Pulsed electro-catalysis enables effective conversion of low-concentration nitrate to ammonia over Cu2O@Pd tandem catalyst.

Electro-catalytic conversion of nitrate (NO3-) to ammonia (NH3) via the Nitrate Reduction to Ammonia (NORA) process represents a promising strategy for both ammonia synthesis and environmental remediation. Despite its potential, the efficiency of low-concentration NORA is often hindered by mass transfer limitations, competing byproducts (N2 and NO2-), and side reactions such as hydrogen evolution. This study introduces a novel pulsed electro-synthesis technique that alternates the potential to periodically accumulate and transform NO2- intermediates near a Cu2O@Pd electrode, enhancing the NORA process. Compared with that under potentiostatic conditions, the Cu2O@Pd electrodes exhibited a higher NORA activity under the optimized pulsed condition, where a NH3-N Faradaic efficiency (FE) of 81.2%, a yield rate of 1.08 mg h-1 cm-2 and a selectivity efficiency (SE) of 81.5%, were achieved. In-situ characterization revealed an enhancement mechanism characterized by optimized adsorption of the key *NO intermediate, followed by the hydrogenation path "*N → *NH → *NH2→ *NH3". Further investigations indicated the electro-catalytic synergies between Pd sites and Cu species, where the Pd atoms were the reaction sites for the H adsorption while the Cu species were responsible for the NO3- activation. This research offers a novel insight into a method of enhancing low-concentration NORA.

Engineering Morphology and Electron Redistribution of a Ni/WO3 Mott-Schottky Bifunctional Electrocatalyst for Efficient Alkaline Urea Splitting.

Construction of the desired morphology and nanointerface to expose the active sites and modulate the electronic structure offers an effective approach to boosting urea splitting for energy-saving hydrogen generation. Herein, we fabricate a Ni/WO3 Mott-Schottky heterojunction electrocatalyst with a hedgehog-like structure supported on Ni foam toward alkaline urea splitting. Different Ni/WO3 morphologies, such as microspheres, hedgehog-like structures, octahedrons, and cubes, were obtained when various ratios of Ni/W feeds were used. The Mott-Schottky nanointerfaces between Ni and WO3 domains are visually confirmed by high-resolution transmission electron microscopy images, which also accelerated the charge transfer rate. Benefiting from the high electrochemically active surface area and enhanced charge transferability, the optimal Ni/WO3 electrode exhibits outstanding catalytic activity toward hydrogen generation with a low overpotential of 163 mV at 100 mA cm-2 in alkaline solution and reduced cell voltage of 1.67 V when coupled with urea oxidation reaction. Theoretical calculations reveal that the Ni sites in Ni/WO3 optimize the H adsorption energy (ΔGH*) with the |ΔGH*| value of 0.097 eV, much lower than that of Ni (0.35 eV) and WO3 (0.235 eV). This work demonstrates important guidance in designing an efficient electrocatalyst for urea splitting.

Engineering of 3D graphene hydrogel-supported MnO2-FeOOH nanoparticles with synergistic effect of oxidation and adsorption toward highly efficient removal of arsenic.

Iron-manganese-based adsorbent has been regarded as a promising candidate for arsenic purification from water, especially the inorganic As(III), due to its inherent advantage of low cost and large-scale producibility. However, the nanoparticle aggregation, metal leaching and insufficient removal efficiency remain the main challenges in the practical applications of the granular adsorbents. In this work, we develop a universal strategy for the fabrication of an active Fe(III) oxyhydroxide-Mn(IV) oxide/3D graphene oxide (GO) gel composite via a simple hydrothermal reaction. The successful immobilization of Fe-Mn oxyhydroxide/oxides on the interconnected GO gels was intuitively confirmed by the transmission electron microscopy and atomic force microscopy. The combinative characterizations of the X-ray absorption near edge structure and X-ray photoelectron spectroscopy clearly reveal the electron transfer from Fe atoms to Mn atoms. The optimized Fe-Mn/GO composites possess the superior performance with the removal efficiency of over 90% for As(III) at pH 7.0 and ∼97% for As(V) at pH 5.0 and the As(III, V) levels (100 µg l-1) are reduced to below the WHO guideline of 10 µg l-1. The sorption isotherm and kinetic experiments on the As removal were also carried out. The post characterizations are employed to better unveil the oxidation-adsorption mechanism. Notably, the application of Fe-Mn/GO composites in the treatment of As-simulated natural water demonstrated a stable and continuous operation for over 20 days and an effluent concentration of arsenic as low as the 10 µg l-1 in a specially designed flow reactor.