RESUMO
Hydrolysis of ammonia borane (NH3BH3, AB) involves multiple undefined steps and complex adsorption and activation, so single or dual sites are not enough to rapidly achieve the multi-step catalytic processes. Designing multi-site catalysts is necessary to enhance the catalytic performance of AB hydrolysis reactions but revealing the matching reaction mechanisms of AB hydrolysis is a great challenge. In this work, we propose to construct RuPt-Ti multi-site catalysts to clarify the multi-site tandem activation mechanism of AB hydrolysis. Experimental and theoretical studies reveal that the multi-site tandem mode can respectively promote the activation of NH3BH3 and H2O molecules on the Ru and Pt sites as well as facilitate the fast transfer of *H and the desorption of H2 on Ti sites at the same time. RuPt-Ti multi-site catalysts exhibit the highest turnover frequency (TOF) of 1293â min-1 for AB hydrolysis reaction, outperforming the single-site Ru, dual-site RuPt and Ru-Ti catalysts. This study proposes a multi-site tandem concept for accelerating the dehydrogenation of hydrogen storage material, aiming to contribute to the development of cleaner, low-carbon, and high-performance hydrogen production systems.
RESUMO
In recent years, there has been increasing interest in synthesis of reduced graphene oxide (rGO)-metal oxide semiconductor (MOS) nanocomposites for room temperature gas sensing applications. Generally, the sensitivity of a MOS can be obviously enhanced by the incorporation of rGO. However, a lack of knowledge regarding how rGO can enhance gas-sensing performances of MOSs impedes its sensing applications. Herein, in order to get an insight into the sensing mechanism of rGO-MOS nanocomposites and further improve the sensing performances of NiO-based sensors at room temperature, an rGO-NiO nanocomposite was synthesized. Through a comparison study on room temperature NO2 sensing of rGO-NiO and pristine NiO, an inverse gas-sensing behavior in different NO2 concentration ranges was observed and the sensitivity of rGO-NiO was enhanced obviously in the high concentration range (7-60 ppm). Significantly, the stimulating effect of rGO on the recovery rate was confirmed by the sensing characteristics of rGO-NiO that was advantageous for the development of NO2 sensors at room temperature. By comprehending the electronic interactions between the rGO-MOS nanocomposite and the target gas, this work may open up new possibilities for further improvement of graphene-based hybrid materials with even higher sensing performances.
RESUMO
Rare-earth-based AB2-type compounds with Laves phase structure are readily subject to hydrogen-induced amorphization and disproportionation upon hydrogenation. In this work, we conducted the Sc alloying on Y0.95Ni2 to improve its hydrogen storage properties. The results show that the amorphization degree of Y0.95Ni2 deepens with the increasing hydrogenation time, pressure, and temperature. The Y(Sc)0.95Ni2 ternary compounds show a significant improvement in reversibility and dehydriding thermodynamics due to the reduced atomic radius ratio RA/RB and cell volume. Hydrogen-induced amorphization is fully eliminated in the Y0.25Sc0.7Ni2. The Y0.25Sc0.7Ni2 delivers a reversible hydrogen storage capacity of 0.94 wt.% and the dissociation pressure of 0.095 MPa at the minimum dehydrogenation temperature of 100 °C.