Towards the 4 V-class n-type organic lithium-ion positive electrode materials: the case of conjugated triflimides and cyanamides

Literature Information

Publication Date 2023-11-20
DOI 10.1039/D3EE02897F
Impact Factor 38.532
Authors

Xiaolong Guo, Petru Apostol, Xuan Zhou, Jiande Wang, Xiaodong Lin, Darsi Rambabu, Mengyuan Du, Süleyman Er, Alexandru Vlad


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Abstract

Organic electrode materials have garnered a great deal of interest owing to their sustainability, cost-efficiency, and design flexibility metrics. Despite numerous endeavors to fine-tune their redox potential, the pool of organic positive electrode materials with a redox potential above 3 V versus Li+/Li0, and maintaining air stability in the Li-reservoir configuration remains limited. This study expands the chemical landscape of organic Li-ion positive electrode chemistries towards the 4 V-class through molecular design based on electron density depletion within the redox center via the mesomeric effect of electron-withdrawing groups (EWGs). This results in the development of novel families of conjugated triflimides and cyanamides as high-voltage electrode materials for organic lithium-ion batteries. These are found to exhibit ambient air stability and demonstrate reversible electrochemistry with redox potentials spanning the range of 3.1 V to 3.8 V (versus Li+/Li0), marking the highest reported values so far within the realm of n-type organic chemistries. Through comprehensive structural analysis and extensive electrochemical studies, we elucidate the relationship between the molecular structure and the ability to fine-tune the redox potential. These findings offer promising opportunities to customize the redox properties of organic electrodes, bridging the gap with their inorganic counterparts for application in sustainable and eco-friendly electrochemical energy storage devices.

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Energy & Environmental Science

Energy & Environmental Science
CiteScore: 32.34
Self-citation Rate: 3.4%
Articles per Year: 481

Energy & Environmental Science is an international journal dedicated to publishing exceptionally important and high quality, agenda-setting research tackling the key global and societal challenges of ensuring the provision of energy and protecting our environment for the future. The scope is intentionally broad and the journal recognises the complexity of issues and challenges relating to energy conversion and storage, alternative fuel technologies and environmental science. For work to be published it must be linked to the energy-environment nexus and be of significant general interest to our community-spanning readership. All scales of studies and analysis, from impactful fundamental advances, to interdisciplinary research across the (bio)chemical, (bio/geo)physical sciences and chemical engineering disciplines are welcomed. Topics include, but are not limited to, the following: Solar energy conversion and photovoltaics Solar fuels and artificial photosynthesis Fuel cells Hydrogen storage and (bio) hydrogen production Materials for energy systems Capture, storage and fate of CO2, including chemicals and fuels from CO2 Catalysis for a variety of feedstocks (for example, oil, gas, coal, biomass and synthesis gas) Biofuels and biorefineries Materials in extreme environments Environmental impacts of energy technologies Global atmospheric chemistry and climate change as related to energy systems Water-energy nexus Energy systems and networks Globally applicable principles of energy policy and techno-economics

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