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S. Bossmann

Kansas State University, Chemistry, Faculty Member

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Papers

Supramolekular Sensibilisatoren zum Photoinduzierten Elektronentransfer

Biomimetic Models Based on Ru-Polypyridine-Complexes : Electron Transfer in Supramolecular Assemblies

Journal of Information Recording, 1998

An integrated system for delivering hyperthermia to small-animal targets under 14 T ultra-high field MRI guidance 1

Ruthenium(II)-Tris-Bipyridin Und Titandioxid : Photokatalysatoren Zum Solarinduzierten Abbau Von Schadstoffen

Biomimetische Photosysteme zur sakrifiziellen Wasserreduktion / Novel Biomimetic Systems for Visible Light Induced Water Reduction

Zeitschrift für Naturforschung B, 1993

Novel microheterogeneous systems for the direct photoreduction of water using visible light in an... more Novel microheterogeneous systems for the direct photoreduction of water using visible light in analogy to the photochemical reaction center of Rhodopseudomonas viridis are described in detail. These physical model systems for photosynthesis feature the recently synthesized bisheteroleptic metal complexes [Ru(bpy)2(PP)]Cl2, [Ru(bpy)2(PPB)]Cl2, [Ru(bpy)2(PPB-pCl)]Cl2 and [Ru(bpy)3]Cl2, adsorbed on a negatively charged SiO2—TiO2-colloid, the zwitterionic electron relay PVS and a long-term stable and highly efficient TiO2—Pt-“antenna” catalyst as well as TEOA as sacrificial electron donor. Evidence for the directed absorption of the sensitizers on the SiO2—TiO2-colloid is taken from UV-VIS-measurements, steady-state luminescence-spectroscopy and the quantum yields for PVS-reduction. The hydrogen production in the presence of the SiO2—TiO2-colloid is clearly enhanced and proofs the validity of the underlying concept of physical model systems for photosynthesis.

Long-range photoinduced electron transfer through a DNA helix

Science, 1993

Rapid photoinduced electron transfer is demonstrated over a distance of greater than 40 angstroms... more Rapid photoinduced electron transfer is demonstrated over a distance of greater than 40 angstroms between metallointercalators that are tethered to the 5&#39; termini of a 15-base pair DNA duplex. An oligomeric assembly was synthesized in which the donor is Ru(phen)2dppz2+ (phen, phenanthroline, and dppz, dipyridophenazine) and the acceptor is Rh(phi)2phen3+ (phi, phenanthrenequinone diimine). These metal complexes are intercalated either one or two base steps in from the helix termini. Although the ruthenium-modified oligonucleotide hybridized to an unmodified complement luminesces intensely, the ruthenium-modified oligomer hybridized to the rhodium-modified oligomer shows no detectable luminescence. Time-resolved studies point to a lower limit of 10(9) per second for the quenching rate. No quenching was observed upon metallation of two complementary octamers by Ru(phen)3(2+) and Rh(phen)3(3+) under conditions where the phen complexes do not intercalate. The stacked aromatic heterocycles of the DNA duplex therefore serve as an efficient medium for coupling electron donors and acceptors over very long distances.

Fast photoinduced electron transfer through DNA intercalation

Proceedings of the National Academy of Sciences, 1994

We report evidence for fast photoinduced electron transfer mediated by the DNA helix that require... more We report evidence for fast photoinduced electron transfer mediated by the DNA helix that requires metal complexes that are avid intercalators of DNA. Here the donor bis(phenanthroline)(dipyridophenazine)ruthenium(II) [Ru(phen)2dppz2+] and acceptor bis(9,10-phenanthrenequinone diimine)(phenanthroline)rhodium(III) [Rh(phi)2phen3+] intercalate into DNA with Kb > 10(6) M-1. Luminescence quenching experiments in the presence of two different lengths of DNA yield upward-curving Stern-Volmer plots and the loss of luminescence intensity far exceeds the change in emission lifetimes. In the presence of a nonintercalative electron acceptor, Ru(NH3)3+(6), Ru(phen)2dppz2+ luminescence is quenched much less efficiently compared to that found for the intercalative Rh(phi)2phen3+ quencher and follows linear Stern-Volmer kinetics; steady-state and time-resolved Stern-Volmer plots are comparable in scale. These experiments are consistent with a model involving fast long-range electron transfer be...

Biomimetic approaches to the construction of supramolecular catalysts: titanium dioxide—platinum antenna catalysts to reduce water using visible light

Journal of Photochemistry and Photobiology A: Chemistry, 1993

Acid monolayer functionalized iron oxide nanoparticles as catalysts for carbohydrate hydrolysis

Green Chemistry, 2014

New Evidence against Hydroxyl Radicals as Reactive Intermediates in the Thermal and Photochemically Enhanced Fenton Reactions

The Journal of Physical Chemistry A, 1998

Carbon dioxide hydrogenation to aromatic hydrocarbons by using an iron/iron oxide nanocatalyst

Beilstein journal of nanotechnology, 2014

The quest for renewable and cleaner energy sources to meet the rapid population and economic grow... more The quest for renewable and cleaner energy sources to meet the rapid population and economic growth is more urgent than ever before. Being the most abundant carbon source in the atmosphere of Earth, CO2 can be used as an inexpensive C1 building block in the synthesis of aromatic fuels for internal combustion engines. We designed a process capable of synthesizing benzene, toluene, xylenes and mesitylene from CO2 and H2 at modest temperatures (T = 380 to 540 °C) employing Fe/Fe3O4 nanoparticles as catalyst. The synthesis of the catalyst and the mechanism of CO2-hydrogenation will be discussed, as well as further applications of Fe/Fe3O4 nanoparticles in catalysis.

ChemInform Abstract: Crown Ether Linked Ruthenium Coronates. A New Type of Photostable Electron Transfer Sensitizers

ChemInform, 1993

Ruthenium Polypyridine Complexes. On the Route to Biomimetic Assemblies as Models for the Photosynthetic Reaction Center

Accounts of Chemical Research, 2001

ChemInform Abstract: An Electron Spin Polarization Study of the Interaction of Photoexcited Triplet Molecules with Mono- and Polynitroxyl Stable Free Radicals

ChemInform, 1993

New insights into the mechanisms of the thermal Fenton reactions occurring using different iron(II)-complexes

Water science and technology : a journal of the International Association on Water Pollution Research, 2004

Although the Fenton reagent (a mixture of hydrogen peroxide and an iron(II) salt) has been known ... more Although the Fenton reagent (a mixture of hydrogen peroxide and an iron(II) salt) has been known for more than a century, the manifold mechanisms occurring during the thermal Fenton reaction are still under discussion. Indeed, this discussion served as a powerful driving force for the steadily increasing insight into the field of inorganic radical and electron transfer chemistry. In this work, an experimental approach towards the elucidation of the first steps taking place in the reaction between several iron(II)-complexes and hydrogen peroxide (H2O2) in water at pH = 3.0 is presented. 2,4-xylidine (2,4-dimethylaniline) reacts differently with reactive intermediates via the addition or hydrogen abstraction by the hydroxyl radical (HO*) or electron transfer reactions to higher valent iron-species, such as a hydrated ferryl-complex (Fe(IV)). The chemical reactivity of the employed iron(II)-complexes with H2O2 differed strongly depending on their ground-state one-electron oxidation pot...

An N,N'-dialkyl-4,4'-bipyridinium-modified titanium-dioxide photocatalyst for water remediation--observation and application of supramolecular effects in photocatalytic degradation of pi-donor organic compounds

Fresenius' journal of analytical chemistry, 2001

The photocatalytic activity of TiO2 (Degussa P-25) modified with a 4,4'-bipyridinium monolaye... more The photocatalytic activity of TiO2 (Degussa P-25) modified with a 4,4'-bipyridinium monolayer (V2+-TiO2) has been compared with that of conventional TiO2-P-25 by investigating the efficiency of degradation of a series of four organic model compounds with increasing pi-donor capacity (2,4-xylidine, 2,4-dimethylphenol, hydroquinone, and dimethylhydroquinone). As far as the mechanism of the first oxidation reaction is concerned, evidence for the formation of supramolecular donor-acceptor complexes with the bipyridinium units at the semiconductor surface was obtained by comparison of the Langmuir-adsorption characteristics and the efficiencies of photodegradation of the different substrates. Furthermore, the main intermediates of the photocatalytic degradation of 2,4-xylidine were identified, and the presence of 2,4-dimethylphenol indicates that the main pathway of substrate oxidation proceeds via electron transfer from the adsorbed organic substrate to the "holes" within...

Optimal experimental design and artificial neural networks applied to the photochemically enhanced Fenton reaction

by S. Bossmann and R Guardani

Water science and technology : a journal of the International Association on Water Pollution Research, 2001

Among advanced oxidation processes (AOPs), the photochemically enhanced Fenton reaction may be co... more Among advanced oxidation processes (AOPs), the photochemically enhanced Fenton reaction may be considered as one of the most efficient for the degradation of contaminants in industrial wastewater. This process involves a series of complex reactions. Therefore, an empirical model based on artificial neural networks has been developed for fitting the experimental data obtained in a laboratory batch reactor for the degradation of 2,4-dimethyl aniline (2,4-xylidine), chosen as a model pollutant. The model describes the evolution of the pollutant concentration during irradiation time as a function of the process conditions. It has been used for simulating the behavior of the reaction system in sensitivity studies aimed at optimizing the amounts of reactants employed in the process, an iron(III) salt and hydrogen peroxide, as well as the temperature. The results show that the process is most sensitive to the concentration of iron(III) salt and temperature, whereas the concentration of hyd...

Degradation of polyvinyl alcohol (PVA) by homogeneous and heterogeneous photocatalysis applied to the photochemically enhanced Fenton reaction

Water science and technology : a journal of the International Association on Water Pollution Research, 2001

The reaction mechanism of the oxidative degradation of polyvinyl alcohol (PVA) by the photochemic... more The reaction mechanism of the oxidative degradation of polyvinyl alcohol (PVA) by the photochemically enhanced Fenton reaction was studied using a homogeneous (Fe2+(aq) + H2O2) and a heterogeneous reaction system (iron(III)-exchanged zeolite Y+ H2O2). In the homogeneous Fenton system, efficient degradation was observed in a batch reactor, equipped with a medium pressure mercury arc in a Pyrex envelope and employing 80% of the stoichiometric amount of H2O2 required for the total oxidation of PVA and a concentration ratio as low as I mole of iron(II) sulfate per 20 moles of PVA sub-units (C2H40). Model PVA polymers of three different molecular weights (15,000, 49,000 and 100,000 g mol(-1)) were found to follow identical degradation patterns. Strong experimental evidence supports the formation of supermacromolecules (MW: 1-5 x 10(6) g/mol) consisting of oxidized PVA and trapped iron(III) at an early reaction stage. Low molecular weight intermediates, such as oxalic acid, formic acid or...

Green synthesis of soy polyol using acidic iron nanoparticle catalyst

Photochemistry of the singlet oxygen O-2((1)Delta(g)) sensitizer perinaphthenone (phenalenone) in N,N '-dimethylacetamide and 1,4-dioxane

New Journal of Chemistry, 1999

ABSTRACT

Supramolekular Sensibilisatoren zum Photoinduzierten Elektronentransfer

Biomimetic Models Based on Ru-Polypyridine-Complexes : Electron Transfer in Supramolecular Assemblies

Journal of Information Recording, 1998

An integrated system for delivering hyperthermia to small-animal targets under 14 T ultra-high field MRI guidance 1

Ruthenium(II)-Tris-Bipyridin Und Titandioxid : Photokatalysatoren Zum Solarinduzierten Abbau Von Schadstoffen

Biomimetische Photosysteme zur sakrifiziellen Wasserreduktion / Novel Biomimetic Systems for Visible Light Induced Water Reduction

Zeitschrift für Naturforschung B, 1993

Novel microheterogeneous systems for the direct photoreduction of water using visible light in an... more Novel microheterogeneous systems for the direct photoreduction of water using visible light in analogy to the photochemical reaction center of Rhodopseudomonas viridis are described in detail. These physical model systems for photosynthesis feature the recently synthesized bisheteroleptic metal complexes [Ru(bpy)2(PP)]Cl2, [Ru(bpy)2(PPB)]Cl2, [Ru(bpy)2(PPB-pCl)]Cl2 and [Ru(bpy)3]Cl2, adsorbed on a negatively charged SiO2—TiO2-colloid, the zwitterionic electron relay PVS and a long-term stable and highly efficient TiO2—Pt-“antenna” catalyst as well as TEOA as sacrificial electron donor. Evidence for the directed absorption of the sensitizers on the SiO2—TiO2-colloid is taken from UV-VIS-measurements, steady-state luminescence-spectroscopy and the quantum yields for PVS-reduction. The hydrogen production in the presence of the SiO2—TiO2-colloid is clearly enhanced and proofs the validity of the underlying concept of physical model systems for photosynthesis.

Long-range photoinduced electron transfer through a DNA helix

Science, 1993

Rapid photoinduced electron transfer is demonstrated over a distance of greater than 40 angstroms... more Rapid photoinduced electron transfer is demonstrated over a distance of greater than 40 angstroms between metallointercalators that are tethered to the 5&#39; termini of a 15-base pair DNA duplex. An oligomeric assembly was synthesized in which the donor is Ru(phen)2dppz2+ (phen, phenanthroline, and dppz, dipyridophenazine) and the acceptor is Rh(phi)2phen3+ (phi, phenanthrenequinone diimine). These metal complexes are intercalated either one or two base steps in from the helix termini. Although the ruthenium-modified oligonucleotide hybridized to an unmodified complement luminesces intensely, the ruthenium-modified oligomer hybridized to the rhodium-modified oligomer shows no detectable luminescence. Time-resolved studies point to a lower limit of 10(9) per second for the quenching rate. No quenching was observed upon metallation of two complementary octamers by Ru(phen)3(2+) and Rh(phen)3(3+) under conditions where the phen complexes do not intercalate. The stacked aromatic heterocycles of the DNA duplex therefore serve as an efficient medium for coupling electron donors and acceptors over very long distances.

Fast photoinduced electron transfer through DNA intercalation

Proceedings of the National Academy of Sciences, 1994

We report evidence for fast photoinduced electron transfer mediated by the DNA helix that require... more We report evidence for fast photoinduced electron transfer mediated by the DNA helix that requires metal complexes that are avid intercalators of DNA. Here the donor bis(phenanthroline)(dipyridophenazine)ruthenium(II) [Ru(phen)2dppz2+] and acceptor bis(9,10-phenanthrenequinone diimine)(phenanthroline)rhodium(III) [Rh(phi)2phen3+] intercalate into DNA with Kb > 10(6) M-1. Luminescence quenching experiments in the presence of two different lengths of DNA yield upward-curving Stern-Volmer plots and the loss of luminescence intensity far exceeds the change in emission lifetimes. In the presence of a nonintercalative electron acceptor, Ru(NH3)3+(6), Ru(phen)2dppz2+ luminescence is quenched much less efficiently compared to that found for the intercalative Rh(phi)2phen3+ quencher and follows linear Stern-Volmer kinetics; steady-state and time-resolved Stern-Volmer plots are comparable in scale. These experiments are consistent with a model involving fast long-range electron transfer be...

Biomimetic approaches to the construction of supramolecular catalysts: titanium dioxide—platinum antenna catalysts to reduce water using visible light

Journal of Photochemistry and Photobiology A: Chemistry, 1993

Acid monolayer functionalized iron oxide nanoparticles as catalysts for carbohydrate hydrolysis

Green Chemistry, 2014

New Evidence against Hydroxyl Radicals as Reactive Intermediates in the Thermal and Photochemically Enhanced Fenton Reactions

The Journal of Physical Chemistry A, 1998

Carbon dioxide hydrogenation to aromatic hydrocarbons by using an iron/iron oxide nanocatalyst

Beilstein journal of nanotechnology, 2014

The quest for renewable and cleaner energy sources to meet the rapid population and economic grow... more The quest for renewable and cleaner energy sources to meet the rapid population and economic growth is more urgent than ever before. Being the most abundant carbon source in the atmosphere of Earth, CO2 can be used as an inexpensive C1 building block in the synthesis of aromatic fuels for internal combustion engines. We designed a process capable of synthesizing benzene, toluene, xylenes and mesitylene from CO2 and H2 at modest temperatures (T = 380 to 540 °C) employing Fe/Fe3O4 nanoparticles as catalyst. The synthesis of the catalyst and the mechanism of CO2-hydrogenation will be discussed, as well as further applications of Fe/Fe3O4 nanoparticles in catalysis.

ChemInform Abstract: Crown Ether Linked Ruthenium Coronates. A New Type of Photostable Electron Transfer Sensitizers

ChemInform, 1993

Ruthenium Polypyridine Complexes. On the Route to Biomimetic Assemblies as Models for the Photosynthetic Reaction Center

Accounts of Chemical Research, 2001

ChemInform Abstract: An Electron Spin Polarization Study of the Interaction of Photoexcited Triplet Molecules with Mono- and Polynitroxyl Stable Free Radicals

ChemInform, 1993

New insights into the mechanisms of the thermal Fenton reactions occurring using different iron(II)-complexes

Water science and technology : a journal of the International Association on Water Pollution Research, 2004

Although the Fenton reagent (a mixture of hydrogen peroxide and an iron(II) salt) has been known ... more Although the Fenton reagent (a mixture of hydrogen peroxide and an iron(II) salt) has been known for more than a century, the manifold mechanisms occurring during the thermal Fenton reaction are still under discussion. Indeed, this discussion served as a powerful driving force for the steadily increasing insight into the field of inorganic radical and electron transfer chemistry. In this work, an experimental approach towards the elucidation of the first steps taking place in the reaction between several iron(II)-complexes and hydrogen peroxide (H2O2) in water at pH = 3.0 is presented. 2,4-xylidine (2,4-dimethylaniline) reacts differently with reactive intermediates via the addition or hydrogen abstraction by the hydroxyl radical (HO*) or electron transfer reactions to higher valent iron-species, such as a hydrated ferryl-complex (Fe(IV)). The chemical reactivity of the employed iron(II)-complexes with H2O2 differed strongly depending on their ground-state one-electron oxidation pot...

An N,N'-dialkyl-4,4'-bipyridinium-modified titanium-dioxide photocatalyst for water remediation--observation and application of supramolecular effects in photocatalytic degradation of pi-donor organic compounds

Fresenius' journal of analytical chemistry, 2001

The photocatalytic activity of TiO2 (Degussa P-25) modified with a 4,4'-bipyridinium monolaye... more The photocatalytic activity of TiO2 (Degussa P-25) modified with a 4,4'-bipyridinium monolayer (V2+-TiO2) has been compared with that of conventional TiO2-P-25 by investigating the efficiency of degradation of a series of four organic model compounds with increasing pi-donor capacity (2,4-xylidine, 2,4-dimethylphenol, hydroquinone, and dimethylhydroquinone). As far as the mechanism of the first oxidation reaction is concerned, evidence for the formation of supramolecular donor-acceptor complexes with the bipyridinium units at the semiconductor surface was obtained by comparison of the Langmuir-adsorption characteristics and the efficiencies of photodegradation of the different substrates. Furthermore, the main intermediates of the photocatalytic degradation of 2,4-xylidine were identified, and the presence of 2,4-dimethylphenol indicates that the main pathway of substrate oxidation proceeds via electron transfer from the adsorbed organic substrate to the "holes" within...

Optimal experimental design and artificial neural networks applied to the photochemically enhanced Fenton reaction

by S. Bossmann and R Guardani

Water science and technology : a journal of the International Association on Water Pollution Research, 2001

Among advanced oxidation processes (AOPs), the photochemically enhanced Fenton reaction may be co... more Among advanced oxidation processes (AOPs), the photochemically enhanced Fenton reaction may be considered as one of the most efficient for the degradation of contaminants in industrial wastewater. This process involves a series of complex reactions. Therefore, an empirical model based on artificial neural networks has been developed for fitting the experimental data obtained in a laboratory batch reactor for the degradation of 2,4-dimethyl aniline (2,4-xylidine), chosen as a model pollutant. The model describes the evolution of the pollutant concentration during irradiation time as a function of the process conditions. It has been used for simulating the behavior of the reaction system in sensitivity studies aimed at optimizing the amounts of reactants employed in the process, an iron(III) salt and hydrogen peroxide, as well as the temperature. The results show that the process is most sensitive to the concentration of iron(III) salt and temperature, whereas the concentration of hyd...

Degradation of polyvinyl alcohol (PVA) by homogeneous and heterogeneous photocatalysis applied to the photochemically enhanced Fenton reaction

Water science and technology : a journal of the International Association on Water Pollution Research, 2001

The reaction mechanism of the oxidative degradation of polyvinyl alcohol (PVA) by the photochemic... more The reaction mechanism of the oxidative degradation of polyvinyl alcohol (PVA) by the photochemically enhanced Fenton reaction was studied using a homogeneous (Fe2+(aq) + H2O2) and a heterogeneous reaction system (iron(III)-exchanged zeolite Y+ H2O2). In the homogeneous Fenton system, efficient degradation was observed in a batch reactor, equipped with a medium pressure mercury arc in a Pyrex envelope and employing 80% of the stoichiometric amount of H2O2 required for the total oxidation of PVA and a concentration ratio as low as I mole of iron(II) sulfate per 20 moles of PVA sub-units (C2H40). Model PVA polymers of three different molecular weights (15,000, 49,000 and 100,000 g mol(-1)) were found to follow identical degradation patterns. Strong experimental evidence supports the formation of supermacromolecules (MW: 1-5 x 10(6) g/mol) consisting of oxidized PVA and trapped iron(III) at an early reaction stage. Low molecular weight intermediates, such as oxalic acid, formic acid or...

Green synthesis of soy polyol using acidic iron nanoparticle catalyst

Photochemistry of the singlet oxygen O-2((1)Delta(g)) sensitizer perinaphthenone (phenalenone) in N,N '-dimethylacetamide and 1,4-dioxane

New Journal of Chemistry, 1999

ABSTRACT