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Bio-inspired hydrogen production with photo-active surfaces

ABG-105599 Sujet de Thèse
14/05/2022 Contrat doctoral
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Faculté des Sciences et Techniques, Aix-Marseille Université
Marseille - Provence-Alpes-Côte d'Azur - France
Bio-inspired hydrogen production with photo-active surfaces
  • Physique
  • Chimie
  • Energie
photovoltaic, hydrogen, synthetic chemistry

Description du sujet

The development of photochemistry exploiting sunlight to produce fuels and basic chemicals (ammonia, hydrogen peroxide, …) from readily available raw materials (water, carbon dioxide, atmospheric nitrogen and oxygen, …) is a major research priority for the 21st century. Natural photosynthesis is a source of inspiration in this field, and the first functional molecular-based photocathodes for hydrogen production have recently appeared in the literature, combining molecular photosensitizers as a substitute for photosystems and catalytic centers mimicking the enzymes involved in bioenergetic processes. [1,2] The great challenges in the field of photocatalytic hydrogen production include the development of systems based on earth-abundant materials as well as improving their efficiency and longevity. The efficient production of green hydrogen is a crucial step towards a green energy economy that mitigates the harmful effects of fossil fuels and combats global warming. This interdisciplinary project bringing together physicists and chemists aims to tackle the main problem of hydrogen production, namely the use of a noble, rare and expensive metal: platinum. To produce a greener source of hydrogen, we will use sunlight as an inexpensive, abundant and non-polluting source of energy. In this context, we propose to design new solid-state photocatalysts using crystalline silicon photovoltaic cells which will be surface-enhanced with suitable and functional molecular catalysts to produce hydrogen using solar energy and from a proton source.

For this, we are going to divert a silicon homo-junction photovoltaic cell from its traditional use. In general, under the effect of light radiation, a photovoltaic cell induces an electron-hole pair which will migrate on either side of the surface. The face receiving the electrons will therefore be reducing (N-type Silicon) and that receiving the holes, or electronic gap, will therefore be oxidizing (P-Type silicon). If we functionalize these different surfaces with molecular catalyses capable of exploiting oxidation-reduction properties, we will be able to carry out chemical transformations of interest in a virtuous way, such as the production of hydrogen.

The main objective of this subject will be to focus on the functionalization of the photo-reductive surface by molecular catalysts to induce the transformation of protons and electrons into dihydrogen in an efficient, stable and sustainable way. Based on the catalysts already developed by the BiosCiences team at iSm2 [3-5], new targets will have to be synthesized in order to be grafted onto a solid surface. Many grafting solutions have been described in the past in the literature and make use of carboxylate and phosphonate functions or silane oxides [6] In this context and taking into account the chemically modulable structure of our catalysts, two options can be be reasonably considered to combine phosphonate groups with our catalysts.

[1] J. Am. Chem. Soc. 2016, 138, 38, 12308 – 12311
[2] Eur. J. Inorg. Chem. 2021, 30, 3097-3103
[3] Chem. Cat. Chem., 2017, 9, 2262-2268
[4] Chem. Eur. J., 2018, 24, 8779-8786.
[5] Dalton Trans., 2020, 49, 5064-5073.
[6] ACS Appl. Mater. Interfaces 2015, 7, 6, 3427–3455.
 

Nature du financement

Contrat doctoral

Précisions sur le financement

The successful candidate will have to invest time to prepare for the competition.

Présentation établissement et labo d'accueil

Faculté des Sciences et Techniques, Aix-Marseille Université

The interaction between the BiosCiences teams of iSm2 (https://ism2.univ-amu.fr/fr/biosciences/biosciences) and IRM-PV of IM2NP (https://www.im2np.fr/en) will allow the design and characterization of samples in an efficient and complete way for rapid convergence towards the most relevant strategy.

In particular, we will be able to rely on the IRM-PV team and its expertise in photovoltaic conversion and radiation detection. The latter owns and develops a range of specific characterization tools to carry out studies ranging from material to device.

We will also be able to rely on the BiosCiences team which uses specific equipment and its expertise to develop a mixed approach based on experience and theory in the context of molecular photo-electrocatalysis centered on the production of hydrogen and with a special emphasis on understanding the structural and electronic factors governing the reactivity of the developed systems.

As part of this project, the IRM-PV team will be in charge of the development of functionalizable surfaces and the BiosCiences team will be responsible for the synthesis of molecular catalysts and surface grafting. The photo-physical studies will be carried out by the IRM-PV team and the photo-catalytic studies will be carried out by the hydrogen team. All of these studies will ultimately make it possible to obtain original photovoltaic cells whose functionalized surfaces will be used to carry out the photo-conversion of protons and electrons to produce hydrogen in a clean, efficient and sustainable manner.

Intitulé du doctorat

Doctorat de physique

Pays d'obtention du doctorat

France

Etablissement délivrant le doctorat

Aix-Marseille Université

Ecole doctorale

Physique et sciences de la matière

Profil du candidat

This phD proposal is for a inter-doctoral school funding, meaning it is a competition between several subjects coming from two different Aix-Marseille University departments. In our case, it is between physics and chemistry. (https://college-doctoral.univ-amu.fr/)

 Due to the highly competitive nature of the funding, we are seeking for a very talented young scientist, willing to invest time and thought in an other science.

For candidates with a French master's degree, an annual average grade of less than 12/20 will not be considered.

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