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  1. Production of clean hydrogen energy from water splitting is vital for the future fuel industry, and nanocomposites have emerged as effective catalysts for the hydrogen evolution reaction (HER). In this study, Ru-CoO@SNG nanocomposites are prepared by controlled pyrolysis where Ru-CoO heterostructured nanoparticles are supported on nitrogen and sulfur codoped graphene oxide nanosheets. With a large surface area, the obtained composites exhibit a remarkable electrocatalytic activity toward HER in 1.0 M KOH with an overpotential of only −90 mV to reach the current density of 10 mA cm−2 , in comparison to −60 mV for commercial Pt/C benchmark, along with high stability. Mechanistically, codoping of sulfur and nitrogen facilitates the dispersion of the nanoparticles, and the formation of Ru-CoO heterostructures increases the active site density, reduces the electron-transfer kinetics and boosts the catalytic performance. Results from this study highlight the unique potential of structural engineering in enhancing the electrocatalytic performance of heterostructured nanocomposites. 
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  2. Low-cost, high-performance oxygen catalysts are critical for electrochemical water splitting and metal-air batteries. Herein, carbon aerogels with skeletons consisting of few-layer graphene are derived pyrolytically from a hydrogel precursor using an array of NaCl crystals as the template, exhibiting a high electrical conductivity (869 S m−1) and an ultralow mass density (11.1 mg cm−3). The deposition of NiFe layered double hydroxide (NiFeLDH) nanocolloids renders the aerogels active towards both the oxygen reduction/evolution reactions (ORR/OER), with the performances highly comparable to those of commercial benchmarks in both alkaline and neutral media. Results from operando Raman spectroscopy measurements and first principles calculations suggest that Fe(OH)3 colloids facilitate the oxidation of Ni2+, which lowers the energy barrier to 0.42 eV for OER, whereas the nitrogen-doped carbon aerogels are responsible for the ORR activity. With the composites used as bifunctional oxygen catalysts for electrochemical water splitting and rechargeable zinc-air batteries, the performances in both alkaline and neutral media are markedly better than those based on the mixture of commercial Pt/C and RuO2. Results from this study highlight the unique advantages of ultrathin graphene aerogels in the development of effective catalysts for electrochemical energy devices. 
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  3. Abstract

    Copper compounds have been extensively investigated for diverse applications. However, studies of cuprous hydroxide (CuOH) have been scarce due to structural metastability. Herein, a facile, wet‐chemistry procedure is reported for the preparation of stable CuOH nanostructures via deliberate functionalization with select organic ligands, such as acetylene and mercapto derivatives. The resulting nanostructures are found to exhibit a nanoribbon morphology consisting of small nanocrystals embedded within a largely amorphous nanosheet‐like scaffold. The acetylene derivatives are found to anchor onto the CuOH forming CuC linkages, whereas CuS interfacial bonds are formed with the mercapto ligands. Effective electronic coupling occurs at the ligand‐core interface in the former, in contrast to mostly non‐conjugated interfacial bonds in the latter, as manifested in spectroscopic measurements and confirmed in theoretical studies based on first principles calculations. Notably, the acetylene‐capped CuOH nanostructures exhibit markedly enhanced photodynamic activity in the inhibition of bacteria growth, as compared to the mercapto‐capped counterparts due to a reduced material bandgap and effective photocatalytic generation of reactive oxygen species. Results from this study demonstrate that deliberate structural engineering with select organic ligands is an effective strategy in the stabilization and functionalization of CuOH nanostructures, a critical first step in exploring their diverse applications.

     
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