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PubMed2003

Uptake and reduction of Cr(VI) to Cr(III) by mesquite (Prosopis spp.): chromate-plant interaction in hydroponics and solid media studied using XAS.

Chromium (Cr) is a well-established carcinogen that is a contaminant at half of the EPA Superfund sites in the United States. Two separate studies were performed to investigate the possibility that mesquite (Prosopis spp.), which is an indigenous desert plant species, can remove Cr from the environment via active transport systems to the aerial portions of the plant. The first study was performed by growing mesquite on solid media (agar) at Cr(VI) concentrations of 75 and 125 ppm. The accumulation found in the leaves under the present conditions indicated that mesquite could be classified as a hyperaccumulator of chromium. The second study was conducted to investigate the differences between the type of Cr ligand involved in Cr uptake with agar and hydroponic cultures. We used X-ray absorption spectroscopy (XAS) to determine the mechanisms involved in the uptake and binding of Cr(VI) in live mesquite tissue. The XAS results for this study showed that some of the supplied Cr(VI) was uptaken by the mesquite roots; however, the data analyses of the plant tissues demonstrated that it was fully reduced to Cr(III) in the leaf tissues. Experiments are currently being performed to evaluate the behavior of the Mesquite plant using lower Cr concentrations.

Biodegradation, Environmental↗
PubMed1997

Pentacyano(pyridine)chromate(III): Synthesis, Characterization, and Photochemistry.

The Cr(CN)(5)(py)(2)(-) anion (py = pyridine) has been prepared by acid-promoted methanolysis of Cr(CN)(6)(3)(-) followed by reaction with pyridine, isolated as the potassium salt, and characterized by absorption spectra (lambda(max): 403 and 256 nm in H(2)O; 411 nm in Me(2)SO) and phosphorescence, observed in Me(2)SO (lambda(max), 774 nm; tau = 56 &mgr;s at 20 degrees C) but not in H(2)O. In acid aqueous solution the complex decomposes stepwise to Cr(H(2)O)(5)(py)(3+); by contrast, the thermal reaction in Me(2)SO leads to Cr(CN)(5)(Me(2)SO)(2)(-) with first-order kinetics (k(25) = 9.8 x 10(-)(7) s(-)(1), DeltaH() = 138 +/- 8 kJ mol(-)(1)). Ligand-field (LF) band irradiation results in substitution of py and CN(-). The quantum yields, measured by ligand analysis, spectrophotometry, and HPLC, are as follows: Phi(py) = 0.08, Phi(CN) = 0.01 in H(2)O (pH 7.2, phosphate buffer) and Phi(py) = 0.04, Phi(CN) = 0.002 in Me(2)SO. The preference for py release obeys the prediction of the Vanquickenborne-Ceulemans, additive angular overlap model (AOM). A notable feature of this complex is that both types of ligands are pi acceptors, and the pi effect of py on bond labilization is evidenced by comparison with the photolysis of Cr(CN)(5)(NH(3))(2)(-). Irradiation of the intense UV absorption due to overlap of charge-transfer (CT) and pi --> pi, py localized transitions causes the increase of both quantum yields, suggesting the involvement of higher-energy states besides the LF ones. Co(sep)(3+) (sep = 1,3,6,8,10,13,16,19-octaazabicyclo[6.6.6]eicosane = sepulchrate) quenches the phosphorescence (k(q) = 1.6 x 10(9) M(-)(1) s(-)(1)) but has no effect on the photoreaction efficiencies: the photochemistry is thus inferred to originate entirely from the lowest quartet excited state(s) in competition with intersystem crossing. The marked solvent effects on the absorption spectrum, on the emission behavior, on the thermal reactivity, on the photolysis quantum yields, and, in particular, on the Phi(py)/Phi(CN) ratio, are discussed in terms of the proneness of the cyanide ligand to either protonation or hydrogen bonding and of solvent orientation toward anionic complexes.

Journal Article↗
PubMed2000

Bond valence sums in coordination chemistry. Calculation of the oxidation state of chromium in complexes containing only Cr-O bonds and a redetermination of the crystal structure of potassium tetra(peroxo)chromate(V).

A simple method for calculating the oxidation state of Cr in complexes containing only Cr-O bonds is presented. A total of 242 CrOn fragments with n = 3-6 were retrieved from the Cambridge Structural Database (CSD) and, together with the data for K3CrO8, were analyzed using the bond valence sum method. New R0 values for Cr(II) of 1.739(21) A, Cr(III) of 1.708(7) A, Cr(V) of 1.762(14) A, and Cr(VI) of 1.793(7) A were derived. An average R0 value of 1.724 A for Cr-O reproduces the oxidation state of 96 of the 110 Cr(II), Cr(III), and Cr(IV) CrOn complexes (n = 3-6) and that of K3CrO8 within 0.30 valence units. The crystal structure of K3CrO8 was redetermined at 173 K to provide accurate data for a Cr complex with both high oxidation state and coordination number. Potassium tetraperoxochromate(V), K3CrO8, is tetragonal, Space group I42m, a = b = 6.6940(3) A, c = 7.7536(5) A, Z = 2. The difficulties with fitting the observed valence for Cr(V) and Cr(VI) complexes with coordination numbers 4 and 5 are discussed. The use of bond valence sums in gaining chemical insight into Cr complexes with noninnocent ligands and in establishing oxidation states in Cr clusters is presented. An analysis of the Cr-O bond distances used in the calculations shows a large range of values that can be understood in terms of the bond valence sum calculation.

Journal Article↗
PubMed2005

Ligand adsorption on an activated carbon for the removal of chromate ions from aqueous solutions.

The results presented in this work are related to the design of a guideline to develop specific properties at the surface of an activated carbon (AC). For this, two model aromatic compounds have been synthesized and their electrolytic behavior in aqueous solutions was studied by a potentiometric method. The textural characteristics of the activated carbon were determined by porosimetry methods. The nature of oxygen-carrying functions and the acid-base behavior of the AC surface were characterized by TPD and potentiometric titration methods, respectively. The adsorption and desorption equilibria of the aromatic compounds on activated carbon were measured in aqueous solutions, and the hysteresis between adsorption and desorption, which reveals irreversible adsorption, was discussed on the basis of the frontier orbital theory. HOMO and LUMO orbitals of the adsorbent and adsorbates were calculated, and irreversible adsorption was attributed to the small energy difference between HOMO and LUMO of the aromatic adsorbates and the adsorbent. Adsorption equilibria of K2CrO4 in aqueous solution on the AC alone and on the AC-aromatic ligand adsorbents, respectively, prove the efficient development of specific chemical functions at the carbon surface provided by the adsorbed aromatic compounds.

Journal Article↗
PubMed2002

Cyclization of 1,6-enynes with allylic chromate species.

[reaction: see text] Treatment of 1,6-enynes with tetramethallylchromate induces a cyclization reaction with concurrent introduction of a methallyl group. A catalytic amount of CrCl(3) combined with methallylmagnesium chloride also achieves this cyclization process. The resultant cyclic organometallic species undergo further functionalization upon reaction with electrophiles.

Journal Article↗