Large-Scale Synthesis of N,S Codoped Carbon-Modified Fe0.975S Composites as a Novel Anode for Lithium/Sodium Ion Batteries with Enhanced Performance.

To overcome obstacles hindering the commercialization of lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs), we introduce a cost-effective single-step sulfurization strategy for synthesizing iron sulfide (Fe0.975S) nanohybrids, augmented by N,S codoped carbon. The resulting N,S codoped carbon-coated Fe0.975S (Fe0.975S@NSC) electrode exhibits exceptional potential as a highly reversible anode material for both LIBs and SIBs. With impressive initial discharge and charge capacities (1658.2 and 1254.9 mAh g-1 for LIBs and 1450.9 and 1077.1 mAh g-1 for SIBs), the electrode maintains substantial capacity retention (900 mA h g-1 after 1000 cycles for LIBs and 492.5 mA h g-1 after 600 cycles for SIBs at 1.0 A g-1). The LiMn2O4//Fe0.975S@NSC and Na3V2(PO4)3//Fe0.975S@NSC full batteries can maintain excellent reversible capacity and robust cycling stability. Ex situ and in situ X-ray diffraction, density functional theory (DFT) calculations, and kinetics analysis confirm the promising energy storage potential of the Fe0.975S@NSC composite.

Carbon Nanotube Support, Carbon Loricae and Oxygen Defect Co-Promoted Superior Activities and Excellent Durability of RuO2 Nanoparticles Towards the pH-Universal H2 Evolution.

This work reports a strategy that integrates the carbon nanotube (CNT) supporting, ultrathin carbon coating and oxygen defect generation to fabricate the RuO2 based catalysts toward the pH-universal hydrogen evolution reaction (HER) with high efficiencies. Specifically, the CNT supported RuO2 nanoparticles with ultrathin carbon loricae and rich oxygen vacancies at the surface (C@OV-RuO2/CNTs-325) have been synthesized. The C@OV-RuO2/CNTs-325 shows superior activities and excellent durability for the HER. It only requires overpotentials of 36.1, 18.0, and 19.3 mV to deliver -10 mA cm-2 in the acidic, neutral, and alkaline media, respectively. Its HER activities are comparable to that of the Pt/C in the acidic media but higher than those of the Pt/C in the neutral and alkaline media. The C@OV-RuO2/CNTs-325 shows excellent HER durability with no activity losses for > 500 h in the acidic, neutral or alkaline media at -250 mA cm-2. The density-functional-theory calculations indicate that the CNT supporting, the carbon coating, and the OVs can modulate the d-band centers of Ru, increasing the HER activities of C@OV-RuO2/CNTs-325, and stabilize the Ru atoms in the catalyst, increasing the durability of the C@OV-RuO2/CNTs-325. More interestingly, the C@OV-RuO2/CNTs-325 shows great potential for practical applications toward overall seawater splitting.

Strong Metal-Support Interaction Modulation between Pt Nanoclusters and Mn3O4 Nanosheets through Oxygen Vacancy Control to Achieve High Activities for Acidic Hydrogen Evolution.

The optimization of metal-support interactions is used to fabricate noble metal-based nanoclusters with high activity for hydrogen evolution reaction (HER) in acid media. Specifically, the oxygen-defective Mn3O4 nanosheets supported Pt nanoclusters of ≈1.71 nm in diameter (Pt/V·-Mn3O4 NSs) are synthesized through the controlled solvothermal reaction. The Pt/V·-Mn3O4 NSs show a superior activity and excellent stability for the HER in the acidic media. They only require an overpotential of 19 mV to drive -10 mA cm-2 and show negligible activity loss at -10 and -250 mA cm-2 for >200 and >60 h, respectively. Their Pt mass activity is 12.4 times higher than that of the Pt/C and even higher than those of many single-atom based Pt catalysts. DFT calculations show that their high HER activity arises mainly from the strong metal-support interaction between Pt and Mn3O4. It can facilitate the charge transfer from Mn3O4 to Pt, optimizing the H adsorption on the catalyst surface and promoting the evolution of H2 through the Volmer-Tafel mechanism. The oxygen vacancies in the V·-Mn3O4 NSs are found to be inconducive to the high activity of the Pt/V·-Mn3O4 NSs, highlighting the great importance to reduce the vacancy levels in V·-Mn3O4 NSs.

Advances in the Removal of Organic Pollutants from Water by Photocatalytic Activation of Persulfate: Photocatalyst Modification Strategy and Reaction Mechanism.

Environmental pollution caused by persistent organic pollutants has imposed big threats to the health of human and ecological systems. The development of efficient methods to effectively degrade and remove these persistent organic pollutants is therefore of paramount importance. Photocatalytic persulfate-based advanced oxidation technologies (PS-AOTs), which depend on the highly reactive SO4 - radicals generated by the activation of PS to degrade persistent organic pollutants, have shown great promise. This work discusses the application and modification strategies of common photocatalysts in photocatalytic PS-AOTs, and compares the degradation performance of different catalysts for pollutants. Furthermore, essential elements impacting photocatalytic PS-AOTs are discussed, including the water matrix, reaction process mechanism, pollutant degradation pathway, singlet oxygen generation, and potential PS hazards. Finally, the existing issues and future challenges of photocatalytic PS-AOTs are summarized and prospected to encourage their practical application. In particular, by providing new insights into the PS-AOTs, this review sheds light on the opportunities and challenges for the development of photocatalysts with advanced features for the PS-AOTs, which will be of great interests to promote better fundamental understanding of the PS-AOTs and their practical applications.

Sb Doping and Amorphization Co-Induced High Capacity and Excellent Durability of Tin Sulfide-Based Anode for K-Ion Batteries.

The carbon nanotubes (CNTs) supported amorphous Sb doped substoichiometric tin dulfide (Sb─SnSx ) with a carbon coating (the C/Sb─SnSx @CNTs-500) is reported to be an efficient anode material for K+ storage. The formation of the C/Sb─SnSx @CNTs-500 is simply achieved through the thermally induced desulfurization of tin sulfide via a controlled annealing of the C/Sb─SnS2 @CNTs at 500 °C. When used for the K+ storage, it can deliver stable reversible capacities of 406.5, 305.7, and 238.4 mAh g-1 at 0.1, 1.0, and 2.0 A g-1 , respectively, and shows no capacity drops when potassiated/depotassiated at 1.0 and 2.0 A g-1 for >3000 and 2400 cycles, respectively. Even at 10, 20, and 30 A g-1 , it can still deliver stable reversible capacities of 138.5, 85.1, and 73.8 mAh g-1 , respectively. The unique structure, which combines the advantageous features of carbon integration/coating, metal doping, and desulfurization-induced amorphous structure, is the main origin of the high performance of the C/Sb─SnSx @CNTs-500. Specifically, the carbon integration/coating can increase the electric conductivity and stability of the C/Sb─SnSx @CNTs-500. The density function theory calculation indicates that the Sb doping and the desulfurization can facilitate the potassiation and increase the electric conductivity of Sb─SnSx . Additionally, the desulfurization can increase the K+ diffusivity in Sb─SnSx .

Sr-Stabilized IrMnO2 Solid Solution Nano-Electrocatalysts with Superior Activity and Excellent Durability for Oxygen Evolution Reaction in Acid Media.

The development of cost-effective catalysts for oxygen evolution reaction (OER) in acidic media is of paramount importance. This work reports that Sr-doped solid solution structural ultrafine IrMnO2 nanoparticles (NPs) (≈1.56 nm) on the carbon nanotubes (Sr-IrMnO2/CNTs) are efficient catalysts for the acidic OER. Even with the Ir use dosage 3.5 times lower than that of the commercial IrO2, the Sr-IrMnO2/CNTs only need an overpotential of 236.0 mV to drive 10.0 mA cm-2 and show outstanding stability for >400.0 h. Its Ir mass activity is 39.6 times higher than that of the IrO2 at 1.53 V. The solid solution and Sr-doping structure of Sr-IrMnO2 are the main origin of the high catalytic activity and excellent stability of the Sr-IrMnO2/CNTs. The density function theory calculations indicate that the solid solution structure can promote strong electronic coupling between Ir and Mn, lowering the energy barrier of the OER rate-determining step. The Sr-doping can enhance the stability of Ir against the chemical corrosion and demetallation. Water electrolyzers and proton exchange membrane water electrolyzers assembled with the Sr-IrMnO2/CNTs show superb performance and excellent durability in the acid media.

Covalently bridged bond assembly of MoS2lamellae onto a graphene sheet: an outstanding electrode for high rate and long-life lithium/sodium-ion batteries.

The practical application of Molybdenum sulphide (MoS2) electrodes has been hindered by its structural instability, and poor electrical conductivity. To enhance the cycle stability and rate performance of MoS2in lithium/sodium-ion batteries (LIBs/SIBs), we synthesized a graphene-supported MoS2composite (MoS2@rGO) with affluent covalent bridged bonds through a facile and scalable hydrothermal and annealing process. The covalent bridged bonds of Mo-S-C, Mo-O-C and C-O-S provide an effective charge transfer path between MoS2and graphene, facilitating fast charge hopping and improving rate performance. As anode materials for LIBs, the MoS2@rGO exhibited exceptional long-term cycle life (906 mAh g-1at 1.0 A g-1after 400 cycles) and outstanding rate capability (1267.7/314.7 mAh g-1at 0.1/6.5 A g-1). Additionally, the MoS2@rGO electrode demonstrated a stable reversible capacity of 521.7 mAh g-1at 1.0 A g-1after 700 cycles and excellent rate capabilities of 665.1 and 326.3 mAh g-1at 0.1 and 10.0 A g-1in SIBs. The edge Mo of MoS2is directly coupled with the oxygen of the functional group on rGO, achieved by adjusting the pH value of the solution to tune the surface charge feature, can effectively enhance the structural stability of electrode even under higher current density.

Shell thickness controlled core-shell Fe3O4@CoO nanocrystals as efficient bifunctional catalysts for the oxygen reduction and evolution reactions.

Core-shell Fe3O4@CoO NCs have been demonstrated to be efficient bifunctional catalysts for the oxygen reduction (ORR) and evolution (OER) reactions. Their activities are strongly shell thickness dependent. Specifically, nanocrystals with ∼2 monolayers of CoO can exhibit a potential difference of 0.794 V at OER and ORR current densities of 10 and -3 mA cm-2, respectively. This value is competitive to those of most active bifunctional catalysts reported. In addition, they are also used as the oxygen cathode for Zn-air batteries and can deliver a peak power density of 109 mW cm-2, much higher than that of the Pt-RuO2/C (88.1 mW cm-2).

Core@shell structured Co-CoO@NC nanoparticles supported on nitrogen doped carbon with high catalytic activity for oxygen reduction reaction.

A composite with a hierarchical structure consisting of nitrogen doped carbon nanosheets with the deposition of nitrogen doped carbon coated Co-CoO nanoparticles (Co-CoO@NC/NC) has been synthesized by a simple procedure involving the drying of the reaction mixture containing Co(NO3)2, glucose, and urea and its subsequent calcination. The drying step is found to be necessary to obtain a sample with small and uniformly sized Co-CoO nanoparticles. The calcination temperature has a great effect on the catalytic activity of the final product. Specifically, the sample prepared at the calcination temperature of 800 °C shows better catalytic activity of the oxygen reduction reaction (ORR). Urea in the reaction mixture is crucial to obtain the sample with the uniformly sized Co-CoO nanoparticles and also plays an important role in improving the catalytic activity of the Co-CoO@NC/NC. Additionally, there exists a strong electronic interaction between the Co-CoO nanoparticles and the NC. Most interestingly, the Co-CoO@NC/NC is highly efficient for the ORR and can deliver an ORR onset potential of 0.961 V vs. RHE and a half-wave potential of 0.868 V vs. RHE. Both the onset and half-wave potentials are higher than those of most catalysts reported previously and even close to those of the commercial Pt/C (the ORR onset and half-wave potential of the Pt/C are 0.962 and 0.861 V vs. RHE, respectively). This, together with its high stability, strongly suggests that the Co-CoO@NC/NC could be used as an efficient catalyst for the ORR.