Electrochemical characterization of biodeterioration of paint films containing cadmium yellow pigment

[EN] The voltammetry of microparticles (VMP) methodology was used to characterize the biological attack of different bacteria and fungi to reconstructed egg tempera and egg linseed oil emulsion paint films containing cadmium yellow (CdS), which mimic historical painting techniques. When these paint films are in contact with aqueous acetate buffer, different cathodic signals are observed. As a result of the crossing of VMP data with attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR), scanning electrochemical microscopy (SECM), field emission scanning electron microscopy (FESEM), and atomic force microscopy (AFM), these voltammetric signals can be associated with the reduction of CdS and different complexes associated to the proteinaceous and fatty acid fractions of the binders. After biological attack with different fungi (Acremonium chrysogenum, Aspergillus niger, Mucor rouxii, Penicillium chrysogenum, and Trichoderma pseudokoningii) and bacteria (Arthrobacter oxydans, Bacillus amyloliquefaciens, and Streptomyces cellulofans), the observed electrochemical signals experience specific modifications depending on the binder and the biological agent, allowing for an electrochemical monitoring of biological attack.Financial support from the MINECO Projects CTQ2014-53736-C3-1-P and CTQ2014-53736-C3-2-P which are supported with ERDF funds is gratefully acknowledged. The authors also wish to thank Dr. José Luis Moya López, Mr. Manuel Planes Insausti, and Mrs. Alicia Nuez Inbernón (Microscopy Service of the Universitat Politècnica de València) for technical support.Ortiz-Miranda, A.; Domenech Carbo, A.; Domenech Carbo, MT.; Osete Cortina, L.; Valle-Algarra, FM.; Bolivar Galiano, F.; Martin Sanchez, I.... (2016). Electrochemical characterization of biodeterioration of paint films containing cadmium yellow pigment. Journal of Solid State Electrochemistry. 20(12):3287-3302. https://doi.org/10.1007/s10008-016-3349-6S328733022012Ratledge C (1994) Biochemistry of microbial degradation. Springer, BerlinCaneva G, Nugari MP, Salvadori O (2008) Plant biology for cultural heritage, the Getty Conservation Institute, Los AngelesSterflinger K (2010) Fungi: their role in deterioration of cultural heritage. Fungal Biol Rev 47–55 and references thereinGargani G (1968) Fungus contamination of Florence art masterpieces before and after the 1966 disaster. In: Walters AH, Elphick JJ (eds) Biodeterioration of materials. Elsevier, Amsterdam, pp. 252–257Seves AM, Sora S, Ciferr O (1996) The microbial colonization of oil paintings—a laboratory investigation. Int Biodeter Biodegr. 37:215–224Tiano P (2002) Biodegradation of cultural heritage: decay mechanisms and control methods. University of LisbonStrzelczyk AB (2004) Observations on aesthetic and structural changes induced in polish historic objects by microorganisms. Int Biodeter Biodegr. 53:151–156López-Miras M, Piñar G, Romero-Noguera J, Bolivar-Galiano FC, Ettenauer J, Sterflinger K, Martín-Sánchez I (2013) Microbial communities adhering to the obverse and reverse sides of an oil painting on canvas: identification and evaluation of their biodegradative potential. Aerobiologia 29:301–314Koszewski A, Rymuza Z, Reuther F (2008) Evaluation of nanomechanical, nanotribological and adhesive properties of ultrathin polymer resist film by AFM. Micro Engn 85:1189–1192Schabereiter-Gurtner C, Piñar G, Lubitz W, Rölleke S (2001) An advanced molecular strategy to identify bacterial communities on art objects. J Microbiol Meth 45:77–87Florian MLE (1996) The role of the conidia of fungi in fox spots. Stud Conserv 41:65–75Arai H, Matsui N, Matsumura N, Murakita H (1988) Biochemical investigations on the formation mechanisms of foxing. Stud Conserv 33:11–12Arai H, Matsumura N, Murakita H (1990) Microbiological studies on the conservation of paper and related cultural properties: part 9, induction of artificial foxing. Science for Conservation 29:25–34Hayashi T, Namili M (1986) Role of sugar fragmentation in early stage browning of amino-carbonyl reaction of sugars with amino acids. Agr Biol Chem Tokyo 50:1965–1970Allsopp D, Seal KJ, Gaylarde CC (2004) Introduction to biodeterioration, 2 edn. Cambridge University Press, CambridgeBock E, Sand W (1993) The microbiology of masonry biodeterioration. J Appl Bacteriol 74:503–514Ciferri O (2002) The role of microorganisms in the degradation of cultural heritage. Rev Conserv 3:35–45Van der Snickt G, Dik J, Cotte M, Janssens K, Jaroszewicz J, De Wolf W, Groenewegen J, Van der Loeff L (2009) Characterization of a degraded cadmium yellow (CdS) pigment in an oil painting by means of synchrotron radiation based X-ray techniques. Anal Chem 81:2600–2610Child AM (1995) Microbial taphonomy of archaeological bone. Stud Conserv 40:19–30Soliman NA, Knoll M, Abdel-Fattah YR, Schmid RD, Lange S (2007) Molecular cloning and characterization of thermostable esterase and lipase from Geobacillus thermoleovorans YN isolated from desert soil in Egypt. Process Biochem 42(2007):1090–1100Kinderlerer JL (1994) Degradation of the lauric acid oils. Int Biodeter Biodegr 33(1994):345–354van den Berg JDJ, van den Berg KJ, Boon JJ (2002) Identification of non-cross-linked compounds in methanolic extracts of cured and aged linseed oil-based paint films using gas chromatography-mass spectrometry. J Chromatogr A 950:195–211 and references thereinLefèvre M (1974) La ‘maladie verte’ de Lascaux. Stud Conserv 19:126–156Petushkova JP, Lyalikova NN (1986) Microbiological degradation of lead-containing pigments in mural paintings. Stud Conserv 31:65–69Breitbach AM, Rocha JC, Gaylarde CC (2011) Influence of pigment on biodeterioration of acrylic paint films in southern Brazil. J Coat Technol Res 8:619–628Keune K, van Loon A, Boon JJ (2011) SEM backscattered-electron images of paint cross sections as information source for the presence of the lead white pigment and lead-related degradation and migration phenomena in oil paintings. Microsc Microanal 17:696–701Meilunas RJ, Bentsen JG, Steinberg A (1990) Analysis of aged paint binders by FTIR spectroscopy. Stud Conserv 35:33–51Mazzeo R, Prati S, Quaranta M, Joseph E, Kendix E, Galeotti M (2008) Attenuated total reflection micro FTIR characterization of pigment–binder interaction in reconstructed paint films. Anal Bioanal Chem 392:65–76Salvadó N, Butí S, Nicholson J, Emerich H, Labrador A, Pradell T (2009) Identification of reaction compounds in micrometric layers from gothic paintings using combined SR-XRD and SR-FTIR. Talanta 79:419–428Scholz F, Meyer B (1998) Voltammetry of solid microparticles immobilized on electrode surfaces. Electroanal Chem 20:1–86Scholz F, Schröder U, Gulabowski R, Doménech-Carbó A (2014) Electrochemistry of immobilized particles and Dropletst, 2 edn. Springer, Berlin-HeidelbergDoménech-Carbó A, Labuda J, Scholz F (2013) Electroanalytical chemistry for the analysis of solids: characterization and classification (IUPAC technical report). Pure Appl Chem 85:609–631Doménech-Carbó A, Doménech-Carbó MT, Costa V (2009) Electrochemical methods for Archaeometry, conservation and restoration (monographs in electrochemistry series Scholz F edit). Springer, Berlin-HeidelbergDoménech-Carbó A (2010) Electrochemistry for conservation science. J Solid State Electr 14:349–351Matteini M, Moles A (1989) La Chimica nel Restauro. Nardini, FirenzeGettens RJ, Stout GL (1966) Painting materials. A short encyclopedia. Dover Publications, New YorkCennini C (1982) Il libro dell’ arte. Akal, MadridCepriá G, García-Gareta E, Pérez-Arantegui J (2005) Cadmium yellow detection and quantification by voltammetry of immobilized microparticles. Electroanalysis 17:1078–1084Domínguez I, Doménech-Carbó A, Cerisuelo JP, López-Carballo G, Henández-Muñoz P, Gavara R (2014) Contact probe electrochemical characterization and metal speciation of silver LLDPE nanocomposite films. J Solid State Electrochem 18:2099–2110Byler DM, Susi H (1986) Examination of the secondary structure of proteins by deconvolved FTIR spectra. Biopolymers 25:469–487Chang CM, Powrie WD, Fennema O (1977) Microstructure of egg yolk. J Food Sci 42:1193–1200Prestrelski SJ, Tedeschi N, Arakawa T, Carpenter JF (1993) Dehydration-induced conformational transitions in proteins and their inhibition by stabilizers. Biophys J 65:661–671Boehm S, Abaturov LV (1977) Structural changes of met-haemoglobin by dehydration. FEBS Lett 77:21–24Karpowicz A (1981) Ageing and deterioration of proteinaceous media. Stud Conserv 26:153–160Koper A, Grabarczyk M (2012) Simultaneous voltammetric determination of trace bismuth(III) and cadmium(II) in water samples by adsorptive stripping voltammetry in the presence of cupferron. J Electroanal Chem 681:1–5Zakharchuk N, Meyer S, Lange B, Scholz F (2000) A comparative study of lead oxide modified graphite paste electrodes and solid graphite electrodes with mechanically immobilized lead oxides. Croat Chem Acta 73:667–704Komorsky-Lovric S, Lovric M, Bond AM (1992) Comparison of the square-wave stripping voltammetry of lead and mercury following their electrochemical or abrasive deposition onto a paraffin impregnated graphite electrode. Anal Chim Acta 258:299–305Arjmand F, Adriaens A (2012) Electrochemical quantification of copper-based alloys using voltammetry of microparticles: optimization of the experimental conditions. J Solid State Electrochem 16:535–543Meyer B, Ziemer B, Scholz F (1995) In situ X-ray diffraction study of the electrochemical reduction of tetragonal lead oxide and orthorhombic Pb(OH)Cl mechanically immobilized on a graphite electrode. J Electroanal Chem 392:79–83Hasse U, Scholz F (2001) In situ atomic force microscopy of the reduction of lead oxide nanocrystals immobilised on an electrode surface. Electrochem Commun 3:429–434Doménech-Carbó A, Doménech-Carbó MT, Mas-Barberá X (2007) Identification of lead pigments in nanosamples from ancient paintings and polychromed sculptures using voltammetry of nanoparticles/atomic force microscopy. Talanta 71:1569–1579Eissler RL, Princen RH (1972) The interface between reactive pigment and binder matrix. J Electroanal Chem 37:327–336Kuznetsov AM, Ulstrup J (1989) Protein dynamics and electronic fluctuation effects in electron transfer reactions of membrane-bound proteins and metalloprotein complexes. J Electroanal Chem 275:289–305Colletti LP, Teklay D, Stickney JL (1994) Thin-layer electrochemical studies of the oxidative underpotential deposition of sulfur and its application to the electrochemical atomic layer epitaxy deposition of CdS. J Electroanal Chem 369:145–152Gulaboski R, Mirceski V, Bogeski I, Hoth M (2012) Protein film voltammetry: electrochemical enzymatic spectroscopy. A review on recent progress. J Solid State Electrochem 16:2315–2328Guidelli R, Becucci L (2011) Ion transport across biomembranes and model membranes. J Solid State Electrochem 15:1459–1470Sutherland K (2003) Solvent-extractable components of linseed oil paint films. Stud Conserv 48:111–135Rossi M, Alamprese C, Ratti S (2007) Tocopherols and tocotrienols as free radical-scavengers in refined vegetable oils and their stability during deep-fat frying. Food Chem 102:812–817Ziyatdinova G, Morozov M, Budnikov H (2012) MWNT-modified electrodes for voltammetric determination of lipophilic vitamins. J Solid State Electrochem 16:2441–2447Madani A, Nessark B, Boukherroub R, Chehimi MM (2011) Preparation and electrochemical behaviour of PPy–CdS composite films. J Electroanal Chem 650:176–181Derrick MR, Stulik DC, Landry MJ (1999) Infrared spectroscopy in conservation science. Getty Conservation Institute, Los Angelesvan der Weerd J, van Loon A, Boon JJ (2005) FTIR studies of the effects of pigments on the aging of oil. Stud Conserv 50:3–22Kong J, Yu S (2007) Fourier transform infrared spectroscopic analysis of protein secondary structures. Acta Bioch Bioph Sin 39:549–559Haris PI, Severcan F (1999) FTIR spectroscopic characterization of protein structure in aqueous and non-aqueous media. J Mol Catal B-Enzym 7:207–221Furlan PY, Scott SA, Peaslee MH (2007) FTIR-ATR study of pH effects on egg albumin secondary structure. Spectrosc Lett 40:475–482Dong A, Huang P, Caughey WS (1990) Protein secondary structures in water from second-derivative amide I infrared spectra. Biochemistry-US 29:3303–3308Rajkhowa R, Hu X, Tsuzuki T, Kaplan DL, Wang X (2012) Structure and biodegradation mechanism of milled B. mori silk particles. Biomacromolecules 13:2503–2512Anton M (2013) Egg yolk: structures, functionalities and processes. J Sci Food Agr 93:2871–2880Hevonoja T, Pentikäinen MO, Hyvönen MT, Kovanen PT, Ala-Korpela M (2000) Structure of low density lipoprotein (LDL) particles: basis for understanding molecular changes in modified LDL. Biochim Biophys Acta 1488:189–210Kumpula LS, Kumpula JM, Taskinen MR, Jauhiainen M, Kaski K, Ala-Korpela M (2008) Reconsideration of hydrophobic lipid distributions in lipoprotein particles. Chem Phys Lipids 155:57–62 and references thereinSchneider H, Morrod RS, Colvin JR, Tattrie NH (1973) The lipid core model of lipoproteins. Chem Phys Lipids 10:328–353Doménech-Carbó MT, Osete-Cortina L, de la Cruz-Cañizares J, Bolívar-Galiano F, Romero-Noguera J, Martín-Sánchez I, Fernández-Vivas MA (2006) Study of the microbiodegradation of terpenoid resin-based varnishes from easel painting using pirolisis-gas chromatography-mass spectrometry and gas chromatography-mass spectrometry. Anal Bioanal Chem 385:1265–128

Outcomes and prognostic factors of adults with refractory or relapsed T-cell acute lymphoblastic leukemia included in measurable residual disease-oriented trials

Despite high complete remission (CR) rates with frontline therapy, relapses are frequent in adults with T-cell acute lymphoblastic leukemia (T-ALL) with limited salvage options. We analyzed the outcomes and prognostic factors for CR to salvage therapy and overall survival (OS) of patients with R/R T-ALL included in two prospective measurable residual disease-oriented trials. Seventy-five patients (70 relapsed, 5 refractory) were identified. Relapses occurred in bone marrow, isolated or combined in 50 patients, and in the central nervous system (CNS; isolated or combined) in 20. Second CR was attained in 30/75 patients (40%). Treatment with FLAG-Ida and isolated CNS relapse were independently associated with a higher CR rate after first salvage therapy. The median OS was 6.2 (95% confidence interval [CI], 3.9–8.6) months, with a 4-year OS probability of 18% (95% CI, 9%–27%). No differences in survival were observed according to the treatment with hematopoietic stem cell transplantation in patients in CR after first salvage therapy. Multivariable analysis showed a ≥12-month interval between first CR and relapse, CR after first salvage therapy and isolated CNS relapse as favorable prognostic factors for OS with hazard ratios (HR) (95% CI) of 1.931 (1.109–3.362), 2.958 (1.640–5.334), and 2.976 (1.157–7.655), respectively. This study confirms the poor outcomes of adults with R/R T-ALL among whom FLAG-Ida was the best of the rescue therapies evaluated. Late relapse, CR after first rescue therapy and isolated CNS relapse showed prognostic impact on survival. More effective rescue therapies are needed in adults with R/R T-ALL.La Caixa" Foundation and ISCIII, Grant/ Award Number: PI19/01828; Generalitat de Catalunya (GRC), Grant/Award Number: 2017 SGR28

Field observations of volatile organic compound (VOC) exchange in red oaks

Volatile organic compounds (VOCs) emitted by forests strongly affect the chemical composition of the atmosphere. While the emission of isoprenoids has been largely characterized, forests also exchange many oxygenated VOCs (oVOCs), including methanol, acetone, methyl ethyl ketone (MEK), and acetaldehyde, which are less well understood. We monitored total branch-level exchange of VOCs of a strong isoprene emitter (Quercus rubra L.) in a mixed forest in New England, where canopy-level fluxes of VOCs had been previously measured. We report daily exchange of several oVOCs and investigated unknown sources and sinks, finding several novel insights. In particular, we found that emission of MEK is linked to uptake of methyl vinyl ketone (MVK), a product of isoprene oxidation. The link was confirmed by corollary experiments proving in vivo detoxification of MVK, which is harmful to plants. Comparison of MEK, MVK, and isoprene fluxes provided an indirect indication of within-plant isoprene oxidation. Furthermore, besides confirming bidirectional exchange of acetaldehyde, we also report for the first time direct evidence of benzaldehyde bidirectional exchange in forest plants. Net emission or deposition of benzaldehyde was found in different periods of measurements, indicating an unknown foliar sink that may influence atmospheric concentrations. Other VOCs, including methanol, acetone, and monoterpenes, showed clear daily emission trends but no deposition. Measured VOC emission and deposition rates were generally consistent with their ecosystem-scale flux measurements at a nearby sit