Nitrogen-Doped Carbon-Stabilized Ru Nanoclusters as Excellent Catalysts for Hydrogen Production

Abstract

The synthesis of ruthenium nanoclusters (NCs) is crucially important but challenging for hydrogen production. By taking advantage of confinement effect of nanopores in 3D porous carbon and urea as nitrogen source, we developed a straightforward method for preparation of uniform Ru NCs and simultaneous nitriding of the carbon scaffolds (Ru/3DNPC). The resulting Ru/3DNPC-500 had a measured overpotential of 15 mV at 10 mA cm–2 toward hydrogen evolution reaction as well as very high turnover frequency (584 mol of H2 (mol of Ru min)−1) for hydrolytic decomposition of ammonia–borane, outperforming many previously reported Ru-based catalysts. Ru NCs confined in 3DNPC substrate can supply numerous catalytically active sites for the reactions, thereby leading to high catalytic activity. The present synthetic strategy could open a new direction for preparing metal NCs catalysts.

Ruthenium Nanoparticles for Catalytic Water Splitting

“…The key role of Nd oping in C-supported Ru NP HERe lectrocatalysts under alkaline conditions is also supported by two recent contributions by Fan and co-workers. [77,78] These reports introduce Nd oping into CB and 3D carbon supports throught he pyrolysis of a[ Ru(bpy) 3 ] 2 + complex [77] or RuCl 3 /urea, [78] respectively, yieldings upported Ru NPs about1 .3 nm in size in both cases as best performing systems. Both electrocatalysts show low HER overpotentials (h 10 = 14-15 mV) and relatively high stabilities in 1.0 m KOH (1000 CV cycles) that outperform those of Pt/ C( Table 4, entries 14 and 15).…”

Ultrafine Pd Nanoparticles Supported on Soft Nitriding Porous Carbon for Hydrogen Production from Hydrolytic Dehydrogenation of Dimethyl Amine-Borane

“…Pd/NPC with Pd loading of 1.00 wt% are expected to supply substantial large number of active sites for DMAB hydrolysis to produce hydrogen. An XPS survey scan result clearly gives the information that the Pd/NPC is composed of C, Pd, N, and O, suggesting that Pd NPs are successfully introduced to the NPC support (Figure 2a) [22]. The surface atomic percentages of C, Pd, N and O were 71.21, 1.30, 10.98, and 16.53%, respectively.…”

“…Additionally, the peak located at 285.4 eV is ascribed to C=N [33,34], suggesting the successful nitrogen-doping of PC via the soft nitriding processing [35].The high-resolution Pd 3d core level spectrum (Figure 2d) can be divided into two groups peaks corresponding to oxidized Pd species as a result of the oxidation occurred on the surface of the catalyst during the preparation and characterization procedures. An XPS survey scan result clearly gives the information that the Pd/NPC is composed of C, Pd, N, and O, suggesting that Pd NPs are successfully introduced to the NPC support (Figure 2a) [22]. The surface atomic percentages of C, Pd, N and O were 71.21, 1.30, 10.98, and 16.53%, respectively.…”

“…In addition, the removal of such protecting molecules under harsh conditions also results in the loss of catalytic activity [21]. Recent studies have indicated that the heteroatom-doped carbon materials can be used as ideal platforms to synthesize ligand-free metal NPs for catalytic applications [17,[22][23][24]. However, most of the synthetic strategies for heteroatom-doping of carbon matrixes are conducted by strong acid treatment and high temperature calcination, leading to the production of carbon materials with relatively low content of heteroatom, which are adverse to the preparation of metal NPs with ultrafine sizes [25].…”

Photocatalytic H2 Evolution from Ammonia Borane: Improvement of Charge Separation and Directional Charge Transmission

“…[7,8] Solid-state hydrogen storage is a kind of hydrogen storage method, which uses physical or chemical changes between hydrogen and hydrogen storage materials to store hydrogen. [9][10][11] Among them, ammonia borane (NH 3 BH 3 , AB) is known as one of the most promising hydrogen storage materials because of its 19.6 wt% high hydrogen content. [11][12][13][14][15][16][17] The hydrolysis of AB could proceed rapidly to generate hydrogen (NH 3 BH 3 + 2H 2 O!…”