Developing low-cost and efficient electrocatalysts to accelerate oxygen evolution reaction (OER) kinetics is vital for water and carbon-dioxide electrolyzers. The fastest-known water oxidation catalyst, Ni(Fe)O x H y , usually produced through an electrochemical reconstruction of precatalysts under alkaline condition, has received substantial attention. However, the reconstruction in the reported catalysts usually leads to a limited active layer and poorly controlled Feactivated sites. Here, we demonstrate a new electrochemistry-driven Fenabled surface-reconstruction strategy for converting the ultrathin NiFeO x F y nanosheets into an Fe-enriched Ni(Fe)O x H y phase. The activated electrocatalyst shows a low OER overpotential of 218 ± 5 mV at 10 mA cm −2 and a low Tafel slope of 31 ± 4 mV dec −1 , which is among the best for NiFe-based OER electrocatalysts. Such superior performance is caused by the effective formation of the Fe-enriched Ni(Fe)O x H y active-phase that is identified by operando Raman spectroscopy and the substantially improved surface wettability and gas-bubble-releasing behavior.

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Atomic regulation of metal catalysts has emerged as an intriguing yet challenging strategy to boost product selectivity. Here, we report a density functional theory‐guided atomic design strategy for the fabrication of a NiGa intermetallic catalyst with completely isolated Ni sites to optimize acetylene semi‐hydrogenation processes. Such Ni sites show not only preferential acetylene π‐adsorption, but also enhanced ethylene desorption. The characteristics of the Ni sites are confirmed by multiple characterization techniques, including aberration‐corrected high‐resolution scanning transmission electron microscopy and X‐ray absorption spectrometry measurements. The superior performance is also confirmed experimentally against a Ni5Ga3 intermetallic catalyst with partially isolated Ni sites and against a Ni catalyst with multi‐atomic ensemble Ni sites. Accordingly, the NiGa intermetallic catalyst with the completely isolated Ni sites shows significantly enhanced selectivity to ethylene and suppressed coke formation.

We report that a new 2D 3d-4f phosphonate [Co(III)La(III)(notpH)(H2O)6]ClO4·5H2O (CoLa-II) can undergo a phase transition above 45 °C and 93% relative humidity, resulting in [H3O][CoLa(notp)(H2O)4]ClO4·3H2O (CoLa-III). The transition is accompanied by the release of the proton from intralayer to interlayer, and thus the proton conductivity of the material is increased by 1 order of magnitude.

The electrochemical mechanism of the cathode material Li2FeSiO4 with reversible extraction/insertion of more than one Li+ from/into the structure has been studied by techniques of in situ synchrotron X-ray absorption near edge structure (XANES) and X-ray diffraction (XRD). These advanced techniques provide effective solutions to address the limitations of characterization by traditional ex situ methods. The study of in situ Fe K-edge XANES indicates that the Fe ion in the Li2FeSiO4 is oxidized continuously to high valence during the charging process from open circuit potential to 4.8 V, which contributes to the high reversible capacities of the materials. In situ XRD and theoretical study from first-principles calculations have been employed to reveal the structural evolution of the Li2FeSiO4 underlying the high capacity during the charge/discharge process. The results of both experimental and theoretical studies are consistent and indicate that Li2FeSiO4 undergoes two two-phase reactions when the electrode is charged to a high voltage of 4.8 V.

Electrochemical synthesis based on electrons as reagents provides a broad prospect for commodity chemical manufacturing. A direct one‐step route for the electrooxidation of amino C−N bonds to nitrile C≡N bonds offers an alternative pathway for nitrile production. However, this route has not been fully explored with respect to either the chemical bond reforming process or the performance optimization. Proposed here is a model of vacancy‐rich Ni(OH)2 atomic layers for studying the performance relationship with respect to structure. Theoretical calculations show the vacancy‐induced local electropositive sites chemisorb the N atom with a lone pair of electrons and then attack the corresponding N(sp3)−H, thus accelerating amino C−N bond activation for dehydrogenation directly into the C≡N bond. Vacancy‐rich nanosheets exhibit up to 96.5 % propionitrile selectivity at a moderate potential of 1.38 V. These findings can lead to a new pathway for facilitating catalytic reactions in the chemicals industry.

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Rechargeable aqueous zinc ion batteries (AZIBs) are attracting extensive attention owing to environmental friendliness and high safety. However, its practical applications are limited to the poor Coulombic efficiency and stability of a Zn anode. Herein, we demonstrate a periodically stacked CuS-CTAB superlattice, as a competitive conversion-type anode for AZIBs with greatly improved specific capacity, rate performance, and stability. The CuS layers react with Zn2+ to endow high capacity, while CTAB layers serve to stabilize the structure and facilitate Zn2+ diffusion kinetics. Accordingly, CuS-CTAB shows superior rate performance (225.3 mA h g–1 at 0.1 A g–1 with 144.4 mA h g–1 at 10 A g–1) and a respectable cyclability of 87.6% capacity retention over 3400 cycles at 10 A g–1. In view of the outstanding electrochemical properties, full batteries constructed with a CuS-CTAB anode and cathode (Zn x FeCo­(CN)6 and Zn x MnO2) are evaluated in coin cells, which demonstrate impressive full-battery performance.