Nanoscaled and Atomic Ruthenium Electrocatalysts Confined Inside Super‐Hydrophilic Carbon Nanofibers for Efficient Hydrogen Evolution Reaction

Abstract

A series of Ru‐based catalysts have been developed for the hydrogen evolution reaction (HER) by the facile impregnation of copious and eco‐friendly bacterial cellulose (BC) with Ru(bpy)3Cl2 (bpy = 2,2′‐bipyridine) followed by pyrolysis. After the oxidation and molecular recomposition processes that occur within the BC precursors during pyrolysis, sub‐2 nm Ru nanoparticles (NPs) and atomic Ru species confined within surface‐oxidized N‐doped carbon nanofibers (CNFs) can be observed in the derived catalysts. The surface oxidation of CNFs leads the derived catalysts with super hydrophilicity and water‐absorbing capacity, and also provides dimensional confinement for the nanoscaled and atomic Ru species. With these added structural advantages and the component synergy, the derived catalysts show superior HER activities, for which the overpotentials are as low as 19.6 mV (1 m KOH) and 55.0 mV (0.5 m H2SO4) for the most active case at the current density of 10 mA cm−2. Moreover, superior HER activity can be also achieved for the catalysts derived with a wide range of Ru loadings. Finally, the influence of Ru NP size on HER activity is investigated by density functional theory simulations. This method provides a reliable protocol for preparing highly active HER catalysts for scale‐up applications.

Ru@Ni3S2 nanorod arrays as highly efficient electrocatalysts for the alkaline hydrogen evolution reaction

“…In the highresolution N 1s spectrum, the N 1s peak was deconvoluted into three peaks: N-H (399.2 eV) and nitrogen cationic radicals (-N + -, 403.8 eV) of polyaniline and N-Ru (399.8 eV). 52,70,71 Meanwhile the Ru 3d 3/2 peak could be fitted to Ru 0 (280.6 eV) and Ru-N (282.1 eV), 52 further confirming the formation of the Ru-N bond. The ratio of Ru/Ru-N species changes to be about 1.25, which might result from the partial reduction of Ru 3+ during the electrodeposition of PANI.…”

Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

“…The anchoring style has also been extensively studied with the Ni/Ni‐N 4 , [ 100 ] Ru/Fe‐N x , [ 101 ] Ru/Ru‐N x . [ 102 ] It should be noted that the above cooperative effect of these anchoring‐type sites employed simplified theoretical models, which diminish the particle size into cluster model or even atomic aggregation. The adsorption sites were normally chosen as those atoms around the strongly coupled M 1 /M 2 ‐H x interfaces. …”

Highly dispersed Ru nanoclusters anchored on B,N co-doped carbon nanotubes for water splitting

“…2a are assigned to the CC bond, C–N or C–O bonds and the overlap with Ru 3d 5/2 , respectively. 13,44,45 The observation of the C–N species in the high-resolution C 1s spectrum indicates that the N atoms have been incorporated in the carbon matrix. The peaks at 398.4, 399.8 and 401.6 eV (Fig.…”

“…11 The abundant functional groups on the surface such as –OH, –COOH, –NH 2 , and so on, will provide many favorable sites for the fabrication of multicomponent photo- and electroactive catalysts. 12–16 With the advances of electrocatalyst studies, it is found that the introduction of heteroatoms in a carbon support plays an important role in regulating the interaction between the support and noble metal particles, and as a result optimizes the catalytic activity. For example, N-doped CNTs have been investigated for a long time as promising substrate materials in the energy conversion and catalytic fields.…”