Redox Promoted Rapid and Deep Reconstruction of Defect-Rich Nickel Precatalysts for Efficient Water Oxidation.

Understanding the reconstruction mechanism to rationally design cost-effective electrocatalysts for oxygen evolution reaction (OER) is still challenging. Herein, a defect-rich NiMoO4 precatalyst is used to explore its OER activity and reconstruction mechanism. In situ generated oxygen vacancies, distorted lattices, and edge dislocations expedite the deep reconstruction of NiMoO4 to form polycrystalline Ni (oxy)hydroxides for alkaline oxygen evolution. It only needs ≈230 and ≈285 mV to reach 10 and 100 mA cm-2, respectively. The reconstruction boosted by the redox of Ni is confirmed experimentally by sectionalized cyclic voltammetry activations at different specified potential ranges combined with ex situ characterization techniques. Subsequently, the reconstruction route is presented based on the acid-base electronic theory. Accordingly, the dominant contribution of the adsorbate evolution mechanism to reconstruction during oxygen evolution is revealed. This work develops a novel route to synthesize defect-rich materials and provides new tactics to investigate the reconstruction.

Dual Interface Compatibility Enabled via Composite Solid Electrolyte with High Transference Number for Long-Life All-Solid-State Lithium Metal Batteries.

The development of solid-state electrolytes (SSEs) effectively solves the safety problem derived from dendrite growth and volume change of lithium during cycling. In the meantime, the SSEs possess non-flammability compared to conventional organic liquid electrolytes. Replacing liquid electrolytes with SSEs to assemble all-solid-state lithium metal batteries (ASSLMBs) has garnered significant attention as a promising energy storage/conversion technology for the future. Herein, a composite solid electrolyte containing two inorganic components (Li6.25 Al0.25 La3 Zr2 O12 , Al2 O3 ) and an organic polyvinylidene difluoride matrix is designed rationally. X-ray photoelectron spectroscopy and density functional theory calculation results demonstrate the synergistic effect among the components, which results in enhanced ionic conductivity, high lithium-ion transference number, extended electrochemical window, and outstanding dual interface compatibility. As a result, Li||Li symmetric battery maintains a stable cycle for over 2500 h. Moreover, all-solid-state lithium metal battery assembled with LiNi0.6 Co0.2 Mn0.2 O2 cathode delivers a high discharge capacity of 168 mAh g-1 after 360 cycles at 0.1 C at 25 °C, and all-solid-state lithium-sulfur battery also exhibits a high initial discharge capacity of 912 mAh g-1 at 0.1 C. This work demonstrates a long-life flexible composite solid electrolyte with excellent interface compatibility, providing an innovative way for the rational construction of next-generation high-energy-density ASSLMBs.

Symbiotic composite composed of MoS2 and pelagic clay with enhanced disinfection efficiency.

Molybdenum disulfide (MoS2) has attracted increasing attention as a promising photocatalyst. In addition to its application in photocatalytic hydrogen production and pollutant degradation, MoS2 is also used in water disinfection. However, its poor disinfection performance limits its practical utility. Herein, we prepared a symbiotic composite composed of MoS2 and pelagic clay (MoS2/PC) as a photocatalyst for water disinfection. The composite achieved a high disinfection rate of 99.95% to Escherichia coli (E. coli) under visible light illumination, which is significantly higher than that of bulk MoS2 (61.87%). Characterization shows that abundant hydroxyl groups in illite/montmorillonite (I/M) formed during hydrothermal synthesis of MoS2, which contributed to the enhanced disinfection activity. Those hydroxyl groups can attract photogenerated holes through electrostatic attraction, and facilitate the separation of photogenerated charge carriers, thereby enhancing the disinfection activity. Moreover, the good hydrophilicity of pelagic clay improves the dispersity of MoS2 in water, which is beneficial for its utility in aqueous solutions. In addition, the symbiotic structure restricts the growth and aggregation of MoS2 nanosheets and shortens the diffusion distance of charge carriers to the material surface, further reducing the recombination of electrons and holes. This study provides a way to improve the disinfection activity of MoS2 and also sheds light on high value-added utilization of pelagic clay.

Electrochemical Fixation of Nitrogen by Promoting N2 Adsorption and N-N Triple Bond Cleavage on the CoS2/MoS2 Nanocomposite.

An electrochemical N2 reduction reaction (NRR), as an environmentally benign method to produce NH3, is a suitable alternative to substitute the energy-intensive Haber-Bosch technology. Unfortunately, to date, it is obstructed by the lack of efficient electrocatalysts. Here, a CoS2/MoS2 nanocomposite with CoS2 nanoparticles decorated on MoS2 nanosheets is fabricated and adapted as a catalyst for the NRR. As unveiled by experimental and theoretical results, the strong interaction between CoS2 and MoS2 modulates interfacial charge distribution with electrons transferring from CoS2 to MoS2. Consequently, a local electrophilic region is formed near the CoS2 side, which enables effective N2 absorption. On the other hand, the nucleophilic area formed near the MoS2 side is in favor of breaking stable N≡N, the potential-determining step (*N2 → *N2H) which brings about a much decreased energy barrier than that on pure MoS2. As a result, this catalyst exhibits an excellent NRR performance, NH3 yield and Faradaic efficiency of 54.7 µg·h-1·mg-1 and 20.8%, respectively, far better than most MoS2-based catalysts.