Non-metal ammonium-ion aqueous supercapacitors are raising notable attention owing to their cost, safety, and environmental advantages, but the development of optimized electrode materials for ammonium ion storage still lacks behind expectations. To overcome current challenges, here, w e propose a sulfide-based composite electrode based on MoS2 and polyaniline (MoS2 @PANI) as an ammonium ion host. The optimized composite possesses specific capacitances above 450 F·g-1 at a current density of 1 A·g-1 , and 86.3% capacitance retention after 5000 cycles in a three-electrode configuration. PANI not only contributes to the electrochemical performance but also plays a key role in defining the final MoS2 architecture. Symmetric supercapacitors assembled with such electrode display energy densities above 60 Wh·kg-1 at a power density of 725 W·kg-1 . Compared with Li+ and K+ ions, the surface capacitive contribution in NH4 + -based devices is lower at every scan rate, which points to an effective generation/breaking of H-bonds as the mechanism controlling the rate of NH4 + insertion/de-insertion. This result is supported by density functional theory (DFT) calculations, which also show that sulfur vacancies effectively enhance the NH4 + adsorption energy and improve the electrical conductivity of the whole composite. Overall, this work demonstrates the great potential of composite engineering in optimizing the performance of ammonium-ion insertion electrodes. This article is protected by copyright. All rights reserved.

MoS2 @Polyaniline for Aqueous Ammonium-Ion Supercapacitors.

Low electrical conductivity and poor accessibility of MoS2 reaction sites raise great challenges in maximizing the triple-phase-boundary (TPB) sites of MoS2-based electrodes and minimizing ohmic losses for efficient hydrogen evolution reaction (HER) in practical proton exchange membrane (PEM) water electrolysis. Herein, we report a scalable hydrothermal approach to fabricate ionomer-free integrated electrodes with engineered 1 T-2 H heterophase and defect-rich MoS2 nanosheets (MoS2NSs) in-situ grown onto the carbon fiber paper (CFP). With an ultralow loading of 0.14 mg/cm2, a small voltage of 2.25 V was obtained at 2000 mA/cm2 in a practical cell with Nafion115 membrane, which outperforms all previously reported high-loading non-precious catalyst-based electrodes. Impressively, it shows 44 times higher mass activity than a high-loading and ionomer-mixed MoS2 assemblies electrode. This work builds a bridge from catalyst optimization to electrode fabrication and provides a promising direction for improving intrinsic catalytic activity, electrode conductivity and stability for practical PEM water electrolysis. 

http://manuscript.elsevier.com/S092633732200399X/pdf/S092633732200399X.pdf

MoS2 nanosheet integrated electrodes with engineered 1T-2H phases and defects for efficient hydrogen production in practical PEM electrolysis

Currently, inner-generate hydrogen peroxide to enhance the degradation of pollutants is an outstanding way. However, few studies have been done on MoS2 photocatalysts with sulfur vacancies at the phase-junction to produce innergenerate-H2O2 to promote contaminants degradation. Herein, we prepared Mo1−xS2−y photocatalysts with sulfur vacancies at the phase-junction by a simple method (temperature-programmed reduction in hydrogen atmosphere) to achieve high innergenerate-H2O2 and high degradation efficiency. Specifically, Mo1−xS2−y exhibited a high yield of innergenerate-H2O2 (35 μmol L−1 h−1, 1.5 times as high as bulk MoS2) under simulated solar irradiation, because the promoted electron transfer can increase superoxide radical to generate innergenerate-H2O2. Hydroxyl radicals generated by decomposition of innergenerate-H2O2 through the transformation of variable metal molybdenum atom (Mo(Ⅳ)/Mo(Ⅵ)) can effectively improve the degradation efficiency of tetracycline and diclofenac sodium (twice as high as bulk MoS2). The novel and concise way was paved to synthesize photocatalysts for high-efficiency photocatalytic degradation by innergenerate-H2O2. 

Efficient degradation of PPCPs by Mo1-xS2-y with S vacancy at phase-junction: promoted by innergenerate-H2O2

Superior Fenton-like and photo-Fenton-like activity of MoS2@TiO2/N-doped carbon nanofibers with phase-regulated and vertically grown MoS2 nanosheets

To improve the production rate of MoS2 nanosheets as an excellent supercapacitor (SC) material and enhance the performance of the MoS2-based solid-state SC, a liquid phase exfoliation method is used to prepare MoS2 nanosheets on a large scale. Then, the MnO2 nanowire sample is synthesized by a one-step hydrothermal method to make a composite with the as-synthesized MoS2 nanosheets to achieve a better performance of the solid-state SC. The interaction between the MoS2 nanosheets and MnO2 nanowires produces a synergistic effect, resulting in a decent energy storage performance. For practical applications, all-solid-state SC devices are fabricated with different molar ratios of MoS2 nanosheets and MnO2 nanowires. From the experimental results, it can be seen that the synthesized nanocomposite with a 1:4 M ratio of MoS2 nanosheets and MnO2 nanowires exhibits a high Brunauer–Emmett–Teller surface area (∼118 m2/g), optimum pore size distribution, a specific capacitance value of 212 F/g at 0.8 A/g, an energy density of 29.5 W h/kg, and a power density of 1316 W/kg. Besides, cyclic charging–discharging and retention tests manifest significant cycling stability with 84.1% capacitive retention after completing 5000 rapid charge–discharge cycles. It is believed that this unique, symmetric, lightweight, solid-state SC device may help accomplish a scalable approach toward powering forthcoming portable energy storage applications.

High-Performance MnO2 Nanowire/MoS2 Nanosheet Composite for a Symmetrical Solid-State Supercapacitor

Molybdenum disulfide (MoS2) is a promising candidate for use as a supercapacitor electrode material and non-noble-metal electrocatalyst owing to its relatively high theoretical specific capacitance, Pt-like electronic feature, and graphene-like structure. However, insufficient electrochemically active sites along with poor conductivity significantly hinder its practical application. Heteroatom doping and phase engineering have been regarded as effective ways to overcome the inherent limitations of MoS2 and enhance its ion storage and electrocatalytic performance. In this study, a plasma-assisted nitrogen-doped 1T/2H MoS2 heterostructure has been proposed for the first time, resulting in excellent supercapacitor performance and hydrogen evolution reaction activity. XPS, Raman, and TEM analysis results indicate that N atoms have been successfully doped into MoS2 nanosheets via room-temperature low-power N2 plasma, and the 1T/2H hybrid phase is maintained. As expected, the 1T/2H MoS2 heterostructure after a 10 min plasma treatment displayed a much boosted supercapacitive performance with a high specific capacitance of 410 F g-1 at 1 A g-1 and an excellent hydrogen evolution property with a low overpotential of 131 mV vs RHE at 10 mA cm-2 for hydrogen evolution reaction. The excellent performance is superior to most of the recently reported outstanding MoS2-based electrode and electrocatalytic materials. Moreover, the as-assembled flexible symmetric supercapacitor shows a high specific capacitance of 84.8 F g-1 and superior mechanical robustness with 84.5% capacity retention after 2000 bending cycles.

Controllably Doping Nitrogen into 1T/2H MoS2 Heterostructure Nanosheets for Enhanced Supercapacitive and Electrocatalytic Performance by Low-Power N2 Plasma.

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Controllably Doping Nitrogen into 1T/2H MoS2 Heterostructure Nanosheets for Enhanced Supercapacitive and Electrocatalytic Performance by Low-Power N2 Plasma.