Atomic-Scale Tailored Materials for Electrochemical Methane Activation and Production of Valuable Chemicals

Project Information

ATOMISTIC

Grant agreement ID: 101045778

DOI

10.3030/101045778

EC signature date 7 June 2022

Start date 1 June 2023

End date 31 May 2028

Funded under

• European Research Council (ERC)

Total cost

€ 1 999 774,00

EU contribution

€ 1 999 774,00

Coordinated by

FUNDACIO INSTITUT CATALA DE NANOCIENCIA I NANOTECNOLOGIA
Spain

Periodic Reporting for period 1 - ATOMISTIC (Atomic-Scale Tailored Materials for Electrochemical Methane Activation and Production of Valuable Chemicals)

Reporting period: 2023-06-01 to 2025-11-30

Summary of the context and overall objectives of the project

Electrochemical methane activation and direct conversion to methanol is highly attractive – a dream reaction that would convert a greenhouse gas into a valuable liquid fuel in a dream device, on-site, and powered by renewable electricity. However, sustainable C-H activation and direct methane to methanol conversion at ambient conditions remain as great fundamental challenges.
My aim with ATOMISTIC is: (i) to develop new methods for electrochemical methane activation and partial oxidation, (ii) to control the structure of the electrochemical interface and the catalytically active site, in order to tune selectivity for the synthesis of valuable fuels and chemicals (such as methanol) from methane, and dimethyl carbonate from methanol. I will use three main strategies:
- To establish the ideal catalyst structures and electrolytes, using well-defined tailored materials that enable methane activation by its direct adsorption on the electrode material.
- To realise advanced materials that enable the indirect electrochemical activation of methane through the generation of solution phase radicals.
- To tailor the active site at the atomic level for selective methane to methanol and methanol to dimethyl carbonate conversion on functional materials.
I will elucidate the design principles and unveil the structure-reactivity-selectivity relations and the molecular mechanisms of these reactions, as well as the atomic-scale structure of the catalyst materials. I will achieve these ambitious goals by leveraging my work combining the insight from model studies with experiments under realistic conditions to discover new materials. I will combine electrochemical methods, in situ optical spectroscopy, online mass spectrometry, electrochemical scanning probe microscopy and operando synchrotron-based x-ray techniques. The success of ATOMISTIC will result in significant breakthroughs in the fields of chemistry and catalysis, opening up new sustainable ways to produce valuable chemicals.

Work performed from the beginning of the project to the end of the period covered by the report and main results achieved so far

The initial phase of the project focused on:
- Establishing laboratories and core research infrastructure to enable key experimental techniques required for the ATOMISTIC project.
- Preparing, characterising, and tailoring well-defined electrodes and advanced materials for electrochemical methane conversion into methanol via both direct and indirect activation pathways.
Key developments include the implementation of in-situ Raman and infrared spectroscopy, scanning electrochemical microscopy (SECM), electrochemical scanning tunnelling microscopy (EC-STM), and quantitative product detection. The interdisciplinary foundation combines physical/surface chemistry, spectroscopy, microscopy, materials and chemical engineering, and electrochemistry. This integrated approach is crucial for advancing catalyst and mechanistic design for electrochemical methane activation.
We have developed and characterised well-defined interfaces and electrocatalysts for the direct electrochemical activation and partial oxidation of methane and have initiated studies on structure sensitivity using single-crystalline electrodes. These model investigations are essential for understanding how various experimental parameters influence activation mechanisms on well-defined surfaces. In parallel, we are investigating metal oxides for this reaction and their competition with the oxygen evolution reaction. Our studies on electrochemical methane conversion have focused on identifying the impact of key experimental conditions, which is critical for elucidating structure–activity–selectivity relationships. Even in simplified model systems, our results show that multiple parameters significantly affect the outcome, highlighting the need for fundamental mechanistic studies on model catalysts and a systematic understanding of how operating conditions shape catalytic performance.
Finally, we have designed and developed advanced materials with tailored active sites. Novel composite materials have been prepared and characterised for the partial oxidation of methane into methanol. Our work aims to uncover new structure–activity relationships and opens new possibilities for discovering efficient and selective catalysts for electrochemical methane-to-methanol conversion.
Overall, these interdisciplinary efforts have paved the way for atomic-level material design and the refinement of analytical techniques.

Progress beyond the state of the art and expected potential impact (including the socio-economic impact and the wider societal implications of the project so far)

There are no published results beyond the state-of-the-art.