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Engineered cementitious composites (ECCs) are special types of fibre-reinforced cementitious composites (FRCC) with higher strain capacity which can be achieved with low fibre volume as low as 2% and total elimination of coarse aggregates. Due to the outstanding performance of ECCs, they are suitable for various construction and repair applications. However, in order for ECCs to achieve their properties; a high amount of binder which is primarily composed of Portland cement (PC) is used alongside a special type of ultrafine silica sand (USS) which is different from the conventional natural fine aggregates. The production of PC is known to be detrimental to the environment due to its high carbon dioxide emissions coupled with the high consumption of natural resources. Thus, the high use of PC content in ECCs posed a sustainability threat. Similarly, the USS used in ECCs are not readily available everywhere and are expensive. The processing of the USS coupled with its transportation over long distances would also increase the cost and embodied carbon of ECCs. Hence, in order to promote more development and applications of ECCs for various applications; this dissertation aims to provide innovative ways to improve the sustainability of ECCs and their performances. This dissertation offers four solutions to improve the sustainability of ECCs which are (i) use of unconventional industrial by-products as partial replacement of PC (ii) total replacement of PC in ECCs with alternative sustainable binders (iii) replacement of USS in ECCs with recycled materials and (iv) the use of supplementary cementitious materials to replace a high volume of PC. The findings from this study revealed sustainable ECCs with acceptable mechanical and durability performance can be achieved with the use of alternative binders or replacement of the conventional USS used in ECC mixtures. The sustainability and cost assessment of the ECCs indicated that the incorporation of industrial by-products such as blast furnace slag (BFS) especially at higher content is beneficial to reducing the negative environmental impact and economic burden associated with ECCs compared to the conventional ECC. The sustainability index and cost index of the ECCs further showed that the use of BFS is more beneficial when the sustainability and cost of the ECCs are compared with the corresponding performance. Similarly, the use of recycled materials as an alternative to USS was found to result in a significant reduction in the embodied carbon and cost of ECCs. The use of recycled materials such as expanded glass (EG) as aggregates in ECCs was also found to improve the thermal insulation properties of ECCs making such ECC suitable for the production of building envelope elements.

In industrialized countries, large amounts of mineral wastes are produced. They are re-used in various ways, particularly in road and earth constructions, substituting primary resources such as gravel. However, they may also contain pollutants, such as heavy metals, which may be leached to the groundwater. The toxic impacts of these emissions are so far often neglected within Life Cycle Assessments (LCA) of products or waste treatment services and thus, potentially large environmental impacts are currently missed. This study aims at closing this gap by assessing the ecotoxic impacts of heavy metal leaching from industrial mineral wastes in road and earth constructions. The flows of metals such as Sb, As, Pb, Cd, Cr, Cu, Mo, Ni, V and Zn originating from three typical constructions to the environment are quantified, their fate in the environment is assessed and potential ecotoxic effects evaluated. For our reference country, Germany, the industrial wastes that are applied as Granular Secondary Construction Material (GSCM) carry more than 45,000 t of diverse heavy metals per year. Depending on the material quality and construction type applied, up to 150 t of heavy metals may leach to the environment within the first 100 years after construction. Heavy metal retardation in subsoil can potentially reduce the fate to groundwater by up to 100%. One major challenge of integrating leaching from constructions into macro-scale LCA frameworks is the high variability in micro-scale technical and geographical factors, such as material qualities, construction types and soil types. In our work, we consider a broad range of parameter values in the modeling of leaching and fate. This allows distinguishing between the impacts of various road constructions, as well as sites with different soil properties. The findings of this study promote the quantitative consideration of environmental impacts of long-term leaching in Life Cycle Assessment, complementing site-specific risk assessment, for the design of waste management strategies, particularly in the construction sector.

Organic solar cells utilize an energy-level offset to generate free charge carriers. Although a very small energy-level offset increases the open-circuit voltage, it remains unclear how exactly charge generation is affected. Here we investigate organic solar cell blends with highest occupied molecular orbital energy-level offsets (∆EHOMO) between the donor and acceptor that range from 0 to 300 meV. We demonstrate that exciton quenching at a negligible ∆EHOMO takes place on timescales that approach the exciton lifetime of the pristine materials, which drastically limits the external quantum efficiency. We quantitatively describe this finding via the Boltzmann stationary-state equilibrium between charge-transfer states and excitons and further reveal a long exciton lifetime to be decisive in maintaining an efficient charge generation at a negligible ∆EHOMO. Moreover, the Boltzmann equilibrium quantitatively describes the major reduction in non-radiative voltage losses at a very small ∆EHOMO. Ultimately, highly luminescent near-infrared emitters with very long exciton lifetimes are suggested to enable highly efficient organic solar cells. Donor–acceptor systems with low energy-level offset enable high power efficiency in organic solar cells yet it is unclear what drives charge generation. Classen et al. show that long exciton lifetimes enable efficient exciton splitting and thus generation of free charges while also suppressing voltage losses.

An important limitation of polymer electrolyte fuel cell technology is the low mechanical strength and dimensional instability with changes of water content of proton exchange membranes (PEMs). A range of different approaches to more stable PEMs based on Nafion have been studied of which composite materials of Nafion with mechanically stronger polymers is one of the most promising directions. If successful, they will lead to thinner composite PEMs with enhanced fuel cell performance, life span, and cost-effectiveness. Developed in this thesis are electrospinning conditions for the fabrication of electrospun mats for potential application in PEMs. Polysulfone (PSU), poly vinylidene fluoride-co-hexafluoropropylene (PVDF-HFP), and polyvinylidene fluoride (PVDF) were tested as mechanically stronger but inert (minimal contribution to proton transport) polymers that can tolerate the fuel cell condition. PVDF-HFP generated defect free electrospun mats over a wide range of spinning conditions, while PSU required very specific conditions and no successful conditions were found for PVDF mostly due to over-wetting. These mats might function as mechanical support and could be tested as PEMs when filled with Nafion, but the complete filling of electrospun mats with Nafion has been proven difficult. Instead, the electrospinning of Nafion was tested to explore options of electrospinning mixed mats of two different polymers and co-electrospinning of core-sheath fibers. Two commercial Nafion solutions D520 and D2020 with 5 wt% and 20 wt% content of Nafion were electrospun together with polyethylene oxide of two different molecular weights as a carrier polymer. Mats of sufficient quality for PEM tests were obtained with solutions based on 20 wt% content of Nafion, a low flow rate of 0.2 mL/h, and the lower molecular weight polyethylene oxide as the carrier. Finally, coaxial electrospinning conditions for the formation of core-sheath fibers were developed for Nafion as sheath material and PVDF-HFP or PSU as the core material. Defect-free, core-sheath fibers were generated when the concentration of both solutions was high (20 wt%), the Nafion flow rate was about 0.2 mL/h for the sheath, and the core flow rate was below the flow rate of the sheath (0.1-0.15 mL/h for PVDF-HFP and 0.15 mL/h for PSU). Mats of these core-sheath fibers should provide good mechanical strength combined with much better compatibility with Nafion. A straightforward pore filling with Nafion solutions is expected and their investigation as PEMs in fuel cells is planned as future work.

Abstract As main contributors to greenhouse gas emissions, power and transportation are crucial sectors for energy system decarbonization. Their interaction is expected to increase significantly: plug-in electric vehicles add a new electric load, increasing grid demand and potentially requiring substantial grid upgrade; hydrogen production for fuel cell electric vehicles or for clean fuels synthesis could exploit the projected massive power overgeneration by intermittent and seasonally-dependent renewable sources via Power-to-Hydrogen. This work investigates the infrastructural needs involved with a broad diffusion of clean mobility, adopting a sector integration perspective at the national scale. The analysis combines a multi-node energy system balance simulation and a techno-economic assessment of the infrastructure to deliver energy vectors for mobility. The article explores the long-term case of Italy, considering a massive increase of renewable power generation capacity and investigating different mobility scenarios, where low-emission vehicles account for 50% of the stock. First, the model solves the energy balances, integrating the consumption related to mobility energy vectors and taking into account power grid constraints. Then, an optimal infrastructure is identified, composed of both a hydrogen delivery network and a widespread installation of charging points. Results show that the infrastructural requirements bring about investment costs in the range of 43–63 G€. Lower specific costs are associated with the exclusive presence of FCEVs, whereas the full reliance on BEVs leads to the most significant costs. Scenarios that combine FCEVs and BEVs lie in between, suggesting that the overall power + mobility system benefits from the presence of both drivetrain options.

The optical and photovoltaic properties of Si NCs / SiC multilayers (MLs) are investigated using a membrane-based solar cell structure. By removing the Si substrate in the active cell area, the MLs are studied without any bulk Si substrate contribution. The occurrence is confirmed by scanning electron microscopy and light-beam induced current mapping . Optical characterization combined with simulations allows us to determine the absorption within the ML absorber layer, isolated from the other cell stack layers. The results indicate that the absorption at wavelengths longer than 800 nm is only due to the SiC matrix. The measured short-circuit current is significantly lower than that theoretically obtained from absorption within the ML absorber, which is ascribed to losses that limit carrier extraction. The origin of these losses is discussed in terms of the material regions where recombination takes place. Our results indicate that carrier extraction is most efficient from the Si NCs themselves, whereas recombination is strongest in SiC and residual a-Si domains . Together with the observed onset of the external quantum efficiency (EQE) at 700-800 nm, this fact is an evidence of quantum confinement in Si NCs embedded in SiC on device level.

Abstract Latest trends in the photovoltaic sector see the use of innovative photovoltaic technologies with extended spectral responsivity ranging from 300 to 1200 nm for non-concentrating terrestrial applications, and to 1800 nm for concentrating PV and space applications. As a consequence, an update of the IEC 60904-9 standard is ongoing with a definition of new spectral ranges for the assessment of the spectral match. This poses new challenges to laboratories and research centers on whether or not they still are able to accurately measure the spectral mismatch of their sun simulator in the newly-defined spectral regions. Prior to that, there is a need to understand if the commercially available spectroradiometers are ready to extend their measurement range as prescribed by the forthcoming new standard. This paper analyses two options for an extension of the spectrum characterisation of solar simulators to 300–1200 nm and compares them in terms of spectral match of global normal irradiance (GNI) spectra acquired under natural sunlight by eight spectroradiometers during the 6th European Spectroradiometer Intercomparison. The acquired spectra are also compared in terms of an index of consistency of the spread of the measured spectra with the estimated measurement uncertainty, hereafter named as performance statistics E n . Results show that all investigated laboratories assure the equivalence of the spectral match classification well below the 25% limit corresponding to class-A simulators. When considering the more stringent class-A+ corresponding to a 12.5% limit, one of the two considered options that rearranges the 300–1200 nm spectral range into 6 bands appears to still assure the equivalence of the class A+ limits among considered instruments. The E n performance index analysis highlights some inconsistencies with the estimated measurement uncertainty or instrument drifts from the expected performance, and the need of further improvements in calibration, set up and measurement procedures.