Oxygen-mediated (self-)rechargeable organic batteries

Project Information

SoloBat

Grant agreement ID: 101064286

DOI

10.3030/101064286

Project closed

EC signature date 1 August 2022

Start date 1 October 2022

End date 30 September 2024

Funded under

• Marie Skłodowska-Curie Actions (MSCA)

Total cost

No data

EU contribution

€ 191 760,00

Coordinated by

UNIVERSITE CATHOLIQUE DE LOUVAIN
Belgium

Periodic Reporting for period 1 - SoloBat (Oxygen-mediated (self-)rechargeable organic batteries)

Reporting period: 2022-10-01 to 2024-09-30

Summary of the context and overall objectives of the project

The SoloBat project is set against a backdrop of urgent global challenges—namely climate change and the energy crisis—that demand sustainable energy solutions. Traditional energy sources, rooted in fossil fuels, are rapidly depleting and contributing significantly to environmental pollution and climate change, undermining future societal resilience. In response, the European Union has committed to transitioning towards a decarbonized energy system, as outlined in the European Green Deal, aiming for climate neutrality by 2050.

Li-ion batteries (LIBs) play a crucial role in this energy transition due to their efficiency and ability to support renewable energy storage and electrified transport. However, further advances are needed to enhance sustainability and performance. In this context, oxygen-mediated Li-organic batteries represent an innovative direction with potential for self-rechargeability using ambient oxygen. This builds on early-stage work by Poizot et al., who proposed a primary Li-organic battery concept capable of chemical recharge through air exposure. Yet, the limitations of reversibility and cycling stability have hindered its practical application.

SoloBat's main objectives are to transform this initial concept into a rechargeable system capable of over 300 cycles, termed as an oxygen-mediated, self-rechargeable organic battery. This will involve addressing key challenges including the accumulation of oxygen reduction products, the identification of reaction chemistry, and the prevention of anode degradation. The project will achieve these aims through an interdisciplinary approach encompassing organic chemistry, catalysis, and advanced electrochemical analysis.

By realizing a robust, rechargeable SoloBat system, the project expects to contribute significantly to the EU's strategic goals of energy decarbonization, aligning with Horizon 2020 and the UN Sustainable Development Goals. The outcomes could establish new paradigms in sustainable battery technology, reduce dependence on non-renewable resources, and foster economic growth through innovative energy solutions.

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

During the execution of the SoloBat project, we developed a comprehensive suite of operando and ex situ characterization techniques to analyze oxygen reduction species in SoloBat systems. These techniques include operando synchrotron X-ray diffraction and imaging, in situ electrochemical differential mass spectrometry, X-ray diffraction, Fourier transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy, iodine titration analysis, scanning electron microscopy, and electron paramagnetic resonance (EPR) spectroscopy. Additionally, we designed and evaluated a range of advanced electrode materials, such as high-voltage n-type organic cathodes, quinone-based derivatives, conductive metal-organic frameworks (MOFs), and fluorine-doped bimetallic oxide oxygen catalysts, significantly enriching the SoloBat project's material library. Furthermore, we developed novel dicarbonate and ternary salt-solvent electrolytes with excellent lithium metal compatibility, offering potential as innovative electrolyte systems for the SoloBat system. These electrolytes form unique solid electrolyte interphases (SEIs) and integrate well with solid-state separators, providing effective protection against oxygen corrosion of lithium metal. Collectively, these efforts exceeded the project’s objectives by achieving >300 stable cycles and contributing to the advancement of sustainable battery technologies.

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)

The research conducted under the SoloBat project demonstrates significant advancements beyond the state of the art in multiple areas of sustainable energy storage and battery technology. Below is an overview of these results and their potential impacts:

Results and Advancements
1. Novel Energy Storage Concepts and Reaction Mechanisms
o Pioneering the SoloBat Concept: The project introduced an innovative oxygen-mediated, self-rechargeable organic battery system, integrating the chemistries of lithium-organic and lithium-oxygen batteries. This concept addresses limitations in existing primary O2-mediated Li−organic battery (PoloBat) technology, transforming the initial‘PoloBat’ concept into a rechargeable ‘SoloBat’ system.
o Reaction Mechanism Insights: Detailed understanding of oxygen-reduction processes and interfacial chemistries was achieved, including the development of competitive adsorption catalytic mechanisms via fluorine-doped bimetallic oxides. These insights redefine catalytic designs for lithium-oxygen batteries and other energy applications.
2. Material Innovations for Cathodes and Electrolytes
o High-Voltage Organic Cathodes: Development of conjugated triflimides and cyanamides achieved redox potentials up to 3.8 V, representing the highest values reported for n-type organic materials. These materials provide significant opportunities for advancing high-energy-density and sustainable battery systems.
o Electrolyte Systems for High-Voltage Stability: Novel dicarbonate solvents and ternary salt-solvent electrolytes were developed, achieving anodic stability up to 5.2 V and supporting efficient lithium-metal interfaces. These systems resolve challenges in lithium dendrite formation and electrolyte decomposition, paving the way for safer, high-performance batteries.
3. Ionic Conduction in MOFs
o For the first time, solid-state ionic conductivity was demonstrated in bimetallic anionic MOFs, achieving high cation transport with reversible redox capabilities. These results address the long-standing challenge of integrating solid-state ionic conduction in MOFs for charge storage.

Potential Impacts
• Scientific Impact:
o The insights and innovations contribute to advancing the understanding of interfacial chemistries, catalyst designs, and material compatibility in energy storage systems. This work sets a foundation for further exploration of oxygen-mediated systems and high-voltage organic chemistries.
• Technological Impact:
o The materials and electrolytes developed have direct applicability in next-generation batteries, offering higher energy densities, improved safety profiles, and longer lifetimes.
• Economic and Societal Impact:
o By enhancing the sustainability and efficiency of battery technologies, these results support the transition to renewable energy solutions and align with global climate goals.

Key Needs for Further Uptake
1. Further Research:
o Expand studies on the long-term stability and scalability of oxygen-mediated organic batteries.
o Explore the integration of novel cathode and electrolyte materials in prototype systems for large-scale applications.
2. Demonstration and Commercialization:
o Conduct real-world testing of the SoloBat system in operational environments to validate its performance.
o Establish partnerships with industry to commercialize high-voltage cathodes and electrolytes.
3. IPR and Regulatory Support:
o Secure intellectual property rights for the materials and systems developed, ensuring competitive positioning in the market.
o Engage with regulatory bodies to establish standards for novel battery chemistries.
4. International Collaboration:
o Strengthen partnerships with global research and industry players to enhance technological development and market access.

This project’s results not only exceed current standards but also chart a pathway for continued innovation and impactful contributions to sustainable energy storage technologies.

A fluorine-doped bimetallic cobalt-nickel oxide oxygen cathode was proposed and designed

A new electrolyte solvent with good lithium metal and high voltage anodic stability was proposed

A lithium oxygen battery with more than 580 cycles was realized

Proposed design principle of organic quinone redox systems for solid-state Li metal batteries

High voltage lithium-based batteries with more than 300 cycles were realized

A solid-state organic battery with 2000 cycles and energy density as high as 718 Wh/kg was realized