Periodic Reporting for period 4 - SCOPE (Surface-COnfined fast-modulated Plasma for process and Energy intensification in small molecules conversion)
Reporting period: 2023-10-01 to 2025-03-31
Catalysing the transformation to a more sustainable and innovative society requires the development of innovative technologies in chemical and energy transformation/utilisation areas that use directly renewable energy to substitute fossil fuels. It is necessary to develop novel technologies for producing chemicals, fuels and chemical energy storage vectors that allow overcoming the current limitations in renewable energy production to realise this vision.
The SCOPE proposal aims to develop the scientific basis for a ground-breaking approach (based on catalysis-plasma symbiosis) for direct chemical syntheses using the renewable energy of large-volume key chemicals or energy vectors. Although the project's core is plasma-catalysis, the project is extended to a comparative analysis of photo- and electrocatalysis to better understand how to design effective "reactive" catalysts, e.g. the catalysis trio (electro, photo and plasma catalysis), which uses renewable energy rather than thermal energy (from fossil fuels). This catalysis trio shares several technological and fundamental aspects, besides the possibilities to integrate photo and electrocatalysis in plasma processes, another project objective. Thus, we aim to put the scientific basis for this new catalytic chemistry at the core of the energy and chemistry transition.
We have three target reactions: (i) N2 fixation, a key reaction for the production of ammonia (NH3) and NOx-made fertilisers; (ii) CH4 valorisation to produce longer C-chain hydrocarbons; (iii) CO2 conversion to liquid solar fuels.
The SCOPE proposal aims to develop the scientific basis for a ground-breaking approach (based on catalysis-plasma symbiosis) for direct chemical syntheses using the renewable energy of large-volume key chemicals or energy vectors. Although the project's core is plasma-catalysis, the project is extended to a comparative analysis of photo- and electrocatalysis to better understand how to design effective "reactive" catalysts, e.g. the catalysis trio (electro, photo and plasma catalysis), which uses renewable energy rather than thermal energy (from fossil fuels). This catalysis trio shares several technological and fundamental aspects, besides the possibilities to integrate photo and electrocatalysis in plasma processes, another project objective. Thus, we aim to put the scientific basis for this new catalytic chemistry at the core of the energy and chemistry transition.
We have three target reactions: (i) N2 fixation, a key reaction for the production of ammonia (NH3) and NOx-made fertilisers; (ii) CH4 valorisation to produce longer C-chain hydrocarbons; (iii) CO2 conversion to liquid solar fuels.
The SCOPE project started in April 2019, and after an amendment, the end was shifted to March 2026. The situation is now back to normal after delays from the pandemic and related impacts on recruitment, mobility, and meetings. The general project organisation is the following:
- UniME (cPI) is developed the novel catalysts/electrodes, as well as comparative testing with photo- and electrocatalytic conversion, besides the development of novel reactor concepts for plasma-catalysis,
- UANT (PI1) developed physicochemical models of plasma-catalysis systems and did experiments on different modalities of plasma generation and interaction with the catalyst
- UNIWAR (PI2, I3), and associated TUe and UoA, developed a novel two-jet reactor concept, developed plasma-enzyme catalysis, characterised the plasma bubble reactor fundamentally and explored it for two applications (air N-fixation, urine recovery), as well as assessed the sustainability of diverse plasma processes (TEA, LCA, Circularity, ESG).
The project is organised into six work packages (WPs), all active in the fourth RP. The active WPs were WP1 (Identify the mechanisms of controlling the selectivity), WP2 (Surface-confined plasma ), WP3 (Fast-modulated operations in the presence of plasma), WP4 (Advanced processes for direct conversion of target small molecules) and WP5 (Intensified process-sustainability opportunities), in addition to WP6 (Coordination and Dissemination).
The scientific work performed up to the fourth RP aligns with the planned activities. Within the project, 155 publications (all with an indication of project support and green/gold open access) and over 200 dissemination activities (lectures and other relevant events) were realised. PIS also made many additional publications on closely related aspects.
Only online meetings were held during the pandemic, but later, a series of physical meetings between PIs and related teams was organized and will continue. As part of the dissemination, various international conferences and workshops were also organized as part of the SCOPE activities. Mobility of the PhD students and researchers' exchange was also implemented.
An important action regards the realisation of a joint international Doctorate ( ACCESS - Advanced Catalytic Processes for using Renewable Energy Sources), stemming directly from the ERC Synergy SCOPE. The Doctorate is now in the 5th cycle, and it has transformed into an Industrial Doctorate (supported by various companies). Various PhD students spend mobility periods in other PIs' labs. Also, various PhD students work in co-tutelle between PIs. Two ERC PoCs projects, and another at submission stage, resulted from the SCOPE project.
- UniME (cPI) is developed the novel catalysts/electrodes, as well as comparative testing with photo- and electrocatalytic conversion, besides the development of novel reactor concepts for plasma-catalysis,
- UANT (PI1) developed physicochemical models of plasma-catalysis systems and did experiments on different modalities of plasma generation and interaction with the catalyst
- UNIWAR (PI2, I3), and associated TUe and UoA, developed a novel two-jet reactor concept, developed plasma-enzyme catalysis, characterised the plasma bubble reactor fundamentally and explored it for two applications (air N-fixation, urine recovery), as well as assessed the sustainability of diverse plasma processes (TEA, LCA, Circularity, ESG).
The project is organised into six work packages (WPs), all active in the fourth RP. The active WPs were WP1 (Identify the mechanisms of controlling the selectivity), WP2 (Surface-confined plasma ), WP3 (Fast-modulated operations in the presence of plasma), WP4 (Advanced processes for direct conversion of target small molecules) and WP5 (Intensified process-sustainability opportunities), in addition to WP6 (Coordination and Dissemination).
The scientific work performed up to the fourth RP aligns with the planned activities. Within the project, 155 publications (all with an indication of project support and green/gold open access) and over 200 dissemination activities (lectures and other relevant events) were realised. PIS also made many additional publications on closely related aspects.
Only online meetings were held during the pandemic, but later, a series of physical meetings between PIs and related teams was organized and will continue. As part of the dissemination, various international conferences and workshops were also organized as part of the SCOPE activities. Mobility of the PhD students and researchers' exchange was also implemented.
An important action regards the realisation of a joint international Doctorate ( ACCESS - Advanced Catalytic Processes for using Renewable Energy Sources), stemming directly from the ERC Synergy SCOPE. The Doctorate is now in the 5th cycle, and it has transformed into an Industrial Doctorate (supported by various companies). Various PhD students spend mobility periods in other PIs' labs. Also, various PhD students work in co-tutelle between PIs. Two ERC PoCs projects, and another at submission stage, resulted from the SCOPE project.
The following progress beyond the state of the art can be mentioned:
CPI/UniME:
- A new concept of a DBD planar plasma reactor equipped with a quartz window for catalyst illumination to explore potential synergies between light and plasma in the catalytic non-oxidative coupling of methane (NOCM) reaction.
- Analysis of the effects of assisting plasma conversion with light irradiation, design of materials for this objective.
- Novel improved technology for N2 conversion to NH3 in plasma-electrocatalytic conditions, benchmarking of the results to electrocatalytic solution and HB technology.
- Development of controlled synthesis of nanoporous carbon layers with modulated surface morphology for surface-confined plasma
- photocatalytic NOCM process in a novel type of flow-through photoreactor with very high C2 productivity using a Pd-based photocatalyst
- a porous stainless steel (PSS) tube as the internal electrode in a coaxial tubular DBD reactor
- a framework analysis of the role of direct electrification technologies (plasma-, photo- and electro-catalysis) for future sustainable and low-carbon energy and chemical productiono
PI1/UANT:
- Development of plasma chemical kinetics models and comparison with thermal kinetics
- Development of the first fully coupled model of gas flow dynamics, plasma physics and chemistry for predicting imporved plasma reactor designs
- Improved DFT simulations for plasma-catalytic CO2 hydrogenation
- Experiments on dry reforming of methane, and how oxygen or water vapor addition can enhance oxygenates formation, avoid soot deposition and increase the syngas ratio
- Experiments on plasma-based conversion of Martian atmosphere (mainly CO2) into life-sustaining chemicals, for in-situ resource utilization
- Significant improvements in plasma-based CO2 conversion, by post-plasma quenching and post-plasma carbon bed
- Novel insights in upscaling of plasma-based CO2 conversion and N2 fixation, by two different methods: placing several reactos in parallel, and enlarging the reactor size
- Detailed techno-economic and cost analysis, and life-cycle assessments of plasma-based CO2 conversion, together with I3
PI2/UNIWAR, TUe and I3/UNIWAR, UoA:
- Novel method for detecting plasma species using tunable diode laser absorption spectroscopy (TDLAS)
- Novel plasma reactors: single-jet stagnant layer reactor, two-jet convective flow reactor
- Plasma-enzyme catalysis: urease in plasma bubble reactor for urine decomposition
- Biomass cell proliferation by jet microplasma for extraction of nutrients (bioactives)
- NH3 and NOx formation in single-jet stagnant layer reactor, NH3 and NOx formation in two-jet convective flow reactor, NH3 and NOx formation in plasma bubble reactor, urine decomposition (for N fixation) in plasma bubble reactor
- Fundamental electrical & chemical-engineering assessment of the plasma microbubble gas-liquid system.
- Techno-economic and life-cycle assessment of plasma-based CO2 conversion, together with I3
- Environmental, Social and Governance (ESG) on distributed plasma-ammonia plants
CPI/UniME:
- A new concept of a DBD planar plasma reactor equipped with a quartz window for catalyst illumination to explore potential synergies between light and plasma in the catalytic non-oxidative coupling of methane (NOCM) reaction.
- Analysis of the effects of assisting plasma conversion with light irradiation, design of materials for this objective.
- Novel improved technology for N2 conversion to NH3 in plasma-electrocatalytic conditions, benchmarking of the results to electrocatalytic solution and HB technology.
- Development of controlled synthesis of nanoporous carbon layers with modulated surface morphology for surface-confined plasma
- photocatalytic NOCM process in a novel type of flow-through photoreactor with very high C2 productivity using a Pd-based photocatalyst
- a porous stainless steel (PSS) tube as the internal electrode in a coaxial tubular DBD reactor
- a framework analysis of the role of direct electrification technologies (plasma-, photo- and electro-catalysis) for future sustainable and low-carbon energy and chemical productiono
PI1/UANT:
- Development of plasma chemical kinetics models and comparison with thermal kinetics
- Development of the first fully coupled model of gas flow dynamics, plasma physics and chemistry for predicting imporved plasma reactor designs
- Improved DFT simulations for plasma-catalytic CO2 hydrogenation
- Experiments on dry reforming of methane, and how oxygen or water vapor addition can enhance oxygenates formation, avoid soot deposition and increase the syngas ratio
- Experiments on plasma-based conversion of Martian atmosphere (mainly CO2) into life-sustaining chemicals, for in-situ resource utilization
- Significant improvements in plasma-based CO2 conversion, by post-plasma quenching and post-plasma carbon bed
- Novel insights in upscaling of plasma-based CO2 conversion and N2 fixation, by two different methods: placing several reactos in parallel, and enlarging the reactor size
- Detailed techno-economic and cost analysis, and life-cycle assessments of plasma-based CO2 conversion, together with I3
PI2/UNIWAR, TUe and I3/UNIWAR, UoA:
- Novel method for detecting plasma species using tunable diode laser absorption spectroscopy (TDLAS)
- Novel plasma reactors: single-jet stagnant layer reactor, two-jet convective flow reactor
- Plasma-enzyme catalysis: urease in plasma bubble reactor for urine decomposition
- Biomass cell proliferation by jet microplasma for extraction of nutrients (bioactives)
- NH3 and NOx formation in single-jet stagnant layer reactor, NH3 and NOx formation in two-jet convective flow reactor, NH3 and NOx formation in plasma bubble reactor, urine decomposition (for N fixation) in plasma bubble reactor
- Fundamental electrical & chemical-engineering assessment of the plasma microbubble gas-liquid system.
- Techno-economic and life-cycle assessment of plasma-based CO2 conversion, together with I3
- Environmental, Social and Governance (ESG) on distributed plasma-ammonia plants