A General Route to Flame Aerosol Synthesis and In Situ Functionalization of Mesoporous Silica.

Mesoporous silica is a versatile material for energy, environmental, and medical applications. Here, for the first time, we report a flame aerosol synthesis method for a class of mesoporous silica with hollow structure and specific surface area exceeding 1000 m2 g-1 . We show its superior performance in water purification, as a drug carrier, and in thermal insulation. Moreover, we propose a general route to produce mesoporous nanoshell-supported nanocatalysts by in situ decoration with active nanoclusters, including noble metal (Pt/SiO2 ), transition metal (Ni/SiO2 ), metal oxide (CrO3 /SiO2 ), and alumina support (Co/Al2 O3 ). As a prototypical application, we perform dry reforming of methane using Ni/SiO2 , achieving constant 97 % CH4 and CO2 conversions for more than 200 hours, dramatically outperforming an MCM-41 supported Ni catalyst. This work provides a scalable strategy to produce mesoporous nanoshells and proposes an in situ functionalization mechanism to design and produce flexible catalysts for many reactions.

Single-Step Flame Aerosol Synthesis of Active and Stable Nanocatalysts for the Dry Reforming of Methane.

We introduce a flame-based aerosol process for producing supported non-noble metal nanocatalysts from inexpensive aqueous metal salt solutions, using catalysts for the dry reforming of methane (DRM) as a prototype. A flame-synthesized nickel-doped magnesia (MgO) nanocatalyst (NiMgO-F) was fully physicochemically characterized and tested in a flow reactor system, where it showed stable DRM activity from 500 to 800 °C. A kinetic study was conducted, and apparent activation energies were extracted for the temperature range of 500-650 °C. It was then compared with a Ni-decorated MgO nanopowder prepared by wet impregnation of (1) flame-synthesized MgO (NiMgO-FI) and (2) a commercial MgO nanopowder (NiMgO-CI) and with (3) a NiMgO catalyst prepared by co-precipitation (NiMgO-CP). NiMgO-F showed the highest catalytic activity per mass and per metallic surface area and was stable for continuous H2 production at 700 °C for 50 h. Incorporation of potential promoters and co-catalysts was also demonstrated, but none showed significant performance improvement. More broadly, nanomaterials produced by this approach could be used as binary or multicomponent catalysts for numerous catalytic processes.

Boron-hyperdoped silicon for the selective oxidative dehydrogenation of propane to propylene.

Boron containing catalysts have great potential in the oxidative dehydrogenation of propane. Herein, a series of 15, 25 and 42 at% boron-hyperdoped silicon catalysts synthesized by laser pyrolysis was studied. Boron-hyperdoped silicon samples showed >6 times higher propylene productivity than commercial h-BN at 450 °C.

Author Correction: Activating low-temperature diesel oxidation by single-atom Pt on TiO2 nanowire array.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Activating low-temperature diesel oxidation by single-atom Pt on TiO2 nanowire array.

Supported metal single atom catalysts (SACs) present an emerging class of low-temperature catalysts with high reactivity and selectivity, which, however, face challenges on both durability and practicality. Herein, we report a single-atom Pt catalyst that is strongly anchored on a robust nanowire forest of mesoporous rutile titania grown on the channeled walls of full-size cordierite honeycombs. This Pt SAC exhibits remarkable activity for oxidation of CO and hydrocarbons with 90% conversion at temperatures as low as ~160 oC under simulated diesel exhaust conditions while using 5 times less Pt-group metals than a commercial oxidation catalyst. Such an excellent low-temperature performance is sustained over hydrothermal aging and sulfation as a result of highly dispersed and isolated active single Pt ions bonded at the Ti vacancy sites with 5 or 6 oxygen ions on titania nanowire surfaces.

Dendrimer-mediated synthesis of supported rhodium nanoparticles with controlled size: effect of pH and dialysis.

Rh-dendrimer nanocomposites were synthesized in solution under different conditions and were subsequently used as precursors for the preparation of ZrO2-supported Rh nanoparticles. Elemental analysis, UV-vis, XPS, and STEM measurements were used to estimate the extent of the Rh-dendrimer interactions and to illustrate how the solution pH and dialysis affect the number of Rh atoms complexed with each dendrimer molecule, as well as the final size of the ZrO2-supported Rh particles. When the solution acidity was not controlled and the solution was not purified by dialysis, Rh particles with sizes in the 1-6 nm range were formed on the ZrO2 support. In contrast, the formation of nearly uniform Rh particles was observed when the synthesis was performed under controlled pH and dialysis conditions. Furthermore, the size of these Rh particles can be regulated by controlling the Rh/dendrimer ratio in the original solution.