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Redox Polymer with synergetic electrical and ionic conducting properties for all-Organic Batteries. [RPOB]

Periodic Reporting for period 1 - RPOB (Redox Polymer with synergetic electrical and ionic conducting properties for all-Organic Batteries. [RPOB])

Reporting period: 2021-05-01 to 2023-04-30

The development of more efficient and safer solid-state energy storage is imperative to sustainably meet the energy demand of our future society and was recently announced as one of the top 10 emerging technologies in chemistry by the International Union of Pure and Applied Chemistry, IUPAC. The current Li-ion battery technology, which is mainly based on inorganic transition metal oxide materials (e.g. lithium cobalt oxide (LCO) and nickel cobalt manganese oxide (NMC)), has recently drawn health, social and environmental concerns due to the toxicity or limited mineral resources of some inorganic components (e.g. nickel and cobalt). On the contrary, organic redox polymers are environmentally friendly and offer significant advantages, which are not easily achievable with inorganic electrode materials, including low cost, structural diversity, flexibility, ease of processability and recyclability. However, all-organic batteries suffer several challenges, limiting their implementation: i) fast capacity fading due to dissolution of the organic redox polymer in the liquid electrolyte and ii) low redox active polymer loading (~50 wt.%) due to poor electronic conduction, leading to impractical electrode loading for battery applications.
The aim of RPOB project is to develop organic redox copolymers with enhanced electronic and ionic conduction properties, for application in organic batteries. This could potentially reduce the need for weight consuming conductive carbon additives, and thus, enhancing electrode loading to a practical level.
The RPOB project aimed on the development of redox co-polymer with enhanced ionic and/electronic conduction properties. To achieve this main goal, two synthetic strategies have been developed: I) Development of redox-active polymeric nanoparticles. II) Development of redox-active random co-polymer with inherent π conjugation and porosity. In the first strategic, it was hypothesized that the nanosizing of the redox-active particles would reduce the ion diffusion pathway for electrolyte to reach the core of the redox-active particles, and thus, will improve the ionic conduction properties within the material. In the second approach, it was rationalized that the π conjugation would improve the electronic conductivity of the polyimide material. While simultaneously the high surface area and pore structure would promote high ionic conductivity within the electrode composite after the liquid electrolyte has filled the networks and frameworks’ porosity due to the reduced diffusion pathways to access the redox active sites as compared to dense polymers.


The chemical structure and purity of all materials developed in this project was characterized by nuclear magnetic resonance (NMR), Fourier transform infrared (FTIR) and elemental analysis. Additionally, the structural properties were characterized by means of scanning and transmission electron microscopies, X-ray diffraction, Brunauer-Emmett-Teller (BET) surface area analysis and dynamic light scattering. The electrochemical characterization of the monomer model molecules and the corresponding polymer was initially investigated by cyclic voltammetry in order to assess electrolyte compatibility.
Finally, the use of the redox co-polymers as active electrode materials in organic-based batteries was investigated. For this purpose, electrode formulation protocols were developed, and their cycling performance assessed in a coin cell configuration. Rate capability and long-term cycling stability of the battery prototypes were assessed and compared with the literature.

Over the course of the RPOB project, the ER published three research articles and one review article:

1. Chemical Engineering Journal 461, 142001 (2023).
2. Mater Horiz 10, 967–976 (2023).
3. Prog Polym Sci 122, 101449 (2021).
4. Sustainable Chemistry 2, 610–621 (2021).

Additionally, the ER is currently preparing three manuscripts with the remaining results from the RPOB project.

Finally, the ER participated in four international conferences over the course of the fellowship. Of which, three of them were with an oral presentation, and one as an invited speaker. The ER also gave an invited seminar as an outreach activity.
To fight against climate change, our society is now racing towards a carbon-neutral economy, through the electrification of the transport sector and the transitioning from oil-based to renewable-based energy production, via the deployment of stationary energy storage system. As foreseen by the International Energy Agency (IEA), batteries will be a key actor of these technological transitions, with an expected 30-fold increase of the global battery demand by 2030.

The main outcome of the RPOB was the design of novel redox co-polymer materials, demonstrating great promise as alternative active electrode materials for the next generation of batteries. It is noteworthy that the development of more sustainable active electrode materials is of a crucial importance, as highlighted by the rising health, social and environmental concerns from the current inorganic electrode technology used in lithium-ion batteries. In addition to designing electrode materials based on non-scarce elements, the RPOB project also developed synthesis protocol to produce organic-based electrode materials from PET waste, potentially opening a new circular economy for PET waste. Overall, the actions of the RPOB project align with the Sustainable Development Goals (SDGs), in particular SDGs#7 and SDGs#12, proposed by the United Nations, which promoted “Affordable and clean energy” and “Responsible consumption and production”.
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