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Development of a Semi-Artificial Chloroplast

Periodic Reporting for period 1 - SmArtC (Development of a Semi-Artificial Chloroplast)

Okres sprawozdawczy: 2020-10-01 do 2022-09-30

The transition to a green and sustainable energy-based economy is a critical challenge facing society. Using artificial photosynthesis to produce renewable fuels from CO2 and water using sunlight is an attractive approach. However, efficient CO2 reduction and water oxidation remain major obstacles. A biohybrid approach using both biological and synthetic components has been developed to produce fuels and chemicals in a sustainable manner. The project has achieved most of its objectives and milestones, but modifications were made to the initially planned biohybrid system to make it more robust.
The work carried out in Work Package 1 involved the synthesis, surface modification, and structural study of carbon-based photocatalysts, such as carbon dots and carbon nitrides. These materials were chosen for their environmental friendliness, scalability, low cost, non-toxicity, and robustness.
Work Package 2 focused on interfacing carbon-based materials with synthetic catalysts and enzymes to explore their catalytic activity capabilities, such as immobilization and/or covalent labeling of the carbon-based light harvesters with synthetic and biological catalysts and other proteins to form hybrid systems. This was done to study the effect of the interface in photocatalytic fuel (hydrogen production and CO2 reduction reactions) or chemical production reactions.Moreover mechanistic studies of the hybrid systems under catalytic conditions were performed.
Work Package 3: Anchoring of synthetic carbon-based photocatalysts onto membranes and studying their capacity for compartmentalized reactivity. Carbon-based photocatalysts were anchored onto the natural membrane of the non-photosynthetic bacterium Shewanella Oneidensis MR-1 and artificial lipidic membranes (liposomes) to study their ability to perform an oxidation reaction outside and demonstrate electron transfer across the membrane. The goal of this study was to demonstrate efficient electron transfer across the membrane and the use of transported electrons by another encapsulated catalyst to perform a reductive transformation, thus compartmentalizing two different reactions, oxidation in the outer medium and reduction inside the membrane encapsulated space.
Work Package 4: Development of a whole cell biohybrid fuel producing catalytic system. Synthetic light harvesters were covalently attached to the membrane of the bacterium through site-specific labeling of a transmembrane cytochrome protein found in this microorganism. The covalent labeling of this protein allowed for the demonstration of the electron flow from the light harvester to the heme groups of the transmembrane protein to further engage with other fuel producing reactions.
Work Package 5 (Training) - The researcher gained experience in materials science, heterogeneous catalysis, enzymatic catalysis, biohybrid systems, and various techniques such as TEM, SEM, XPS, DLS, protein/enzyme purification, MS, ICP-OES, microfluidics and electrophoresis. She expanded her background in artificial photosynthesis, photocatalysis, homogeneous catalysis, coordination chemistry and mechanisms, by learning bioconjugation chemistry, biological techniques, and enzymatic/heterogeneous catalysis. She also gained training in technology transference between academia and industry, as well as personal effectiveness in issues relating to the commercialization of technologies, science research management, leadership and application writing.
Work Package 6 (Management, dissemination and communication) - The researcher managed the project, research budget, and data management plan, career development plan and ethics assessment. The plan for exploitation and dissemination of results from the research proposal was followed, and results were published in top tier journals and open-access repositories. She disseminated results through presentations and prestigious events, engaged with EU policy makers and had a strong social media presence.
The project offered the researcher an opportunity to gain new scientific and practical skills for developing hybrid systems for solar fuel production. The research lab has a history of supporting postdoctoral researchers to become independent academics. The researcher benefited from EU networks and established collaborations with other labs. The University of Cambridge offers unique training opportunities for researchers. The researcher gained experience in interfacing natural enzymes with synthetic components for sustainable fuel and chemical production, and in project management, grant writing, and leadership skills. Additionally, the researcher participated in large-scale research initiatives in solar fuel production, and served as the project manager of the UK Solar Fuels Network. Furthermore, researcher was involved in initiatives.

The researcher gained experience in interfacing natural enzymes with synthetic components to produce fuels and chemicals in a sustainable manner, building on her previous expertise in homogeneous catalysis and artificial photosynthesis. The research has impacted the field of semiartificial photosynthesis by developing biohybrid photocatalytic systems for solar fuels and chemicals. They have developed a whole cell fuel producing microbial system from a non-photosynthetic bacterium, by flipping the natural electron flow and using site-specific binding of a light harvester. This could contribute to the discovery and design of new biohybrid systems for sustainable production of solar fuels and chemicals. Additionally, the researcher has been in charge of project management, reports, and supervised undergraduate, MSc, and PhD students and has been engaged in grant writing which helped to improve her leadership and project management skills.

In summary, the fellowship has had a significant impact on the professional development of the beneficiary and has prepared her well to apply for funding and start an independent career. The Marie Curie research project has served as a stepping stone towards this. The beneficiary has been awarded a La Caixa Junior Leader Incoming Program and a prestigious Ramon y Cajal grant, which has allowed her to begin an independent research career in Spain in October 2022.
examples of biohybrid catalystic systems