selective iodoform synthesis at high current remains difficult because of the strong competition between iodide oxidation reaction (IOR) and oxygen evolution reaction (OER). Here, we develop a quinary sulfide catalyst, AgCuCoGeS 4 (ACCGS), synthesized via a thermal injection method, which achieves exceptional IOR selectivity in a flow electrochemical system. Density functional theory (DFT) calculations reveal that the Ag‐Cu synergistic effects in ACCGS widen the adsorption energy gap between I − and *OH intermediates, thereby effectively suppressing the competing OER by weakening *OH binding while strengthening I − chemisorption. Experimentally, ACCGS/GF demonstrates an iodoform yield of 80.3% at 200 mA, marking a substantial enhancement over the 45.0% yield of CoS/GF. It also demonstrates stable operation for 12 h, confirming its excellent long‐term stability. Notably, it sustains a remarkable Faradaic efficiency of 64.1% for IOR at an ampere‐level current of 1000 mA, which highlights its breakthrough in high‐current tolerance. Therefore, this work demonstrates an effective strategy for ampere‐level electrosynthesis by combining multimetallic catalysis with a flow system for halogenated chemical production.
Aqueous polysulfide/ferricyanide redox flow batteries (S/Fe RFBs) are attractive for large-scale energy storage because of their resource abundance and favorable safety, but sluggish polysulfide redox kinetics cause substantial polarization and limit energy efficiency and power density. Here, an industrial cobalt-containing residue from zinc hydrometallurgy is used as a self-sulfidizing precursor for a one step thermal conversion under N2. Its endogenous Co, Zn, and S components form Co1-xS/ZnS multiphase sulfides, whose phase and surface Co valence state are regulated by treatment temperature. X-ray diffraction shows Co1-xS rich products at 500-600 °C, whereas ZnS becomes increasingly dominant at ≥700 °C. X-ray photoelectron spectroscopy further identifies the highest relative surface Co3+ content in the 600 °C sample, coinciding with the strongest polysulfide redox response and the lowest combined interfacial resistance among the investigated electrodes. When slurry coated onto graphite felt, the 600 °C catalyst enables an S/Fe RFB energy efficiency of 89.5% at 20 mA cm-2 and a peak power density of 109.1 mW cm-2 The cell retains approximately 91% of its initial energy retention after 150 cycles over 630 h, corresponding to an average energy decay of 0.06% per cycle. This work demonstrates a simple waste to electrocatalyst strategy based on endogenous sulfur utilization and temperature controlled phase regulation, offering a route for valorizing cobalt-containing metallurgical residues in aqueous flow-battery electrodes.
The selective reduction of nitro group in reactive substituents of Nitrobenzene is a substantial challenge for industrial applications and academia. Inspired by unique Lewis acid character and the malleable oxidation state of Iron element. Fe doped MoS2 exhibits excellent catalytic reduction activity and selectivity towards nitrobenzene. DFT calculations have shown that charge transfer between Fe and Mo atoms is crucial for promoting S2- adsorption and rapid conversion of nitrobenzene. The kinetic study revealed that the reaction is first order with respect to Nitrobenzene and second order with respect to sulphide ion. The turn over number (TON), turn over frequency (TOF) for Fe reaction center and activation energy of the reaction were calculated as 1,291,800 molAn/molFe, 86,120 hr-1 and 22.091 kJ.mol-1 respectively. 5 % Fe-MoS2 showed high stability in N2 flow and retained 100 % selectivity and 80 % of activity for 5 cycles.