A triple-synergistic small-molecule sulfur cathode promises energetic Cu-S electrochemistry.

Metal-sulfur batteries have received great attention for electrochemical energy storage due to high theoretical capacity and low cost, but their further development is impeded by low sulfur utilization, poor electrochemical kinetics, and serious shuttle effect of the sulfur cathode. To avoid these problems, herein, a triple-synergistic small-molecule sulfur cathode is designed by employing N, S co-doped hierarchical porous bamboo charcoal as a sulfur host in an aqueous Cu-S battery. Expect the enhanced conductivity and chemisorption induced by N, S synergistic co-doping, the intrinsic synergy of macro-/meso-/microporous triple structure also ensures space-confined small-molecule sulfur as high utilization reactant and effectively alleviates the volume expansion during conversion reaction. Under a further joint synergy between hierarchical structure and heteroatom doping, the resulting sulfur cathode endows the Cu-S battery with outstanding electrochemical performance. Cycled at 5 A g-1, it can deliver a high reversible capacity of 2,509.8 mAh g-1 with a good capacity retention of 97.9% after 800 cycles. In addition, a flexible hybrid pouch cell built by a small-molecule sulfur cathode, Zn anode, and gel electrolytes can firmly deliver high average operating voltage of about 1.3 V with a reversible capacity of over 2,500 mAh g-1 under various destructive conditions, suggesting that the triple-synergistic small-molecule sulfur cathode promises energetic metal-sulfur batteries.

Ferrous disulfide and iron nitride sites on hydrochar to enhance synergistic adsorption and reduction of hexavalent chromium.

In this study, a novel hydrochar containing ferrous disulfide (FeS2) and iron nitride (FeN) was prepared via a one-pot hydrothermal method to enhance the synergistic adsorption and reduction of hexavalent chromium (Cr(VI)). This material (Fe3-SNHC) exhibited a Cr(VI) removal capacity of 431.3 mg·g-1 and high tolerance to coexisting anions at pH 2. Adsorption occurred via monolayer chemisorption. Variation in material structure and density functional theory calculations proved that multiple active sites formed by interactions between heteroatoms improved the chemical inertness of hydrochar. FeN and FeS2 with two electron-donating groups had strong reducing ability to facilitate the conversion of Cr(VI) to trivalent chromium. It was concluded that next to electrostatic adsorption and complexation, synergistic reduction among multiple active sites were the dominant mechanisms involved in the removal Cr(VI). This study shows that Fe3-SNHC is a promising and environment-friendly material for Cr(VI) to remove it from wastewater.

MOF-Derived Co Nanoparticles Catalyst Assisted by F- and N-Doped Carbon Quantum Dots for Oxygen Reduction.

The oxygen reduction reaction is crucial in the cathode of fuel cells and metal-air batteries. Consequently, designing robust and durable ORR catalysts is vital to developing metal-air batteries and fuel cells. Metal-organic frameworks feature an adjustable structure, a periodic porosity, and a large specific surface area, endowing their derivative materials with a unique structure. In this study, F and N co-doped on the carbon support surface (Co/FN-C) via the pyrolysis of ZIF-67 as a sacrificial template while using Co/FN-C as the non-noble metal catalysts. The Co/FN-C displays excellent long-term durability and electrochemical catalytic performance in acidic solutions. These performance improvements are achieved because the CQDs alleviate the structural collapse during the pyrolysis of ZIF-67, which increases the active sites in the Co nanoparticles. Moreover, F- and N-doping improves the catalytic activity of the carbon support by providing additional electrons and active sites. Furthermore, F anions are redox-stable ligands that exhibit long-term operational stability. Therefore, the well-dispersed Co NPs on the surface of the Co/FN-C are promising as the non-noble metal catalysts for ORR.

Toward Highly Selective Electrochemical CO2 Reduction using Metal-Free Heteroatom-Doped Carbon.

There are growing interests in metal-free heteroatom-doped carbons for electrochemical CO2 reduction. Previous studies extensively focus on the effect of N-doping, and their products severely suffer from low current density (mostly <2 mA cm-2) and limited selectivity (<90%). Here, it is reported that heteroatom codoping offers a promising solution to the above challenge. As a proof of concept, N,P-codoped mesoporous carbon is prepared by annealing phytic-acid-functionalized ZIF-8 in NH3. In CO2-saturated 0.5 m NaHCO3, the catalyst enables CO2 reduction to CO with great selectivity close to 100% and large CO partial current density (≈8 mA cm-2), which are, to the best of knowledge, superior to all other relevant competitors. Theoretical simulations show that the improved activity and selectivity are stemmed from the enhanced surface adsorption of *COOH and *CO intermediates as a result of the synergy of N and P codoping.

Nitrogen and Sulfur Co-Doped Graphene Nanosheets to Improve Anode Materials for Sodium-Ion Batteries.

Sodium-ion batteries (SIBs) attract more attention because of sodium's abundant availability, affordable price, and potential to be an effective anode material. Meanwhile, carbon-based materials provide the most promising anode materials. Because of the large radius of sodium ions, SIBs do not exhibit favorable electrochemical performance. Introducing heteroatoms into the carbon-lattice is an effective strategy to enlarge the interlayer space of carbon-based materials which can improve carbon's electrochemical performance. In addition, anode materials with a surface-induced capacitive process can enhance the SIB's electrochemical performance because its capacitive process increases the kinetics of ion diffusion. Here, we describe an SIB's anode material containing nitrogen and sulfur co-doped graphene sheets [denoted as poly(2,5-dimercapto-1,3,4-thiadiazole) (PDMcT)/reduced graphene oxide (RGO)] which are synthesized via carbonization of PDMcT polymerized on the surface of GO. PDMcT/RGO exhibited high capacities (240 mA h g-1 at 500 mA g-1), improved rate performance (144 mA h g-1 at 10 A g-1), and good cycling stability (153 mA h g-1 after 5000 cycles at 5000 mA g-1). These unique results are attributed to the enlarged interlayer spacing and electronic conductivity from the heteroatoms which facilitate the sodium ion's insertion and electron transport. These results represent that PDMcT/RGO is a great potential anode material for SIBs.