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H2020

DIACAT Report Summary

Project ID: 665085
Funded under: H2020-EU.1.2.1.

Periodic Reporting for period 1 - DIACAT (Diamond materials for the photocatalytic conversion of CO2 to fine chemicals and fuels using visible light)

Reporting period: 2015-07-01 to 2016-06-30

Summary of the context and overall objectives of the project

In DIACAT we propose the development of a completely new technology for the direct photocatalytic conversion of CO2 into fine chemicals and fuels using visible light. The approach utilises the unique property of man-made diamond, now widely available at low economic cost, to generate solvated electrons upon light irradiation in solutions (e.g. in water and ionic liquids).

The project will achieve the following major objectives on the way to the efficient production of chemicals from CO2:

- experimental and theoretical understanding of the principles of production of solvated electrons stemming from diamond

- identification of optimal forms of nanostructured diamond (wires, foams, porous materials) and different surface modifications such as chemical functionalization and controlled termination with suitable atoms and structures to achieve high photoelectron yield and long term performance

- investigation of optimized energy up-conversion using optical nearfield excitation as a means for the direct use of sunlight for the excitation of electrons-characterisation of the chemical reactions which are driven by the solvated electrons in “green” solvents like water or ionic liquids and reaction conditions to maximise product yields.

- demonstration of the feasibility of the direct reduction of CO2 in a laboratory environment. The ultimate outcome of the project will be the development of a novel technology for the direct transformation of CO2 into organic chemicals using illumination with visible light.

On a larger perspective, this technology will make an important contribution to a future sustainable chemical production as man-made diamond is a low cost industrial material identified to be environmentally friendly.

As an early-stage research project, DIACAT aims at generating fundamental knowledge and developing a new technology towards the long-term goal of a sustainable conversion of CO2. Our approach lays the foundation for the removal and transformation of carbon dioxide and at the same time a chemical route to store and transport energy from renewable sources. This will have a transformational impact on society as whole by bringing new opportunities for sustainable production and growth.

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

From the beginning of the project the partners have worked on the production of novel diamond materials that are suitable for the generation of solvated electrons in solution and the transformation of carbon dioxide into fuels and chemicals.

All work packages of the project have been active in the first funding period. In the first 12 months we have laid the foundation for the in-depth investigation of the photoelectrochemical transformation of carbon dioxide. The necessary starting materials and a first reactor design are ready and will be applied for the next steps.
In WP1 and WP2 diamond materials of different kinds (submicrocrystalline films, first examples of nanostructured membranes and nanoparticles) with and without doping have been developed and produced. They have been provided to the partners responsible for the spectroscopic investigation of the electronic structure.
Experiments on the suitability of ionic liquids for the use of diamond in them have been successfully completed.
Regarding the engineering of the diamond surface several procedures have been developed for the controllable surface termination.
Different types of diamond materials have been successfully terminated with hydrogen and fluorine using plasma and thermal methods.
Furthermore, the oxygen termination of diamond materials was achieved in order to produce materials for control experiments. More complex surface functionalizations have been established as well.
Photocatalytically active metal complexes have been immobilized covalently onto diamond.
These different samples have been investigated using advanced spectroscopy such as x-ray emission and x-ray absorption spectroscopy at the synchrotron facility BESSY II. The already obtained results allow an in-depth characterization of the materials produced within the project. This was accompanied by computational investigation of the electronic structure of undoped, doped and functionalized diamond surfaces.
The systematic search for suitable conditions for the transformation of carbon dioxide into fuels and fine chemicals has started as planned. Analytical methods have been identified that allow the identification and quantification of the reaction products of the transformation. Additionally, the necessary light sources for reliable UV and solar light generation have been tested and characterized. The system is ready for the investigation of different types of electrode materials generated in WP1 and 2 according to the results from WP3 and 4.
Furthermore, ionic liquids have been tested in collaboration of partners in WP 1,3 and 4, and a new type of room temperature ionic liquid has been synthesized. Criteria for suitable solvents for the spectroscopic investigation and the transformation of carbon dioxide have been identified.
In-depth electrochemical characterization of a set of more than ten room temperature ionic liquid was carried out and revealed a clear connection between the chemical structure of the ionic liquid and the resulting electrochemical properties. This knowledge will help in the next funding period to select a suitable solvent system for the generation of solvated electrons.
Furthermore, the solubility of carbon dioxide in these ionic liquids has been investigated. At the current stage of the project a set of three suitable ionic liquids has been identified that are very promising for the application as solvents in the transformation of carbon dioxide.
A first reactor has been designed that enables the investigation of photoelectrochemical processes on diamond electrodes and resembles already a future, scalable device. For the moment, the setup has been adjusted to the available size of diamond and ionic liquids. In the future, this will be further optimized and compared with other conceivable reactor designs before the decision on a large-scale demonstrator design will be taken.
Additionally, laboratory scale reactors for both photochemistry and photoelectrochemistry have been designed and fabricated and have been tested electrochemically so far. They will be the base for the photoelectrochemical experiments planned for the next funding period.

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)

This project as a whole will initiate a major new line of technology for the use of CO2 as feedstock for chemical processes and energy storage. The envisaged technology will not only store the emitted CO2 as e.g. in the CCS (carbon (dioxide) capture and storage) approach, but transform it to less oxidized and hence chemically accessible hydrocarbons (which are in many cases liquids and hence easier to handle and store) and their derivatives. The project will lay the foundation for the development of the direct use of sunlight in chemical conversion of CO2.
Furthermore, in the long term, the project’s outcome will help to decarbonize the energy sector. The direct application of sunlight and the generation of solvated electrons in water or ionic liquids make this technology independent from fossil energy sources and hence it will have an important transformational impact on society by shaping of our energy sources in the future. When electricity from strongly fluctuating renewable resources such as wind or sun is employed, directly or indirectly, the system can be used to store this energy in the form of fuels and chemicals. Such decentralized, mobile and flexible energy storage is one of the components of the strategic energy plan for the European Area (SET-Plan), and DIACAT will lay a foundation towards this goal.
Thus, this project will enable the development of a low-cost technology for the removal of CO2 in a sustainable manner with secure supply chain even at large scale. Due to the stability and corrosion resistance of diamond, the system will exhibit improved long-term stability - a key factor for the efficient implementation of the technology. Application of “optical nearfield excitation” to generate free electrons in the conduction band of diamond is a radically new approach. So far, the optical excitation of electrons in a wide band gap semiconductor like diamond has not been explored. In this light, we will provide the scientific community with fundamental new knowledge in a technologically important area.
In the first funding period the project has successfully developed the methods for the production of the necessary starting materials and analytical tools for the investigation of the CO2 transformation into fuels and other chemicals. The consortium has achieved the production and characterization of novel diamond nanomaterials and their controlled functionalization with e.g. photocatalytically active metal complexes. Detailed information on the electronic structure of these novel materials has been obtained using advanced spectroscopy at the synchrotron facility BESSY II.
Furthermore, we have aimed at interaction with policy makers and society as a whole by installing a website (www.diacat.eu) that is explaining the aim of our research in an accessible manner and use social media to inform interested parties about the progress and news from the DIACAT project. In 2016 we have been selected for a collaboration within the framework of FEAT (Future and Emerging Art and Technology) with the well-known artist Pinar Yoldas, Guggenheim Fellow 2015, to further publicize our work by means of artistic interpretation.
In summary, the initial funding period of DIACAT has laid the foundation for the implementation of the proposed novel technology as a truly transformational technology in the field of energy conversion and storage, which will affect the European society by enabling sustainable growth and energy consumption.

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