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The formation of hydrogen on irradiating ferrous ion in aqueous solution or suspension was studied over a wide range of pH. In addition to the known reaction in acid solution which decreases in yield with increasing pH and required far UV light, there is an efficient reaction occurring between pH 6 and 9 which utilizes near UV light. The latter reaction is an approximately linear function of both the concentration of ferrous ion and the light intensity. The quantum yield of hydrogen from the suspension of Fe(OH)2 at pH 7.2 is very high: > or = 0.3. The quantum yield decreases by a factor of five at 1 mole percent of ferric ions. To explain these observations it is proposed that an intermediate formed on excitation of the Fe(OH)2 polymer is further reduced by a neighboring Fe(+2) to form H2. These results support the work of Braterman et al. (1983) which claimed that the near UV driven photooxidation of ferrous ions could be responsible for formation of the Banded Iron Formations on the early earth. The efficient photoreaction observed in the present work could also serve as a source of active reducing equivalents to reduce CO2 and thus provide a solution to a dilemma in the arguments on the role of reduced carbon in the origin of life.
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PMID:Efficient near ultraviolet light induced formation of hydrogen by ferrous hydroxide. 1154 Aug 91

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 formaldehyde were not found during PVA degradation in the homogeneous Fenton system, and we may deduce that the manifold of degradation reactions is mainly taking place within the super-macromolecules from which CO2 is directly released. However, in the heterogeneous Fenton system, the reaction behavior was found to be distinctly different: a decrease of the molecular weights of all three tested monodisperse PVA samples was observed by the broadening of the GPC-traces during irradiation, and oxalic acid was formed. The results lead to the mechanistic hypothesis that during the heterogeneous Fenton process, the cleavage of the PVA-chains may occur at random positions, the reactive centres being located inside the iron(III)-doped zeolite Y photocatalysts.
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PMID:Degradation of polyvinyl alcohol (PVA) by homogeneous and heterogeneous photocatalysis applied to the photochemically enhanced Fenton reaction. 1169 68

Treating pigmented lesions of the skin, especially deep dermal pigmentations, are difficult to achieve satisfactory results without complications. To treat dermal pigmentations, such as nevus of Ota and congenital nevus, the combined therapy of a resurfacing laser (CO2) and a selective photothermolytic laser (the Q-Switched Ruby Laser [QSRL]) was tried, and the results were compared with those treated with the QSRL alone. Combined laser therapy has been performed in 47 patients with nevus of Ota since 1995. The mean treatment period was 6 months and the mean number of treatment was five. Of 47 patients, 46 (98%) showed excellent results. To treat congenital nevus, combined laser therapy was used in 15 patients, and 12 (80%) showed good to excellent results. By combining resurfacing and selective lasers, the treatment period has been reduced by 2 to 3 months, and the number of treatments has been reduced two- to threefold. Furthermore, treatment of congenital nevus has become possible, which was not the case with the QSRL alone. The Er:YAG laser can be used for resurfacing instead of the CO2 laser because it causes less thermal damage and faster wound healing.
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PMID:Combined laser therapy for difficult dermal pigmentation: resurfacing and selective photothermolysis. 1175

Laboratory experiments were conducted in a two-stage horizontal muffle furnace in order to monitor emissions from batch combustion of polystyrene (PS) and identify conditions that minimize them. PS is a dominant component of municipal and hospital waste streams. Bench-scale combustion of small samples (0.5 g) of shredded styrofoam cups was conducted in air, using an electrically heated horizontal muffle furnace, kept at Tgas = 1000 degrees C. Upon devolatilization, combustion of the polymer took place in a diffusion flame over the sample. The gaseous combustion products were mixed with additional air in a venturi and were channeled to a secondary muffle furnace (afterburner) kept at Tgas = 900-1100 degrees C; residence time therein varied between 0.6 and 0.8 s. At the exits of the primary and the secondary furnace the emissions of CO, CO2, O2, NOx, particulates as well as volatile and semivolatile hydrocarbons, such as polycyclic aromatic hydrocarbons (PAH), were monitored. Online analyzers, gravimetric techniques, and gas chromatography coupled to mass spectrometry (GC-MS) were used. Experiments were also conducted with a high-temperature barrier filter, placed just before the exit of the primary furnace to prevent the particulates from entering into the secondary furnace. Results demonstrated the beneficial effect of the afterburner in reducing PAH concentrations, including those of mutagenic species such as benzo[a]pyrene. Concentrations of individual PAH exhibited a pronounced after burner temperature dependence, typically ranging from a small decrease at 900 degrees C to a larger degree of consumption at 1100 degrees C. Consumption of PAH was observed to be the dominant feature at 900 degrees C, while significant quantities of benzene and some of its derivatives, captured by means of carbosieve/Carbotrap adsorbents, were formed in the afterburner at a temperature of 1000 degrees C. In the primary furnace, about 30% of the mass of the initial polystyrene was converted into soot, while the total mass of PAH represented about 3% of the initial mass of combustible. The afterburner reduced the particulate (soot) emissions by only 20-30%, which indicates that once soot is formed its destruction is rather difficult because its oxidation kinetics are slow undertypical furnace conditions. Moreover, increasing the afterburnertemperature resulted in an increasing trend of soot emissions therefrom, which might indicate competition between soot oxidation and formation, with some additional formation occurring at the higher temperatures. Contrary to the limited effect of the afterburner, high-temperature filtration of the combustion effluent prior to the exit of the primary furnace allowed for effective soot oxidation inside of the ceramic filter. Filtration drastically reduced soot emissions, by more than 90%. Limited soot formation in the afterburner was again observed with increasing temperatures. The yields of both CO and CO2 were largely unaffected by the temperature of the afterburner but increased at the presence of the filter indicating oxidation therein. A previously developed kinetic model was used to identify major chemical reaction pathways involving PAH in the afterburner. The experimental data at the exit of the primary furnace was used as input to these model computations. A first evaluation of the predictive capability of the model was conducted for the case with ceramic filter and a temperature of 900 degrees C. The afterburner was approximated as a plug-flow reactor, and model predictions at a residence time of 0.8 s were compared to experimental data collected at its exit. In agreement with the experimental PAH concentration, only a minor impact of the afterburner treatment was observed for most species at 900 degrees C. OH was deduced to be the major reactant with a mole fraction about 4 orders of magnitudes higher than that of hydrogen radicals. Evidence for the need of further work on the quantitative assessment of oxidation of PAH and their radicals is given.
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PMID:Polynuclear aromatic hydrocarbon and particulate emissions from two-stage combustion of polystyrene: the effects of the secondary furnace (afterburner) temperature and soot filtration. 1187

Mucor circinelloides is being investigated as a possible host for the production of heterologous proteins. Thus, the environmental conditions defining the physiology and morphology of this dimorphic fungus have been investigated in submerged batch cultivation. The optimal conditions for growth of each form have been defined. Pure cultures of the multi-polar budding yeast form could be obtained under anaerobic conditions (with 70% N2/30% CO2 or 100% N2 as the sparge gas and without aeration). The highest maximum specific growth rate (0.30 h(-1)) was obtained in anaerobic cultivation, the yield of biomass on glucose (Y(SX)) was 0.12 (c-mole basis). A high maximum specific growth rate was obtained when the organism grew as the filamentous form under aerobic conditions (0.25 h(-1)), with a Y(SX) of 0.24 (c-mole basis). The maximum specific growth rates achieved are comparable to most industrial filamentous fungi under similar growth conditions. High levels of ethanol were observed with all growth conditions. The overriding effector of morphological development was found to be oxygen. In batch cultures it was therefore possible to induce the dimorphic shift by controlling the influent gas atmosphere. A specific growth rate of 0.19 h(-1) was maintained during the shift from the yeast to the filamentous form.
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PMID:Growth physiology and dimorphism of Mucor circinelloides (syn. racemosus) during submerged batch cultivation. 1195 97

A thermodynamic Gibbs energy minimization (GEM) solid solution-aqueous solution (SSAS) equilibrium model was used to determine the solubility of Zn from calcium silicate hydrate (CSH) phases doped with 0, 0.1, 1, 5, and 10% Zn at a unity (Ca+Zn)/Si molar ratio. Both the stoichiometry and standard molar Gibbs energy (G(o)298) of the Zn-bearing end-member in the ideal ternary Zn-bearing calcium silicate hydrate (CZSH) solid solution were determined by a "dual-thermodynamic" (GEM-DT) estimation technique. The SSAS model reproduces a complex sequence of reactions suggested to occur in a long-term weathering scenario of cementitious waste forms at subsurface repository conditions. The GEM model of CZSH leaching at several Zn loadings and solid/water (s/w) ratios in a C02-free system showed that, upon complete dissolution of portlandite and calcium zincate phases at decreasing s/w < 0.01 mol x kg(H2O)(-1), the total dissolved concentrations Si(aq), Ca(aq), and Zn(aq) are controlled by a CZSH solid solution of changing composition, with a trough-like Znaq drop by 2-3 orders of magnitude. Carbonation was simulated in another GEM model run series by CO2 titration of the system with initial s/w approximately 0.9 mol/kg(H2O). Formation of (Ca,Zn)-CO3 nonideal solid solution was predicted already at early reaction stage in the presence of both portlandite and calcium zincate hydrate phases. Upon their disappearance, pH, Zn(aq), C(aq), and fCO2 were predicted to change due to the incongruent dissolution of two concurrent CZSH-I and CZSH-II solid solutions, until the total re-partitioning of Ca and Zn into a carbonate solid solution coexisting with amorphous silica at fCO2 > 0.1 bar. Along this solid-phase transition, dissolved Zn(aq) concentrations follow a highly nonlinear trend. The model results predict that at low to moderate Zn loading (< or = 1% per mole Si), CZSH-type compounds can efficiently immobilize Zn in the near field of a cement-stabilized waste repository.
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PMID:Aqueous solubility diagrams for cementitious waste stabilization systems. 4. A carbonation model for Zn-doped calcium silicate hydrate by Gibbs energy minimization. 1214 69

Cuticular properties affect the gas exchange of leaves, but little is known about how much CO2 and water vapor cross the cuticular barrier or whether low water potentials affect the process. Therefore, we measured the cuticular conductances for CO2 and water vapor in grape (Vitis vinifera L.) leaves having various water potentials. The lower leaf surface was sealed to force all gas exchange through the upper surface, which was stoma-free. In this condition both gases passed through the cuticle, and the CO2 conductance could be directly determined from the internal mole fraction of CO2 near the compensation point, the external mole fraction of CO2, and the CO2 flux. The cuticle allowed small amounts of CO2 and water vapor to pass through, indicating that gas exchange occurs in grape leaves no matter how tightly the stomata are closed. However, the CO2 conductance was only 5.7% of that for water vapor. This discrimination against CO2 markedly affected calculations of the mole fraction of CO2 in leaves as stomatal apertures decreased. When the leaf dehydrated, the cuticular conductance to water vapor decreased, and transpiration and assimilation diminished. This dehydration effect was largest when turgor decreased, which suggests that cuticular gas exchange may have been influenced by epidermal stretching.
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PMID:CO2 and Water Vapor Exchange across Leaf Cuticle (Epidermis) at Various Water Potentials. 1222 98

It was previously shown with concurrent measurements of gas exchange and carbon isotope discrimination that the reduction of ribulose-1,5-bisphosphate carboxylase/oxygenase by an antisense gene construct in transgenic Flaveria bidentis (a C4 species) leads to reduced CO2 assimilation rates, increased bundle-sheath CO2 concentration, and leakiness (defined as the ratio of CO2 leakage to the rate of C4 acid decarboxylation; S. von Caemmerer, A. Millegate, G.D. Farquhar, R.T. Furbank [1997] Plant Physiol 113: 469-477). Increased leakiness in the transformants should result in an increased ATP requirement per mole of CO2 fixed and a change in the ATP-to-NADPH demand. To investigate this, we compared measurements of the quantum yield of photosystem I and II ([phi]PSI and [phi]PSII) with the quantum yield of CO2 fixation ([phi]CO2) in control and transgenic F. bidentis plants in various conditions. Both [phi]PSI/[phi]CO2 and [phi]PSII/[phi]CO2 increased with a decrease in ribulose-1,5-bisphosphate carboxylase/oxygenase content, confirming an increase in leakiness. In the wild type the ratio of [phi]PSI to [phi]PSII was constant at different irradiances but increased with irradiance in the transformants, suggesting that cyclic electron transport may be higher in the transformants. To evaluate the relative contribution of cyclic or linear electron transport to extra ATP generation, we developed a model that links leakiness, ATP/NADP requirements, and quantum yields. Despite some uncertainties in the light distribution between photosystem I and II, we conclude from the increase of [phi]PSII/[phi]CO2 in the transformants that cyclic electron transport is not solely responsible for ATP generation without NADPH production.
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PMID:Expressing an RbcS Antisense Gene in Transgenic Flaveria bidentis Leads to an Increased Quantum Requirement for CO2 Fixed in Photosystems I and II. 1222 65

A fast response, open path tunable diode laser absorption spectroscopy H2O/CO2 gas analyzer suitable for eddy correlation concentration measurements in near surface turbulent environments is presented. The turbulent temperature characteristics, analysis theory, analysis methods, design structure and specifications of this dual laser analyzer are described. A fiber connected optical head with folded optical path is used to extend the resolution to ppb levels for H2O at 1.3964 microm and CO2 at 2.014 microm. The Fourier (discrete cosine) transform absorbance ratio analysis methods are outlined along with the modifications for temperature and pressure measurements in turbulent flows. Synthesis of the reference absorbance function using measured temperature, pressure and the Hitran parameters is extended with incorporation of the Hitran parameters n, gamma temperature exponent and E'', lower state energy. Additionally, the mole fraction equation developed for this Hitran model is presented and an absolute calibration technique is outlined along with methods of calibration retention. Simulation results on mole fraction estimations and errors are presented for synthetic temperature and laser noise processes and are used to verify the specifications.
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PMID:An open path H2O/CO2 gas analyzer for eddy correlation systems: theory and design. 1235 86

Decomposition of trifluoroacetic acid (TFA) was achieved with a tungstic heteropolyacid photocatalyst H3PW12O40*6H2O in order to develop a technique for measures against TFA stationary sources. This is the first example of C-F bond cleavage in an environmentally harmful perfluoromethyl-group-containing compound using a homogeneous photocatalyst. The catalytic reaction proceeds in water at room temperature under UV-visible light irradiation in the presence of oxygen. The system produces only F- ions and CO2; the (mole of formed F-)/(mole of decomposed TFA) and (mole of formed CO2)/(mole of decomposed TFA) ratios were 2.91 and 2.09, respectively. GC/MS measurements showed no trace of other species such as environmentally undesirable CF4, which is the most stable perfluorocarbon and has a very high global warming potential. When the (initial TFA)/(initial catalyst) molar ratio was 20:1, the turnover number of TFA decomposition reached 5.58 by 72 h of irradiation, accompanying with no catalyst degradation. The catalytic reaction mechanism can be explained by a redox reaction between the catalyst and TFA, involving a photo-Kolbe process.
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PMID:Decomposition of environmentally persistent trifluoroacetic acid to fluoride ions by a homogeneous photocatalyst in water. 1256 17


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