Perspective on recent improvements in experiment and theory towards realizing lithium metal electrodes with liquid electrolytes.

This roadmap presents the transformational research ideas proposed by “BATTERY 2030+,” the European large‐scale research initiative for future battery chemistries. A “chemistry‐neutral” roadmap to advance battery research, particularly at low technology readiness levels, is outlined, with a time horizon of more than ten years. The roadmap is centered around six themes: 1) accelerated materials discovery platform, 2) battery interface genome, with the integration of smart functionalities such as 3) sensing and 4) self‐healing processes. Beyond chemistry related aspects also include crosscutting research regarding 5) manufacturability and 6) recyclability. This roadmap should be seen as an enabling complement to the global battery roadmaps which focus on expected ultrahigh battery performance, especially for the future of transport. Batteries are used in many applications and are considered to be one technology necessary to reach the climate goals. Currently the market is dominated by lithium‐ion batteries, which perform well, but despite new generations coming in the near future, they will soon approach their performance limits. Without major breakthroughs, battery performance and production requirements will not be sufficient to enable the building of a climate‐neutral society. Through this “chemistry neutral” approach a generic toolbox transforming the way batteries are developed, designed and manufactured, will be created.

The timely arrival of novel materials plays a key role in bringing advances to society, as the pace at which major technological breakthroughs take place is usually dictated by the discovery rate at which novel materials are identified within chemical space. High‐throughput experimentation and computation strategy, now widely considered as a watershed in accelerating the discovery and optimization of novel materials in virtually every field, enables simultaneous screening, synthesis and characterization of large arrays of different material classes toward identification of the lead candidates for given system and targeted application. However, the ability to acquire data, through the continued advancement of automation platforms and workflows especially in the field of battery research and development, often outpaces the ability to optimally leverage obtained data for improved decision‐making. Closing this gap inevitably calls for adapted algorithms, development of reliable predictive models and enhanced integration with machine learning, deep learning, and artificial intelligence. This Review aims to highlight state‐of‐the‐art achievements along with an assessment of current and future challenges as well as resulting perspectives toward accelerated development of advanced battery electrolytes and their interfaces.

Development of high‐performing lithium‐based batteries inevitably calls for a profound understanding and elucidation of the reactivity at the electrode–liquid electrolyte interface and its impact on the overall performance and safety. The formation, composition, properties, and mechanisms of the cathode electrolyte interphase (CEI) formation and function are still to a large extent unknown for most lithium‐based battery materials, whereas the same is well considered for the solid electrolyte interphase on negative electrodes in the literature. In particular, in high voltage regions >4.3 V, the oxidative stability limit of most liquid electrolytes is reached and new mechanisms, involving surface reactivity of the active material beside electrolyte decomposition, contribute to the interfacial reactivity and nature of the CEI. Focusing on lithium‐based cell chemistries, this review aims to highlight the impact of the still less understood electrolyte decomposition chemistry, dictated by the nature of its components, as well as the in‐depth research on the physicochemical and electrochemical properties of CEI formation and evolution at positive electrode material surface and sub‐surfaces.