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Herein, a computational predictive tool for redox flow batteries based on NBO and ADCH charge distribution studies is presented and supported by experimental evidence. Using highly water soluble (>2 M) non-planar 2,2′ - bipyridinium salts as a case of study, this work presents a DFT protocol that successfully predicts the stability and forecasts their potential application as active materials for Aqueous Organic Redox Flow Batteries (AORFB). An initial theoretical-experimental characterization of selected bipyridines served to determine the effect of the ring size, geometry, and electron density on the physico-chemical properties of the materials. Nonetheless, the NBO and ADCH charge analyses were essential tools to understand the stability of the reduced species in terms of electronic delocalization and the importance of the molecular design on the stability of electrolyte for AORFB. Based on these results, the cell performance of seven-membered 2,2′ -bypiridinium salt, (2), and m-Me substituted homologous, (4), were compared. The significantly lower capacity decay rendered by compound 4 based electrolyte, (0.35%/cycle) compared with compound 2 based electrolyte, (0.71%/cycle) was in good agreement with the predicted stability. The aim of this work is to highlight the powerful synergy between DFT calculations and organic chemistry in predicting the behaviour of different negolytes, This work has been funded by the European Union under the HIGREEW project, Affordable High-performance Green Redox Flow batteries (Grant agreement no. 875613). H2020: LC-BAT-4-2019. A.C. Lopes acknowledges the Ramon y Cajal (RYC2021-032277-I) research fellowship, the financial support from Ministerio de Ciencia e Innovacion ´ / AEI /10.13039/501100011033 and from European Union NextGenerationEU/PRTR. We also thank the CCC-UAM (Graforr project) for allocation of computer time

Redox-flow batteries, based on their particular ability to decouple power and energy, stand as prime candidates for cost-effective stationary storage, particularly in the case of long discharges and long storage times. Integration of renewables and subsequent need for energy storage is promoting effort on the development of mature and emerging redox-flow technologies. This review aims at providing a critical analysis of redox-flow technologies that can potentially fulfill cost requirements and enable large scale storage, mainly aqueous based systems. A comprehensive overview of the status of those technologies, including advantages and weaknesses, is presented. Compiled data on the market permeability, performance and cost should serve, together with the perspective included, to understand the different strategies to reach the successful implementation, from component development to innovative designs., European Union under HIGREEW, Affordable High-performance Green Redox Flow batteries (Grant Agreement no. 875613) and CuBER, Copper-Based Flow Batteries for energy storage renewables integration (Grant agreement no: 875605) projects. Basque Government (GV-ELKARTEK-2020 KK-2020/00078), Spanish MINECO (RTI2018-099228-A-I00 and RYC2018-026086-I (Ramon y Cajal fellowship) E.V.) and CDTI (Centro para el Desarrollo Tecnológico Industrial, CER-20191006) are also acknowledged for funding this work. R.M. thanks the European Research Council (ERC) through “MFreeB” project (grant agreement no. 726217)