Listen
10 Ergebnisse
Ergebnisse nach Hochschule und Institut
Publikation Organic photovoltaics: Potential fate and effects in the environment(Elsevier, 2012) Zimmermann, Yannick-Serge; Schäffer, Andreas; Hugi, Christoph; Fent, Karl; Corvini, Philippe; Lenz, MarkusIn times of dwindling fossil fuels it is particularly crucial to develop novel “green” technologies in order to cover the increasing worldwide demand for energy. Organic photovoltaic solar cells (OPVs) are promising as a renewable energy source due to low energy requirement for production, low resource extraction, and no emission of greenhouse gasses during use. In contrast to silicium-based solar cells, OPVs offer the advantages of light-weight, semi-transparency and mechanical flexibility. As to a possible forthcoming large-scale production, the environmental impact of such OPVs should be assessed and compared to currently best available technologies. For the first time, this review compiles the existing knowledge and identifies gaps regarding the environmental impact of such OPVs in a systematic manner. In this regard, we discuss the components of a typical OPV layer by layer. We discuss the probability of enhanced release of OPV-borne components into the environment during use-phase (e.g. UV- and biodegradation) and end-of-life phase (e.g. incineration and waste disposal). For this purpose, we compiled available data on bioavailability, bioaccumulation, biodegradation, and ecotoxicity. Whereas considerable research has already been carried out concerning the ecotoxicity of certain OPV components (e.g. nanoparticles and fullerenes), others have not been investigated at all so far. In conclusion, there is a general lack of information about fate, behavior as well as potential ecotoxicity of most of the main OPV components and their degradation/transformation products. So far, there is no evidence for a worrying threat coming from OPVs, but since at present, no policy and procedures regarding recycling of OPVs are in action, in particular improper disposal upon end-of-life might result in an adverse effect of OPVs in the environment when applied in large-scale.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Organic solvent free PbI2 recycling from perovskite solar cells using hot water(Elsevier, 05.04.2023) Schmidt, Felix; Amrein, Meret; Hedwig, Sebastian; Kober-Czerny, Manuel; Paracchino, Adriana; Holappa, Ville; Suhonen, Riikka; Schäffer, Andreas; Constable, Edwin C.; Snaith, Henry J.; Lenz, MarkusPerovskite solar cells represent an emerging and highly promising renewable energy technology. However, the most efficient perovskite solar cells critically depend on the use of lead. This represents a possible environmental concern potentially limiting the technologies’ commercialization. Here, we demonstrate a facile recycling process for PbI2, the most common lead-based precursor in perovskite absorber material. The process uses only hot water to effectively extract lead from synthetic precursor mixes, plastic- and glass-based perovskites (92.6 – 100% efficiency after two extractions). When the hot extractant is cooled, crystalline PbI2 in high purity (> 95.9%) precipitated with a high yield: from glass-based perovskites, the first cycle of extraction / precipitation was sufficient to recover 94.4 ± 5.6% of Pb, whereas a second cycle yielded another 10.0 ± 5.2% Pb, making the recovery quantitative. The solid extraction residue remaining is consequently deprived of metals and may thus be disposed as non-hazardous waste. Therefore, exploiting the highly temperature-dependent solubility of PbI2 in water provides a straightforward, easy to implement way to efficiently extract lead from PSC at the end-of-life and deposit the extraction residues in a cost-effective manner, mitigating the potential risk of lead leaching at the perovskites’ end-of-life.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Environmental selenium volatilization is possibly conferred by promiscuous reactions of the sulfur metabolism(Elsevier, 2023) Liu, Ying; Schäffer, Andreas; Martinez, Mathieu; Lenz, MarkusSelenium deficiency affects many million people worldwide and volatilization of biogenically methylated selenium species to the atmosphere may limit Se entering the food chain. However, there is very little systematic data on volatilization at nanomolar concentrations prevalent in pristine natural environments. Pseudomonas tolaasii cultures efficiently methylated Se at these concentrations. Nearly perfect linear correlations between the spiked Se concentrations and Dimethylselenide, Dimethyldiselenide, Dimethylselenylsulfide and 2-hydroxy-3-(methylselanyl)propanoic acid were observed up to 80 nM. The efficiency of methylation increased linearly with increasing initial Se concentration, arguing that the enzymes involved are not constitutive, but methylation proceeds promiscuously via pathways of S methylation. From the ratio of all methylated Se and S species, one can conclude that between 0.30% and 3.48% of atoms were Se promiscuously methylated at such low concentrations. At concentrations higher than 640 nM (∼50 μg/L) a steep increase in methylation and volatilization was observed, which suggested the induction of specific enzymes. Promiscuous methylation at low environmental concentrations calls into question that view that methylated Se in the atmosphere is a result of a purposeful Se metabolism serving detoxification. Rather, the concentrations of methylated Se in the atmosphere may be “coincidental” i.e., determined by the activity of S cycling microorganisms. Further, a steep increase in methylation efficiency when surpassing a certain threshold concentration (here ∼50 μg/L) calls into question that natural methylation can be estimated from high Se spikes in laboratory systems, yet highlights the possibility of using bacterial methylation as an effective remediation strategy for media higher concentrated in Se. © 2023 The Authors01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Rapid sequestration of perovskite solar cell-derived lead in soil(Elsevier, 08/2022) Schmidt, Felix; Ledermann, Luca; Schäffer, Andreas; Snaith, Henry J.; Lenz, MarkusEfficient and stable perovskite solar cells rely on the use of Pb species potentially challenging the technologies’ commercialisation. In this study, the fate of Pb derived from two common perovskite precursors is compared to cationic lead in soil-water microcosm experiments under various biogeochemical conditions. The rapid and efficient removal of Pb from the aqueous phase is demonstrated by inductively coupled plasma mass spectrometry. Sequential soil extraction results reveal that a substantial amount of Pb is associated with immobile fractions, whereas a minor proportion of Pb may become available again in the long term, when oxygen is depleted (e.g. during water logging). X-ray absorption spectroscopy results reveal that the sorption of Pb on mineral phases represents the most likely sequestration mechanism. The obtained results suggest that the availability of leached Pb from perovskite solar cells is naturally limited in soils and that its adverse effects on soil biota are possibly negligible in oxic soils. All three Pb sources used behaved very similar in the experiments, wherefore we conclude that perovskite derived Pb will have a similar fate compared to cationic Pb, so that established risk assessment considerations for Pb remain legitimate.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Sulfur amino acid status controls selenium methylation in pseudomonas tolaasii. Identification of a novel metabolite from promiscuous enzyme reactions(American Society for Microbiology, 26.05.2021) Liu, Ying; Hedwig, Sebastian; Schäffer, Andreas; Lenz, Markus; Martinez, MathieuSelenium (Se) deficiency affects many millions of people worldwide, and the volatilization of methylated Se species to the atmosphere may prevent Se from entering the food chain. Despite the extent of Se deficiency, little is known about fluxes in volatile Se species and their temporal and spatial variation in the environment, giving rise to uncertainty in atmospheric transport models. To systematically determine fluxes, one can rely on laboratory microcosm experiments to quantify Se volatilization in different conditions. Here, it is demonstrated that the sulfur (S) status of bacteria crucially determines the amount of Se volatilized. Solid-phase microextraction gas chromatography mass spectrometry showed that Pseudomonas tolaasii efficiently and rapidly (92% in 18 h) volatilized Se to dimethyl diselenide and dimethyl selenyl sulfide through promiscuous enzymatic reactions with the S metabolism. However, when the cells were supplemented with cystine (but not methionine), a major proportion of the Se (∼48%) was channeled to thus-far-unknown, nonvolatile Se compounds at the expense of the previously formed dimethyl diselenide and dimethyl selenyl sulfide (accounting for <4% of total Se). Ion chromatography and solid-phase extraction were used to isolate unknowns, and electrospray ionization ion trap mass spectrometry, electrospray ionization quadrupole time-of-flight mass spectrometry, and microprobe nuclear magnetic resonance spectrometry were used to identify the major unknown as a novel Se metabolite, 2-hydroxy-3-(methylselanyl)propanoic acid. Environmental S concentrations often exceed Se concentrations by orders of magnitude. This suggests that in fact S status may be a major control of selenium fluxes to the atmosphere. IMPORTANCE Volatilization from soil to the atmosphere is a major driver for Se deficiency. “Bottom-up” models for atmospheric Se transport are based on laboratory experiments quantifying volatile Se compounds. The high Se and low S concentrations in such studies poorly represent the environment. Here, we show that S amino acid status has in fact a decisive effect on the production of volatile Se species in Pseudomonas tolaasii. When the strain was supplemented with S amino acids, a major proportion of the Se was channeled to thus-far-unknown, nonvolatile Se compounds at the expense of volatile compounds. This hierarchical control of the microbial S amino acid status on Se cycling has been thus far neglected. Understanding these interactions—if they occur in the environment—will help to improve atmospheric Se models and thus predict drivers of Se deficiency.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Redox-stat bioreactors for elucidating mobilisation mechanisms of trace elements: An example of As-contaminated mining soils(Springer, 2018) Rajpert, Liwia; Schäffer, Andreas; Lenz, MarkusThe environmental fate of major (e.g. C, N, S, Fe and Mn) and trace (e.g. As, Cr, Sb, Se and U) elements is governed by microbially catalysed reduction-oxidation (redox) reactions. Mesocosms are routinely used to elucidate trace metal fate on the basis of correlations between biogeochemical proxies such as dissolved element concentrations, trace element speciation and dissolved organic matter. However, several redox processes may proceed simultaneously in natural soils and sediments (particularly, reductive Mn and Fe dissolution and metal/metalloid reduction), having a contrasting effect on element mobility. Here, a novel redox-stat (Rcont) bioreactor allowed precise control of the redox potential (159 ± 11 mV, ~ 2 months), suppressing redox reactions thermodynamically favoured at lower redox potential (i.e. reductive mobilisation of Fe and As). For a historically contaminated mining soil, As release could be attributed to desorption of arsenite [As(III)] and Mn reductive dissolution. By contrast, the control bioreactor (Rnat, with naturally developing redox potential) showed almost double As release (337 vs. 181 μg g−1) due to reductive dissolution of Fe (1363 μg g−1 Fe2+ released; no Fe2+ detected in Rcont) and microbial arsenate [As(V)] reduction (189 μg g−1 released vs. 46 μg g−1 As(III) in Rcont). A redox-stat bioreactor thus represents a versatile tool to study processes underlying mobilisation and sequestration of other trace elements as well.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Production of superparamagnetic nanobiocatalysts for green chemistry applications(Springer, 23.04.2016) Gasser, Christoph; Ammann, Erik; Schäffer, Andreas; Shahgaldian, Patrick; Corvini, PhilippeImmobilization of enzymes on solid supports is a convenient method for increasing enzymatic stability and enabling enzyme reuse. In the present work, a sorption-assisted surface conjugation method was developed and optimized to immobilize enzymes on the surface of superparamagnetic nanoparticles. An oxidative enzyme, i.e., laccase from Trametes versicolor was used as model enzyme. The immobilization method consists of the production of superparamagnetic nanoparticles by co-precipitation of FeCl2 and FeCl3. Subsequently, the particle surface is modified with an organosilane containing an amino group. Next, the enzymes are adsorbed on the particle surface before a cross-linking agent, i.e., glutaraldehyde is added which links the amino groups on the particle surface with the amino groups of the enzymes and leads to internal cross-linking of the enzymes as well. The method was optimized using response surface methodology regarding optimal enzyme and glutaraldehyde amounts, pH, and reaction times. Results allowed formulation of biocatalysts having high specific enzymatic activity and improved stability. The biocatalysts showed considerably higher stability compared with the dissolved enzymes over a pH range from 3 to 9 and in the presence of several chemical denaturants. To demonstrate the reusability of the immobilized enzymes, they were applied as catalysts for the production of a phenoxazinone dye. Virtually, 100 % of the precursor was transformed to the dye in each of the ten conducted reaction cycles while on average 84.5 % of the enzymatic activity present at the beginning of a reaction cycle was retained after each cycle highlighting the considerable potential of superparamagnetic biocatalysts for application in industrial processes.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Degradation of sulfonamide antibiotics by Microbacterium sp. strain BR1 - elucidating the downstream pathway(Elsevier, 2015) Ricken, Benjamin; Fellmann, Oliver; Kohler, Hans-Peter E.; Schäffer, Andreas; Corvini, Philippe; Kolvenbach, Boris01A - Beitrag in wissenschaftlicher ZeitschriftPublikation New insights into biological sulfonamide degradation(2015) Kolvenbach, Boris; Ricken, Benjamin; Fellmann, Oliver; Kohler, Hans-Peter E.; Schäffer, Andreas; Corvini, Philippe06 - PräsentationPublikation Insights into the sulfonamide degrading protein complex(2015) Ricken, Benjamin; Bucher, Andreas; Mariossi, Andrea; Fellmann, Oliver; Adaixo, Ricardo; Schäffer, Andreas; Corvini, Philippe; Kolvenbach, Boris; Kohler, Hans-Peter E.; Leu, Cedric06 - Präsentation