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- Lindh, Linnea, et al.
(författare)
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Dye-sensitized solar cells based on Fe N-heterocyclic carbene photosensitizers with improved rod-like push-pull functionality
- 2021
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Ingår i: Chemical Science. - : Royal Society of Chemistry (RSC). - 2041-6520 .- 2041-6539. ; 12:48, s. 16035-16053
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Tidskriftsartikel (refereegranskat)abstract
- A new generation of octahedral iron(ii)-N-heterocyclic carbene (NHC) complexes, employing different tridentate C^N^C ligands, has been designed and synthesized as earth-abundant photosensitizers for dye sensitized solar cells (DSSCs) and related solar energy conversion applications. This work introduces a linearly aligned push-pull design principle that reaches from the ligand having nitrogen-based electron donors, over the Fe(ii) centre, to the ligand having an electron withdrawing carboxylic acid anchor group. A combination of spectroscopy, electrochemistry, and quantum chemical calculations demonstrate the improved molecular excited state properties in terms of a broader absorption spectrum compared to the reference complex, as well as directional charge-transfer displacement of the lowest excited state towards the semiconductor substrate in accordance with the push-pull design. Prototype DSSCs based on one of the new Fe NHC photosensitizers demonstrate a power conversion efficiency exceeding 1% already for a basic DSSC set-up using only the I−/I3−redox mediator and standard operating conditions, outcompeting the corresponding DSSC based on the homoleptic reference complex. Transient photovoltage measurements confirmed that adding the co-sensitizer chenodeoxycholic acid helped in improving the efficiency by increasing the electron lifetime in TiO2. Time-resolved spectroscopy revealed spectral signatures for successful ultrafast (<100 fs) interfacial electron injection from the heteroleptic dyes to TiO2. However, an ultrafast recombination process results in undesirable fast charge recombination from TiO2back to the oxidized dye, leaving only 5-10% of the initially excited dyes available to contribute to a current in the DSSC. On slower timescales, time-resolved spectroscopy also found that the recombination dynamics (longer than 40 μs) were significantly slower than the regeneration of the oxidized dye by the redox mediator (6-8 μs). Therefore it is the ultrafast recombination down to fs-timescales, between the oxidized dye and the injected electron, that remains as one of the main bottlenecks to be targeted for achieving further improved solar energy conversion efficiencies in future work.
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- Lindh, Linnea, et al.
(författare)
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Multifaceted Deactivation Dynamics of Fe(II) N-Heterocyclic Carbene Photosensitizers
- 2023
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Ingår i: Journal of Physical Chemistry A. - 1089-5639. ; 127:48, s. 10210-10222
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Tidskriftsartikel (refereegranskat)abstract
- Excited state dynamics of three iron(II) carbene complexes that serve as prototype Earth-abundant photosensitizers were investigated by ultrafast optical spectroscopy. Significant differences in the dynamics between the investigated complexes down to femtosecond time scales are used to characterize fundamental differences in the depopulation of triplet metal-to-ligand charge-transfer (3MLCT) excited states in the presence of energetically accessible triplet metal-centered (3MC) states. Novel insights into the full deactivation cascades of the investigated complexes include evidence of the need to revise the deactivation model for a prominent iron carbene prototype complex, a refined understanding of complex 3MC dynamics, and a quantitative discrimination between activated and barrierless deactivation steps along the 3MLCT → 3MC → 1GS path. Overall, the study provides an improved understanding of photophysical limitations and opportunities for the use of iron(II)-based photosensitizers in photochemical applications.
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- Lindh, Linnea, et al.
(författare)
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Side-group switching between metal-to-ligand charge-transfer and metal-centered excited state properties in iron(II) N-heterocyclic carbene complexes
- 2024
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Ingår i: Coordination Chemistry Reviews. - 0010-8545. ; 506
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Forskningsöversikt (refereegranskat)abstract
- Fe(II) N-heterocyclic carbene (NHC) complexes have emerged over the last decade as a promising class of light-harvesting complexes for a variety of photochemical applications relying on the presence of high-energy excited states of mainly charge-transfer character with excited state lifetimes of tens of picoseconds or longer. Recent spectroscopic investigations have significantly refined the understanding of some of the key prototype complexes of this kind and highlighted the subtle balance between population of triplet metal-to-ligand charge-transfer (3MLCT) and triplet metal-centered (3MC) states as a key issue to better understand and ultimately control the excited state dynamics in these complexes. To present a broader perspective on this issue, we here re-examine and discuss the excited state properties of a series of complexes with different side-groups on a common Fe NHC scaffold. Both the steady-state absorption spectrum and excited state dynamics are influenced by the side-group substitution, and the changes are rationalized based on shifting of the lowest metal-to-ligand charge-transfer (MLCT) state in energy based on the electron-withdrawing or electron-donating properties of the side-groups. Only electron-withdrawing substituents such as carboxylic acid groups ensured that the majority excited population stays in the 3MLCT state for ∼20 ps rather than rapidly converting into metal-centered (MC) states. In other complexes, the 3MLCT state survived <300 fs after which the 3MC state was populated for ∼10 ps. The transient absorption results also show that the dynamics can be switched in a simple manner by deprotonating the carboxylic acid group, which renders some of the complexes pH-sensitive. For the here discussed complexes, the results from transient absorption measurements indicate that the 3MLCT and 3MC states were close enough in energy to enable the side-group to determine the photophysics. The emerging understanding of the 3MLCT-3MC balance, as well as the nature and properties of the 3MC state in these complexes with intermediate ligand field strength is used to provide a broader fundamental perspective required to improve the ligand-design of Fe carbene complexes for issues such as to ensure a long-lived 3MLCT state.
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- Andreassen, Eva, et al.
(författare)
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Kokbok för förändringsledare : Metdoder för att stötta engagerade människor att förverkliga idéer
- 2020
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Bok (övrigt vetenskapligt/konstnärligt)abstract
- Det här är en kokbok för förändringsledare. Du kan använda denna bok om du ska leda utvecklingsaktiviteter och letar efter bra och beprövade metoder för att leda grupper och processer. Vi beskriver metoderna som vi har använt inom vårt projekt SMICE, i vilket sammanhang metoderna använts och när de olika metoderna fungerat bra. Vår förhoppning med att nedteckna dessa metoder är att du ska inspireras och vågar prova något nytt för att skapa nytta. Vi tror att ett detaljerat sätt att dokumentera metoderna gör dem mer användbara för dig men också för oss själva. Metoderna är graderade efter vilket behov av förkunskap och förberedelser du behöver, från det enklaste, där du kan öppna kokboken och använda metoden på en gång, till metoder som kräver utbildning eller specialistkompetens innan du sätter igång. Boken är indelad i fyra huvuddelar; Starta, Forma, Utveckla och förankra och Bygga vidare. Till dessa delar har vi identifierat metodstöd som kan användas vid en rad olika tillfällen; vid idégenerering, vid idéutveckling, vid affärsutveckling, för att inspirera, för att skapa samsyn och samverkan och för att mobilisera större grupper av människor och organisationer. Något för alla, alltså. Avslutningsvis finner du tips och stöd för att driva dessa utvecklingsprocesser på distans med digitala verktyg i digitala möten. Ska vi sammanfatta någon lärdom av detta arbete så blir det våra nycklar som presenteras på nästa sida. Du kan se dessa nycklar som våra bästa råd för att du ska lyckas med ditt arbete med att leda processer och att ordna möten. Lycka till! Metoderna har testats och utvecklats inom SMICE - Samskapande Mittnordisk Innovationsarena för Cirkulär Ekonomi, ett projekt inom Interreg som pågått 2017-2020.
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- Bergentall, Martina, et al.
(författare)
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Malolactic fermentation in lingonberry juice and its use as a preservative
- 2024
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Ingår i: Food microbiology (Print). - 0740-0020 .- 1095-9998. ; 121
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Tidskriftsartikel (refereegranskat)abstract
- Lingonberry is a common wild berry that is often sold as jams and beverages. It naturally contains high amounts of the weak acid preservative benzoic acid making it an interesting ingredient for shelf-life extension. Despite this, their use as a raw ingredient is limited by the inherently intense sour taste. This study aimed to improve the taste of lingonberry juice by subjecting it to malolactic fermentation in order to reduce the sourness, and to investigate the benzoic acid in lingonberries as a natural preservative in juice blends by determining the microbial stability. After initial screening of lactic acid bacteria, a Lactiplantibacillus plantarum strain was used as the starter for subsequent investigations. Upon raising the pH, all malic acid was completely converted to lactic acid after seven days. The fermented juice was mixed with blackcurrant juice in different proportions. Challenge tests of the blends showed Listeria monocytogenes could not grow in any juice samples, while Candida albicans only grew in the pure blackcurrant juice. Aspergillus brasiliensis growth was delayed in all samples containing benzoic acid in a concentration-dependent manner. The sourness and astringency were substantially reduced in the juice with added L. plantarum compared to the unfermented juice. © 2024 The Authors
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- Berggren Kleja, Dan, et al.
(författare)
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Bismuth(III) Forms Exceptionally Strong Complexes with Natural Organic Matter
- 2022
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 56, s. 3076-3084
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Tidskriftsartikel (refereegranskat)abstract
- The use of bismuth in the society has steadily increased during the last decades, both as a substitute for lead in hunting ammunition and various metallurgical applications, as well as in a range of consumer products. At the same time, the environmental behavior of bismuth is largely unknown. Here, the binding of bismuth(III) to organic soil material was investigated using extended X-ray absorption spectroscopy (EXAFS) and batch experiments. Moreover, the capacity of suwannee river fulvic acid (SRFA) to enhance the solubility of metallic bismuth was studied in a long-term (2 years) equilibration experiment. Bismuth(III) formed exceptionally strong complexes with the organic soil material, where >99% of the added bismuth(III) was bound by the solid phase, even at pH 1.2. EXAFS data suggest that bismuth(III) was bound to soil organic matter as a dimeric Bi3+ complex where one carboxylate bridges two Bi3+ ions, resulting in a unique structural stability. The strong binding to natural organic matter was verified for SRFA, dissolving 16.5 mmol Bi per gram carbon, which largely exceeds the carboxylic acid group density of this compound. Our study shows that bismuth(III) will most likely be associated with natural organic matter in soils, sediments, and waters.
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- Bose, Aneesh, et al.
(författare)
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Pharmaceutical pollution disrupts the behaviour and predator–prey interactions of two widespread aquatic insects
- 2022
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Ingår i: iScience. - : Elsevier BV. - 2589-0042. ; 25
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Tidskriftsartikel (refereegranskat)abstract
- Pharmaceutical pollution represents a rapidly growing threat to ecosystems worldwide. Drugs are now commonly detected in the tissues of wildlife and have the potential to alter the natural expression of behavior, though relatively little is known about how pharmaceuticals impact predator-prey interactions. We conducted parallel laboratory experiments using larval odonates (dragonfly and damselfly nymphs) to investigate the effects of exposure to two pharmaceuticals, cetirizine and citalopram, and their mixture on the outcomes of predator-prey interactions. We found that exposure to both compounds elevated dragonfly activity and impacted their predation success and efficiency in complex ways. While exposure to citalopram reduced predation efficiency, exposure to cetirizine showed varied effects, with predation success being enhanced in some contexts but impaired in others. Our findings underscore the importance of evaluating pharmaceutical effects under multiple contexts and indicate that these compounds can affect predator-prey outcomes at sublethal concentrations.
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- Buck, Dietrich, 1990-, et al.
(författare)
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Impregnation of Wood / End Grain Treatment
- 2021
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Konferensbidrag (övrigt vetenskapligt/konstnärligt)abstract
- This research presents the findings of a study conducted by Luleå University of Technology (LTU) and Lund University (LTH) on the effect of edge treatment on the end grain of cross-laminated timber (CLT) elements. The objective of the study was to identify whether edge treatment influences the moisture performance and mould risk of CLT.The investigation was conducted through controlled laboratory studies, utilising standardised procedures. Specifically, the end grain of the CLT specimens was exposed to moisture by placing them in contact with a free water surface for 96 hours. Following this exposure, the specimens were dried under controlled conditions. X-ray computed tomography (CT) scanning was used to estimate the moisture content of the specimens and provide detailed spatial information about the moisture distribution within the wood.To further evaluate the effectiveness of edge treatment, the experimental moisture content assessments were compared to values by WUFI simulations. Additionally, annual data for the simulations were conducted using climate data from three different locations: Lund, Stockholm, and Borlänge. These simulations assessed the theoretical impact of edge treatment on mould risk under different climatic conditions.Results revealed that edge treatment has potential to reduce moisture content and mitigate mould risk in CLT elements. Experimentally assessed moisture content values were consistently lower in edge-treated specimens compared to untreated specimens. The calculations and simulations supported these findings, showing a distinct reduction in moisture accumulation and mould risk in edge-treated CLT elements.This study provides insights into the effect of edge treatment on the moisture performance and mould risk in CLT elements. The findings suggest that implementing appropriate edge treatment techniques can enhance the durability of CLT structures, particularly for worksites in regions where climatic conditions fluctuate over the course of construction. Further research and testing are warranted to explore additional factors influencing the effectiveness of edge treatment in CLT applications.
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