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CORDIS - Résultats de la recherche de l’UE

Surface-COnfined fast-modulated Plasma for process and Energy intensification in small molecules conversion

Periodic Reporting for period 3 - SCOPE (Surface-COnfined fast-modulated Plasma for process and Energy intensification in small molecules conversion)

Période du rapport: 2022-04-01 au 2023-09-30

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 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 impact 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) studied the physicochemical modelling of plasma-catalysis systems and did experiments on different modalities of plasma generation and interaction with the catalyst
- at UNIWAR (PI2, I3), and associated TUe and UoA, is investigated the reactor optimisation and simulation, including the development of a novel approach for spatiotemporal characterisation of concentration profiles in plasma catalysis and the sustainability-driven assessment of the processes, including distributed manufacturing scenarios
The project is organised into six work packages (WPs), all active in the third 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 third RP aligns with the planned activities. Over 100 publications (all with an indication of project support and green/gold open access) and over 100 dissemination activities (lectures and other relevant events) were realised within the project. Many additional publications were also made by PIs on closely related aspects.

Only online meetings were made during the pandemic, but in 2022, physical meetings between PIs and related teams started again. A meeting was held in Warwick in Sept. 2022, combined with the UCRA2022 international meeting organised as part of the SCOPE activities. A second project meeting was in Antwerp in Sept. 2023. Mobility of the PhD students also started in 2022.

Important actions regarding the implementation of synergy is the realisation of two joint international Doctorates:
- the first is the Doctorate ACCESS (Advanced Catalytic Processes for using Renewable Energy Sources), stemming directly from the ERC Synergy SCOPE. The Doctorate is now in the 4th cycle, and it has transformed into an Industrial Doctorate (supported by various companies) with the support of the SCOPE project and the four PIs. Various PhD students spend mobility periods in other PIs labs.
- the second is a joint Doctorate between UniWAR and UoA for PhD students in co-tutelle
Two ERC PoCs projects resulted from the SCOPE project.
The following progress beyond the state of the art can be mentioned:

- A new plasma-catalytic reactor based on a confined generation of nanoplasma within a semiconductor TiO2 nanomembrane, to couple nanoconfined plasma with light illumination.
- A new reactor concept of gas-phase photocatalytic conversion of CO2 based on TiO2 nanomembrane.
- Novel improved materials for N2 conversion to NH3 in electrocatalytic conditions (NRR), used as benchmarking.
- TiO2-based nanostructured catalytic electrodes decorated with nanoparticles
- new concept DBD plasma-catalytic reactors
- TiO2 based electrodes for non-oxidative coupling of methane
- Benchmarking with tests on the photo-, electro- or photoelectron-reduction of CO2 and analysis of N2 to NH3 electrocatalytic conversion,
- Preparation of micro/nanopatterned electrodes
- Framework analysis of direct electrification technologies (plasma-, photo- and electrocatalysis) in the future sustainable and low-carbon energy and chemical production.
- Start the development of a general new theory for understanding mechanisms in plasma, electro and photocatalysis trio

- DFT simulations for plasma-catalytic methanol synthesis from CO2 hydrogenation,
- Development of a model for post-plasma-catalytic NO production,
- Development of a novel in-situ FTIR cell for an atmospheric pressure DBD to observe the surface species in plasma-catalytic dry reforming of methane
- Studies on post-plasma quenching nozzles, by both experiments and modelling, for improving plasma-based CO2 conversion,
- Experiments for CO2 conversion into CO by plasma reactors in series to mimic gas recycle flow,
- A study of in-situ resource utilisation of the Martian atmosphere (i.e. CO2 conversion and N2 fixation),
- Experiments on the combined CO2/CH4 conversion into syngas,
- Gliding arc reactor design modification,
- Plasma catalysis NH3 synthesis, demonstrating how catalysts modify the plasma behaviour
- Studying NH3 and HNO2 formation and loss mechanisms from air plasma with water

- Novel method for detecting plasma species using tunable diode laser absorption spectroscopy (TDLAS)
- Novel plasma reactors: surface-confined plasma, nanosecond plasma jet and two electron-temperature plasma reactors
- Intensified field charge injected plasmas in microtip-micropyramid electrodes
- NH3 and NOx formation in the micropyramid reactor
- Nanomaterial synthesis using a plasma microjet in a submerged liquid microvolume
- Non-thermal and thermal plasma studies to identify new industrial translation opportunities
- Sustainability analysis for CH4-to-H2-to-NH3 conversion by integration of high-temperature plasma and non-thermal plasma processes
- Techno-environmental assessment of small-scale Haber-Bosch and plasma-assisted NH3 supply chains
- Plasma technology's Environmental, Social and Governance (ESG) compared to conventional technology
Scheme of N2 fixation to NH3 by plasma-catalytic approach
Scope project
Microplasma in CH4 activation to C2H4
Plasma-array microplasma reactor