Production of ammonia is currently realized by the Haber–Bosch process, while electrochemical N₂ fixation under ambient conditions is recognized as a promising green substitution in the near future. A lack of efficient electrocatalysts remains the primary hurdle for the initiation of potential electrocatalytic synthesis of ammonia. For cheaper metals, such as copper, limited progress has been made to date. In this work, we boost the N₂ reduction reaction catalytic activity of Cu nanoparticles, which originally exhibited negligible N₂ reduction reaction activity, via a local electron depletion effect. The electron-deficient Cu nanoparticles are brought in a Schottky rectifying contact with a polyimide support which retards the hydrogen evolution reaction process in basic electrolytes and facilitates the electrochemical N₂ reduction reaction process under ambient aqueous conditions. This strategy of inducing electron deficiency provides new insight into the rational design of inexpensive N₂ reduction reaction catalysts with high selectivity and activity.

The developed UOR electrocatalyst as the anode can provide a current density of 200 mA cm⁻² at 1.427 V vs. RHE, as well as remarkable operational stability.

The advancement of economically efficient electrocatalysts for alkaline water oxidation based on transition metals is essential for hydrogen production through water electrolysis. In this investigation, a straightforward one-step solvent method was utilized to spontaneously cultivate bimetallic sulfide S-FeCo_1 : 1/NIF on the surface of a nickel–iron foam (NIF). Capitalizing on the synergistic impact between the bimetallic constituents and the highly active species formed through electrochemical restructuring, S-FeCo_1 : 1/NIF exhibited remarkable oxygen evolution reaction (OER) performance, requiring only a 310 mV overpotential based on 500 mA cm⁻² current density. Furthermore, it exhibited stable operation at 200 mA cm⁻² for 275 h. Simultaneously, the catalyst demonstrated excellent hydrogen evolution reaction (HER) and overall water-splitting capabilities. It only requires an overpotential of 191 mV and a potential of 1.81 V to drive current densities of 100 and 50 mA cm⁻². Density functional theory (DFT) calculations were also employed to validate the impact of the bimetallic synergistic effect on the catalytic activity of sulfides. The results indicate that the coupling between bimetallic components effectively reduces the energy barrier required for the rate-determining step in water oxidation, enhancing the stability and activity of bimetallic sulfides. The exploration of bimetallic coupling to improve the OER performance holds theoretical significance in the rational design of advanced electrocatalysts.

The activation of C–H bonds is a central challenge in organic chemistry and usually a key step for the retro-synthesis of functional natural products due to the high chemical stability of C–H bonds. Electrochemical methods are a powerful alternative for C–H activation, but this approach usually requires high overpotential and homogeneous mediators. Here, we design electron-deficient W₂C nanocrystal-based electrodes to boost the heterogeneous activation of C–H bonds under mild conditions via an additive-free, purely heterogeneous electrocatalytic strategy. The electron density of W₂C nanocrystals is tuned by constructing Schottky heterojunctions with nitrogen-doped carbon support to facilitate the preadsorption and activation of benzylic C–H bonds of ethylbenzene on the W₂C surface, enabling a high turnover frequency (18.8 h⁻¹) at a comparably low work potential (2 V versus SCE). The pronounced electron deficiency of the W₂C nanocatalysts substantially facilitates the direct deprotonation process to ensure electrode durability without self-oxidation. The efficient oxidation process also boosts the balancing hydrogen production from as-formed protons on the cathode by a factor of 10 compared to an inert reference electrode. The whole process meets the requirements of atomic economy and electric energy utilization in terms of sustainable chemical synthesis.