CO capture from industry sectors or directly from the atmosphere is drawing much attention on a global scale because of the drastic changes in the climate and ecosystem which pose a potential threat to human health and life on Earth. In the past decades, CO capture technology relied on classical liquid amine scrubbing. Due to its high energy consumption and corrosive property, CO capture using solid materials has recently come under the spotlight.
View Article and Find Full Text PDFThe adsorption states of N and H on MgO-supported Ru nanoparticles under conditions close to those of ammonia synthesis (AS; 1 atm, 250 °C) were uncovered by modulation-excitation infrared spectroscopy and density functional theory calculations using a nanoscale Ru particle model. The two most intense N adsorption peaks corresponded to the vertical chemisorption of N on the nanoparticle's top and bridge sites, while the remaining peaks were assigned to horizontally adsorbed N in view of the site heterogeneity of Ru nanoparticles. Long-term observations showed that vertically adsorbed N molecules gradually migrated from the top sites to the bridge sites.
View Article and Find Full Text PDFWe present a systematic study on the support effect of metal-organic frameworks (MOFs), regarding substrate adsorption. A remarkable enhancement of both catalytic activity and selectivity for the ethanol (EtOH) production reaction through acetic acid (AcOH) hydrogenation (AH) was observed on Pt nanoparticles supported on MOFs. The systematic study on catalysis using homogeneously loaded Pt catalysts, in direct contact with seven different MOF supports (MIL-125-NH, UiO-66-NH, HKUST-1, MIL-101, Zn-MOF-74, Mg-MOF-74, and MIL-121) (abbreviated as ), found that MOFs having a high affinity for the AcOH substrate (UiO-66-NH and MIL-125-NH) showed high catalytic activity for AH.
View Article and Find Full Text PDFDiscrimination between active and spectator species is an important and demanding task in catalysis research. A comparative study of the Pd-catalyzed CO hydrogenation using in situ diffuse reflectance IR Fourier transform spectroscopy (DRIFTS) in steady-state and dynamic (transient) experiments shows that the information on surface species differs significantly depending on the type of experiment. In order to discriminate between active species and spectator species not involved in the surface reactions, DRIFTS was combined with a transient technique, modulation excitation spectroscopy (MES).
View Article and Find Full Text PDFAn understanding of the chiral site-substrate interaction is a necessary prerequisite for the rational design and development of efficient heterogeneous asymmetric catalysts. For the enantioselective hydrogenation of α-ketoesters on cinchona-modified platinum, it has earlier been proposed that the crucial interaction is an N-H-O type hydrogen bonding between the quinuclidine N atom of cinchonidine and the α-carbonyl O atom of the substrate. The involved hydrogen atom has been proposed to originate either from protonation (in protic solvent) or from dissociatively adsorbed hydrogen (in aprotic solvent), but experimental evidence for the latter was lacking so far.
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