The intrinsic catalytic activity of palladium (Pd) is significantly enhanced in gold (Au)-Pd alloy nanoparticles (NPs) under visible light irradiation at ambient temperatures. The alloy NPs strongly absorb light and efficiently enhance the conversion of several reactions, including Suzuki-Miyaura cross coupling, oxidative addition of benzylamine, selective oxidation of aromatic alcohols to corresponding aldehydes and ketones, and phenol oxidation. The Au/Pd molar ratio of the alloy NPs has an important impact on performance of the catalysts since it determines both the electronic heterogeneity and the distribution of Pd sites at the NP surface, with these two factors playing key roles in the catalytic activity. Irradiating with light produces an even more profound enhancement in the catalytic performance of the NPs. For example, the best conversion rate achieved thermally at 30 °C for Suzuki-Miyaura cross coupling was 37% at a Au/Pd ratio of 1:1.86, while under light illumination the yield increased to 96% under the same conditions. The catalytic activity of the alloy NPs depends on the intensity and wavelength of incident light. Light absorption due to the Localized Surface Plasmon Resonance of gold nanocrystals plays an important role in enhancing catalyst performance. We believe that the conduction electrons of the NPs gain the light absorbed energy producing energetic electrons at the surface Pd sites, which enhances the sites' intrinsic catalytic ability. These findings provide useful guidelines for designing efficient catalysts composed of alloys of a plasmonic metal and a catalytically active transition metal for various organic syntheses driven by sunlight.
Metal oxides of earth-abundant elements are promising electrocatalysts to overcome the sluggish oxygen evolution and oxygen reduction reaction (OER/ORR) in many electrochemical energy-conversion devices. However, it is difficult to control their catalytic activity precisely. Here, a general three-stage synthesis strategy is described to produce a family of hybrid materials comprising amorphous bimetallic oxide nanoparticles anchored on N-doped reduced graphene oxide with simultaneous control of nanoparticle elemental composition, size, and crystallinity. Amorphous Fe Co O is obtained from Prussian blue analog nanocrystals, showing excellent OER activity with a Tafel slope of 30.1 mV dec and an overpotential of 257 mV for 10 mA cm and superior ORR activity with a large limiting current density of -5.25 mA cm at 0.6 V. A fabricated Zn-air battery delivers a specific capacity of 756 mA h g (corresponding to an energy density of 904 W h kg ), a peak power density of 86 mW cm and can be cycled over 120 h at 10 mA cm . Other two amorphous bimetallic, Ni Fe O and Ni Co O , are also produced to demonstrate the general applicability of this method for synthesizing binary metal oxides with controllable structures as electrocatalysts for energy conversion.
A novel high throughput method for synthesis and screening of customized proteinresistant surfaces was developed. This method is an inexpensive, fast, reproducible and scalable approach to synthesize and screen protein-resistance surfaces appropriate for a specific feed. The method is illustrated here by combining a high throughput platform (HTP) approach together with our patented photo-induced graft polymerization Additional Supporting Information may be found in the online version of this article.Correspondence concerning this article should be addressed to J. E. Kilduff at kilduff@rpi.edu; or G. Belfort at belfog@rpi.edu. (PGP) method developed for facile modification of commercial poly(aryl sulfone) membranes. This new HTP-PGP method was validated by comparison with our previous published results obtained using a bench-scale filtration assay of six well-studied monomers. Optimally-performing surfaces for resisting a model protein, bovine serum albumin (BSA), were identified from a library of 66 monomers. Surfaces were prepared via graft polymerization onto poly(ether sulfone) (PES) membranes and were evaluated using a protein adsorption assay followed by pressure-driven filtration. Bench-scale verification was conducted for selected monomers using HTP-PGP method; a good correlation with HTP-PGP results was found. V
Lighting the way: Through the combination of a UV‐grafting process with the photoresponsive properties of spiropyran molecules, an optically reversible switching membrane surface was developed. This process can be used in preference to inducing physical movement of long‐chain SAMs toward an electrode and as a result improve many industrial opportunities including those dependent on surface wettability and molecular adhesion.
An efficient and practical one-pot multicomponent reaction of amines with alkyne esters and chalcones promoted by I/PhI(OAc) has been developed under solvent-free ball-milling conditions to afford a variety of polysubstituted trans-2,3-dihydropyrroles in moderate to good yields. The present method features a short reaction time, mild reaction conditions, broad substrate scope, and feasibility of large-scale synthesis. Intriguingly, this protocol can also furnish the corresponding synthetically more attractive pyrroles with the addition of an oxidant in a one-pot way.
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