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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.

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.

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.

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 aggravating global problems of energy crisis, rising atmospheric greenhouse gas concentrations and accumulation of persistent waste have attracted the attention of scientists, policy-makers and global organisations to come up with effective and expeditious solutions to address these challenges. In this context, the development of sustainable technologies driven by renewable energy sources for the production of clean fuels and commodity chemicals from diverse waste feedstocks is an appealing approach towards creating a circular economy. Over the years, semiconductor photocatalysts based on TiO₂, CdS, carbon-nitrides (CNx) and carbon dots (CDs) have been widely used for the photocatalytic reforming (PC reforming) of pre-treated waste substrates to organic products, accompanied with clean hydrogen (H₂) generation. However, these conventional solar-driven processes suffer from major drawbacks such as low production rates, poor product selectivity, CO₂ release, challenging process and catalyst optimisation, and harsh waste pre-treatment conditions, which limit their commercial applicability. These challenges are tackled in this thesis with the introduction of new and efficient photoelectrochemical (PEC) and chemoenzymatic processes for reforming a diverse range of waste feedstocks to sustainable fuels. Solar-driven PEC reforming based on halide perovskite light-absorber is first developed as an attractive alternative to PC reforming. The PEC systems consist of a perovskite|Pt photocathode for clean H₂ production and a Cu-Pd alloy anode for reforming diverse waste streams, including pre-treated cellulosic biomass, polyethylene terephthalate (PET) plastics, and industrial by-product glycerol into industrially-relevant, value-added chemicals (gluconic acid, glycolic acid and glyceric acid) without any externally applied bias or voltage. Additionally, the single light-absorber PEC systems can also convert the airborne waste stream and greenhouse gas CO₂ to diverse products with the simultaneous reforming of PET plastics with no applied voltage. The perovskite-based photocathode enables the integration of different CO₂ reduction catalysts such as a molecular cobalt porphyrin, a Cu-In alloy and formate dehydrogenase enzyme, which produce CO, syngas and formate, respectively. The versatile PEC systems, which can be assembled in either a ‘two-compartment’ or standalone ‘artificial leaf’ configurations achieve 60‒90% oxidation product selectivity (with no over-oxidation) and >100 µmol cm‾² h‾¹ product formation rates, corresponding to 10²‒10⁴ times higher activity than conventional PC reforming systems. In addition to developing PEC platforms, this thesis also explores avenues for circumventing the harsh alkaline pre-treatment strategies (pH >13, 60‒80 ºC) adopted for photoreforming waste substrates. For this purpose, a chemoenzymatic pathway is introduced whereby PET and polycaprolactone plastics were deconstructed using functional enzymes under benign conditions (pH 6‒8, 37‒65 ºC), followed by PC reforming using Pt loaded TiO₂ (TiO₂|Pt) or Ni₂P loaded carbon-nitride (CNx|Ni₂P) photocatalysts. The chemoenzymatic reforming process demonstrates versatility in upcycling polyester films and nanoplastics for H₂ production at high yields reaching ∼10³‒10⁴ µmol gsub‾¹ and activities at >500 µmol gcat‾¹ h‾¹. The utilisation of enzyme pre-treated plastics also allowed the coupling of plastic reforming with photocatalytic CO₂-to-syngas conversion using a phosphonated cobalt bis(terpyridine) co-catalyst immobilised on TiO₂ (TiO₂|CotpyP). Finally, moving beyond solar-driven systems, a bio-electrocatalytic flow process is demonstrated for the conversion of microbe pre-treated food waste to ethylene (an important feedstock in the chemical industry) on graphitic carbon electrodes via succinic acid as the central intermediate. In conclusion, with its focus on improving efficiencies, achieving selective product formation, building versatile platforms, diversifying substrate and product scope, and reducing carbon footprint and economic strain, this thesis aims to bring sustainable waste-to-fuel technologies a step closer to commercial implementation.

The aggravating global problems of energy crisis, rising atmospheric greenhouse gas concentrations and accumulation of persistent waste have attracted the attention of scientists, policy-makers and global organisations to come up with effective and expeditious solutions to address these challenges. In this context, the development of sustainable technologies driven by renewable energy sources for the production of clean fuels and commodity chemicals from diverse waste feedstocks is an appealing approach towards creating a circular economy. Over the years, semiconductor photocatalysts based on TiO₂, CdS, carbon-nitrides (CNx) and carbon dots (CDs) have been widely used for the photocatalytic reforming (PC reforming) of pre-treated waste substrates to organic products, accompanied with clean hydrogen (H₂) generation. However, these conventional solar-driven processes suffer from major drawbacks such as low production rates, poor product selectivity, CO₂ release, challenging process and catalyst optimisation, and harsh waste pre-treatment conditions, which limit their commercial applicability. These challenges are tackled in this thesis with the introduction of new and efficient photoelectrochemical (PEC) and chemoenzymatic processes for reforming a diverse range of waste feedstocks to sustainable fuels. Solar-driven PEC reforming based on halide perovskite light-absorber is first developed as an attractive alternative to PC reforming. The PEC systems consist of a perovskite|Pt photocathode for clean H₂ production and a Cu-Pd alloy anode for reforming diverse waste streams, including pre-treated cellulosic biomass, polyethylene terephthalate (PET) plastics, and industrial by-product glycerol into industrially-relevant, value-added chemicals (gluconic acid, glycolic acid and glyceric acid) without any externally applied bias or voltage. Additionally, the single light-absorber PEC systems can also convert the airborne waste stream and greenhouse gas CO₂ to diverse products with the simultaneous reforming of PET plastics with no applied voltage. The perovskite-based photocathode enables the integration of different CO₂ reduction catalysts such as a molecular cobalt porphyrin, a Cu-In alloy and formate dehydrogenase enzyme, which produce CO, syngas and formate, respectively. The versatile PEC systems, which can be assembled in either a ‘two-compartment’ or standalone ‘artificial leaf’ configurations achieve 60‒90% oxidation product selectivity (with no over-oxidation) and >100 µmol cm‾² h‾¹ product formation rates, corresponding to 10²‒10⁴ times higher activity than conventional PC reforming systems. In addition to developing PEC platforms, this thesis also explores avenues for circumventing the harsh alkaline pre-treatment strategies (pH >13, 60‒80 ºC) adopted for photoreforming waste substrates. For this purpose, a chemoenzymatic pathway is introduced whereby PET and polycaprolactone plastics were deconstructed using functional enzymes under benign conditions (pH 6‒8, 37‒65 ºC), followed by PC reforming using Pt loaded TiO₂ (TiO₂|Pt) or Ni₂P loaded carbon-nitride (CNx|Ni₂P) photocatalysts. The chemoenzymatic reforming process demonstrates versatility in upcycling polyester films and nanoplastics for H₂ production at high yields reaching ∼10³‒10⁴ µmol gsub‾¹ and activities at >500 µmol gcat‾¹ h‾¹. The utilisation of enzyme pre-treated plastics also allowed the coupling of plastic reforming with photocatalytic CO₂-to-syngas conversion using a phosphonated cobalt bis(terpyridine) co-catalyst immobilised on TiO₂ (TiO₂|CotpyP). Finally, moving beyond solar-driven systems, a bio-electrocatalytic flow process is demonstrated for the conversion of microbe pre-treated food waste to ethylene (an important feedstock in the chemical industry) on graphitic carbon electrodes via succinic acid as the central intermediate. In conclusion, with its focus on improving efficiencies, achieving selective product formation, building versatile platforms, diversifying substrate and product scope, and reducing carbon footprint and economic strain, this thesis aims to bring sustainable waste-to-fuel technologies a step closer to commercial implementation.

National net zero emission targets could, if fully implemented, reduce best estimates of projected global average temperature increase to 2.0–2.4 °C by 2100, bringing the Paris Agreement temperature goal within reach. A total of 131 countries are discussing, have announced or have adopted net zero targets, covering 72% of global emissions. These targets could substantially lower projected warming as compared to currently implemented policies (2.9–3.2 °C) or pledges submitted to the Paris Agreement (2.4–2.9 °C). Current pledges for emissions cuts are insufficient to meet the Paris Agreement temperature goal. The wave of net zero targets being discussed and adopted could make the Paris goal possible if further countries follow suit.

National net zero emission targets could, if fully implemented, reduce best estimates of projected global average temperature increase to 2.0–2.4 °C by 2100, bringing the Paris Agreement temperature goal within reach. A total of 131 countries are discussing, have announced or have adopted net zero targets, covering 72% of global emissions. These targets could substantially lower projected warming as compared to currently implemented policies (2.9–3.2 °C) or pledges submitted to the Paris Agreement (2.4–2.9 °C). Current pledges for emissions cuts are insufficient to meet the Paris Agreement temperature goal. The wave of net zero targets being discussed and adopted could make the Paris goal possible if further countries follow suit.