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Photocatalytic Reactions Under Light and Dark with Transient Supramolecular Assemblies

Periodic Reporting for period 1 - PhotoDark (Photocatalytic Reactions Under Light and Dark with Transient Supramolecular Assemblies)

Période du rapport: 2023-10-01 au 2026-03-31

The global transition to clean energy requires new ways of storing sunlight in the form of chemical fuels and useful chemicals. Today, most industrial chemical processes still rely on fossil fuels, high temperatures, or expensive metals. One promising alternative is photocatalysis – using light to drive chemical reactions – but most current systems work only in organic solvents, contain rare metals, or cannot store energy efficiently. As a result, there is a need for new approaches that can operate in water, use abundant materials, and perform complex chemical transformations using only light.

This project addresses these challenges by developing organic molecules and soft materials that can capture sunlight, store its energy, and use it to perform useful chemistry. The central idea is that molecules can behave very differently when they come together and organise into larger structures, known as supramolecular assemblies. By carefully designing the building blocks and controlling how they assemble, we aim to create materials that respond to light in new and useful ways: for example, by generating clean fuels such as hydrogen, converting simple chemicals into more valuable ones, or storing energy for use in the dark.

The project focuses on three main objectives. First, we design and study new light-absorbing organic molecules that can work effectively in water. Second, we explore how these molecules organise into larger structures and how this organisation changes their ability to capture and use light energy. Third, we develop functional catalytic systems, including soft and dynamic materials, that can perform demanding reactions such as the conversion of acetylene into ethylene – an important process for producing plastics – or the transformation of biomass-derived glycerol into valuable products.

By combining molecular design, supramolecular chemistry, and green photocatalysis, the project aims to demonstrate fundamentally new ways to control chemical reactivity using light. The expected impact is twofold: advancing our scientific understanding of how organised molecular systems work, and laying the foundation for future technologies that use sunlight to produce chemicals more sustainably, with minimal waste and no reliance on scarce resources.
Since the start of the project, we have made significant progress in creating new light-responsive molecules and materials that can use sunlight to drive chemical reactions in water. Much of the work focused on designing families of colourful organic molecules and understanding how their behaviour changes when they come together and form organised structures. These studies showed that when the molecules assemble into larger aggregates, their ability to absorb and use light can increase dramatically. In some cases, we discovered that the same molecule can perform different reactions depending on how it is assembled, offering a new way to “switch” photocatalytic behaviour simply by changing the supramolecular structure.

We also developed soft and dynamic materials that respond to light or chemical cues by changing their structure or activity. These included a mechanically responsive hydrogel whose photocatalytic activity can be modulated by swelling and contraction, assemblies driven temporarily by biochemical molecules, and soft materials capable of storing light-generated electrons for use in the dark. Together, these systems demonstrate that flexible and evolving materials can regulate chemical reactivity in ways that traditional catalysts cannot.

In parallel, we made important progress in developing catalytic systems for practical chemical transformations. We created efficient light-driven methods for converting acetylene into ethylene, a key building block for plastics. One of the catalysts developed in the project can operate both in solution and as part of a solid material, opening opportunities to integrate molecular catalysts into larger functional assemblies. We also developed photocatalytic processes that upgrade glycerol – a widely available by-product of biodiesel production – into valuable molecules such as formic acid or glyceraldehyde, using only visible light and water.

Overall, the project has delivered new molecular designs, new forms of supramolecular organisation, and new catalytic functions. These achievements show that carefully designed organic molecules and soft materials can capture sunlight, regulate how energy flows through them, and use that energy to perform useful and selective chemical transformations in water. The results achieved so far provide a strong foundation for developing even more advanced light-powered systems in the next stages of the project.
The project has produced several results that go significantly beyond current approaches to light-driven chemical reactivity. One of the most important advances is the discovery that the way organic molecules organise themselves in water can be used to control the type of chemical reaction they perform. We showed that simply changing how the molecules pack together can “switch” the outcome of a photocatalytic reaction, even though the molecular structure remains the same. This represents a new concept in photocatalysis and opens the door to adaptive and programmable light-driven systems.

Another key advance is the development of soft and dynamic materials that can regulate their activity in response to light, mechanical forces, or biochemical fuels. Unlike conventional catalysts, these materials can reorganise, store light-generated energy temporarily, or operate only for limited periods when fuel is available. Such behaviours are rarely observed in traditional photocatalytic systems and offer new ways to control when and how chemical reactions take place.

The project also demonstrated that light can be used to drive challenging chemical transformations relevant to industry. We developed selective photocatalytic systems for converting acetylene into ethylene – a critical step in producing plastics – using mild conditions and abundant materials. In addition, we created photocatalytic processes that convert glycerol, a waste product of biodiesel production, into valuable chemicals. These results illustrate how sunlight can be used to upgrade widely available feedstocks in a sustainable way.

Together, these achievements point toward new technologies that combine molecular design, self-assembly, and green photocatalysis. For these innovations to reach their full potential, several developments will be important in the future. Further research will be needed to scale up the most promising reactions and to integrate the light-responsive materials into devices or continuous-flow systems. Access to specialised fabrication facilities and photochemical testing platforms will help bridge the gap between laboratory experiments and practical applications. In the long term, collaborations with industrial partners may support demonstration activities, identify suitable markets, and ensure that new methods comply with safety and regulatory frameworks.

Overall, the results go beyond current scientific understanding by showing that organised molecular systems and soft materials can be used to control light-driven chemistry in new ways. They also highlight clear opportunities for sustainable chemical production, renewable-energy storage, and the development of environmentally friendly catalytic processes.
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