Rui You

Regulation of Coordination Number over Single Co Sites: Triggering the Efficient Electroreduction of CO2

The design of active, selective, and stable CO2 reduction electrocatalysts is still challenging. A series of atomically dispersed Co catalysts with different nitrogen coordination numbers were prepared and their CO2 electroreduction catalytic performance was explored. The best catalyst, atomically dispersed Co with two-coordinate nitrogen atoms, achieves both high selectivity and superior activity with 94 % CO formation Faradaic efficiency and a current density of 18.1 mA cm-2 at an overpotential of 520 mV. The CO formation turnover frequency reaches a record value of 18 200 h-1 , surpassing most reported metal-based catalysts under comparable conditions. Our experimental and theoretical results demonstrate that lower a coordination number facilitates activation of CO2 to the CO2.- intermediate and hence enhances CO2 electroreduction activity.

Atomically Dispersed Ru on Ultrathin Pd Nanoribbons

We report a one-pot synthesis of atomically dispersed Ru on ultrathin Pd nanoribbons. By using synchrotron radiation photoemission spectroscopy (SRPES) and extended X-ray absorption fine structure (EXAFS) measurements in combination with aberration corrected high-resolution transmission electron microscopy (HRTEM), we show that atomically dispersed Ru with content up to 5.9% was on the surface of the ultrathin nanoribbon. Furthermore, the ultrathin Pd/Ru nanoribbons could remarkably prohibit the hydrogenolysis in chemoselective hydrogenation of C═C bonds, leading to an excellent catalytic selectivity compared with commercial Pd/C and Ru/C.

Enhancing both selectivity and coking-resistance of a single-atom Pd1/C3N4 catalyst for acetylene hydrogenation

Selective hydrogenation is an important industrial catalytic process in chemical upgrading, where Pd-based catalysts are widely used because of their high hydrogenation activities. However, poor selectivity and short catalyst lifetime because of heavy coke formation have been major concerns. In this work, atomically dispersed Pd atoms were successfully synthesized on graphitic carbon nitride (g-C3N4) using atomic layer deposition. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) confirmed the dominant presence of isolated Pd atoms without Pd nanoparticle (NP) formation. During selective hydrogenation of acetylene in excess ethylene, the g-C3N4-supported Pd NP catalysts had strikingly higher ethylene selectivities than the conventional Pd/Al2O3 and Pd/SiO2 catalysts. In-situ X-ray photoemission spectroscopy revealed that the considerable charge transfer from the Pd NPs to g-C3N4 likely plays an important role in the catalytic performance enhancement. More impressively, the single-atom Pd1/C3N4 catalyst exhibited both higher ethylene selectivity and higher coking resistance. Our work demonstrates that the single-atom Pd catalyst is a promising candidate for improving both selectivity and coking-resistance in hydrogenation reactions.

Ordered Porous Pd Octahedra Covered with Monolayer Ru Atoms

Monolayer Ru atoms covered highly ordered porous Pd octahedra have been synthesized via the underpotential deposition and thermodynamic control. Shape evolution from concave nanocube to octahedron with six hollow cavities was observed. Using aberration-corrected high-resolution transmission electron microscopy and X-ray photoelectron spectroscopy, we provide quantitative evidence to prove that only a monolayer of Ru atoms was deposited on the surface of porous Pd octahedra. The as-prepared monolayer Ru atoms covered Pd nanostructures exhibited excellent catalytic property in terms of semihydrogenation of alkynes.

Reaction Sensitivity of Ceria Morphology Effect on Ni/CeO2 Catalysis in Propane Oxidation Reactions

CeO2 nanocubes (c-CeO2), nanoparticles (p-CeO2), and nanorods calcined at 500 °C (r-CeO2-500) and 700 °C (r-CeO2-700) were used as supports to synthesize a series of Ni/CeO2 catalysts for the propane combustion and oxidative dehydrogenation of propane (ODHP) reactions. The Ni-CeO2 interaction greatly promotes the reducibility of CeO2, but CeO2 morphology-dependent Ni-CeO2 interaction was observed to form different speciation of Ni species (Ni2+ dissolved in CeO2, highly dispersive NiO, NiO aggregate) and oxygen species (strongly activated oxygen species, medially activated oxygen species, weakly activated oxygen species) in various Ni/CeO2 catalysts. Ni-CeO2 interaction is stronger in Ni/c-CeO2 catalysts than in other Ni/CeO2 catalysts. Different morphology-dependences of Ni/CeO2 catalysts in propane combustion and ODHP reactions were observed. The Ni/r-CeO2-500 catalyst with the largest strongly activated oxygen species is most catalytic active in the propane combustion reaction while the Ni/c-CeO2 catalyst with the largest amount of weakly activated oxygen species exhibits the best catalytic performance in the ODHP reaction. Thus, the CeO2 morphology engineering strategy is effective in finely tuning the metal-CeO2 interaction and the reactivity of oxygen species to meet the requirements of different types of catalytic oxidation reactions.