ORCID Profile
0000-0001-8090-5050
Current Organisation
Aarhus Universitet
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Publisher: Wiley
Date: 24-02-2020
Publisher: Wiley
Date: 30-03-2012
DOI: 10.1002/BIT.24500
Abstract: The use of microorganisms as support for reduction of dissolved Pd(II) to immobilized Pd(0) nanoparticles is an environmentally friendly approach for Pd recovery from waste. To better understand and engineer Pd(0) nanoparticle synthesis, one has to consider the mechanisms by which Pd(II) is reduced on microbial surfaces. Escherichia coli, Shewanella oneidensis, and Pseudomonas putida were used as model organisms in order to elucidate the role of microbial cells in Pd(II) reduction under acidic conditions. Pd(II) was reduced by formate under acidic conditions, and the process occurred substantially faster in the presence of cells as compared to cell-free controls. We found no difference between native (untreated) and autoclaved cells, and could demonstrate that even a non-enzymatic protein (bovine serum albumin) stimulated Pd(II) reduction as efficiently as bacterial cells. Amine groups readily interact with Pd(II), and to specifically test their role in surface-assisted Pd(II) reduction by formate, we replaced bacterial cells with polystyrene microparticles functionalized with amine or carboxyl groups. Amine-functionalized microparticles had the same effect on Pd(II) reduction as bacterial cells, and the effect could be h ered if the amine groups were blocked by acetylation. The interaction with amine groups was confirmed by infrared spectroscopy on whole cells and amine-functionalized microparticles. In conclusion, bio-supported Pd(II) reduction on microbial surfaces is possibly mediated by a non-enzymatic mechanism. We therefore suggest the use of amine-rich biomaterials rather than intact cells for Pd bio-recovery from waste.
Publisher: Swiss Chemical Society
Date: 24-09-2008
Abstract: Radical reactions offer many advantages over conventional chemical reactions, lending themselves to numerous bond forming processes and rearrangements that are, clean, rapid, and tolerant of a wide range of functional groups. This review provides a brief overview of the design concepts behind new reactions illustrating, in particular, their relevance for the efficient synthesis of biomolecules. Two general reactions are highlighted: single electron transfer (SET) using SmI2 and hydrogen transfer using reagents such as those based on tin, thiols and phosphorous reagents. Intermolecular influences that may direct radical reactions, such as partial protonation and radical complexation, are also discussed.
Publisher: Wiley
Date: 23-08-2011
DOI: 10.1002/BIT.23293
Abstract: Bimetallic nanoparticles are considered the next generation of nanocatalysts with increased stability and catalytic activity. Bio-supported synthesis of monometallic nanoparticles has been proposed as an environmentally friendly alternative to the conventional chemical and physical protocols. In this study we synthesize bimetallic bio-supported Pd-Au nanoparticles for the first time using microorganisms as support material. The synthesis involved two steps: (1) Formation of monometallic bio-supported Pd(0) and Au(0) nanoparticles on the surface of Cupriavidus necator cells, and (2) formation of bimetallic bio-supported nanoparticles by reduction of either Au(III) or Pd(II) on to the nanoparticles prepared in step one. Bio-supported monometallic Pd(0) or Au(0) nanoparticles were formed on the surface of C. necator by reduction of Pd(II) or Au(III) with formate. Addition of Au(III) or Pd(II) to the bio-supported particles resulted in increased particle size. UV-Vis spectrophotometry and HR-TEM analyses indicated that the previously monometallic nanoparticles had become fully or partially covered by Au(0) or Pd(0), respectively. Furthermore, Energy Dispersive Spectrometry (EDS) and Fast Fourier Transformation (FFT) analyses confirmed that the nanoparticles indeed were bimetallic. The bimetallic nanoparticles did not have a core-shell structure, but were superior to monometallic particles at reducing p-nitrophenol to p-aminophenol. Hence, formation of microbially supported nanoparticles may be a cheap and environmentally friendly approach for production of bimetallic nanocatalysts.
Publisher: Elsevier BV
Date: 07-2011
DOI: 10.1016/J.COLSURFB.2011.03.014
Abstract: The development of nanoparticles has greatly improved the catalytic properties of metals due to the higher surface to volume ratio of smaller particles. The production of nanoparticles is most commonly based on abiotic processes, but in the search for alternative protocols, bacterial cells have been identified as excellent scaffolds of nanoparticle nucleation, and bacteria have been successfully employed to recover and regenerate platinum group metals from industrial waste. We report on the formation of bio-supported palladium (Pd) nanoparticles on the surface of two bacterial species with distinctly different surfaces: the gram positive Staphylococcus sciuri and the gram negative Cupriavidus necator. We investigated how the type of bacterium and the amount of biomass affected the size and catalytic properties of the nanoparticles formed. By increasing the biomass:Pd ratio, we could produce bio-supported Pd nanoparticles smaller than 10nm in diameter, whereas lower biomass:Pd ratios resulted in particles ranging from few to hundreds of nm. The bio-supported Pd nanoparticle catalytic properties were investigated towards the Suzuki-Miyaura cross coupling reaction and hydrogenation reactions. Surprisingly, the smallest nanoparticles obtained at the highest biomass:Pd ratio showed no reactivity towards the test reactions. The lack of reactivity appears to be caused by thiol groups, which poison the catalyst by binding strongly to Pd. Different treatments intended to liberate particles from the biomass, such as burning or rinsing in acetone, did not re-establish their catalytic activity. Sulphur-free biomaterials should therefore be explored as more suitable scaffolds for Pd(0) nanoparticle formation.
No related grants have been discovered for Troels Skrydstrup.