Synergetic Function of the Single-Atom Ru–N₄ Site and Ru Nanoparticles for Hydrogen Production in a Wide pH Range and Seawater Electrolysis

Abstract

Hydrogen production by water splitting and seawater electrolysis is a promising alternative to develop clean hydrogen energy. The construction of high-efficiency and durable electrocatalysts for the hydrogen evolution reaction (HER) in a wide pH range and seawater is critical to overcoming the sluggish kinetic process. Herein, we develop an efficient catalytic material composed of a single-atom Ru–N4 site and Ru nanoparticles anchored on nitrogen-doped carbon (Ru1+NPs/N–C) through the coordination-pyrolysis strategy of the melamine formaldehyde resin. The Ru1+NPs/N–C catalyst shows outstanding HER activity with the smallest overpotentials, the lowest Tafel slopes, the highest mass activity and turnover frequency, as well as excellent stability in both acidic and alkaline media. Moreover, Ru1+NPs/N–C shows comparable hydrogen production performance and a higher faradic efficiency to 20% Pt/C in natural seawater and artificial simulated seawater. Theoretical calculations demonstrate that the strong synergistic effects between the Ru–N4 site and Ru nanoparticles modify the electronic structure to accelerate the HER kinetics. Ru nanoparticles can effectively realize dissociation of H2O to generate adsorbed hydrogen and also promote the single-atom Ru–N4 site to combine adsorbed hydrogen to H2 and desorption. This work provides a new perspective for designing high-efficiency hydrogen production electrocatalysts for large-scale seawater electrolysis.

Convenient Synthesis of a Ru Catalyst Containing Single Atoms and Nanoparticles on Nitrogen-Doped Carbon with Superior Hydrogen Evolution Reaction Activity in a Wide pH Range

“…Raman spectra showed that the peak intensity of the composite catalysts were significantly lower than that of the pure substrate, but the I D / I G intensity of the composite catalysts were lower than that of the pure substrate, which means that the graphitization degree of the substrate is slightly improved (Figure S3c). EPR spectra further revealed the microstructure difference of meso-NC, Ru/meso-NC-300 °C, and Ru/meso-NC-400 °C (Figure S3d). Compared with that of the original meso-NC, the degree of defects in Ru/meso-NC-300 °C and Ru/meso-NC-400 °C was significantly reduced, which indicates the anchoring effect between Ru and defects …”

Lattice Strain and Schottky Junction Dual Regulation Boosts Ultrafine Ruthenium Nanoparticles Anchored on a N-Modified Carbon Catalyst for H2 Production

“…Fitting of the cyclic voltammetry curve in the no Faraday region was used to calculate the double layer capacitance ( C dl ), which is positively correlated with the ECSA (Figure S11 and S12). The highest C dl of Ru NPs/NC-900 than that of other catalysts indicated the largest number of exposed active sites . The EIS analysis revealed the electron/proton transfer of the catalyst and electrolyte at the interface.…”

“…The highest C dl of Ru NPs/NC-900 than that of other catalysts indicated the largest number of exposed active sites. 49 The EIS analysis revealed the electron/proton transfer of the catalyst and electrolyte at the interface. The minimum charge transfer resistance of Ru NPs/NC-900 denoted the fastest electron/ proton transfer and excellent HER activity (Figure S13).…”

Mesoporous Nitrogen-Doped Graphitized Carbon for Recyclable Oxidation of Cyclohexene

“…Most homogeneous and heterogeneous catalysis use metal-based catalysts. − However, metals, especially precious metals, have some disadvantages, such as limited resources, high prices, easy deactivation, and difficult post-treatment (high economic cost of post-treatment and easy to lead to secondary pollution), which have become thorny problems restricting the industrial application . From the perspective of sustainable development and economic cost, the development of new carbon-based metal-free catalysts to replace metal-based catalysts will help alleviate the above problems and are expected to reduce the reliance of the catalytic industry on metals .…”