Design and Preparation of Materials for Advanced Electrochemical Storage

To meet the growing global demand for energy while preserving the environment, it is necessary to drastically reduce the world's dependence on non-renewable energy sources. At the core of this effort will be the ability to efficiently convert, store, transport and access energy in a variety of ways. Batteries for use in small consumer devices have saturated society; however, if they are ever to be useful in large-scale applications such as automotive transportation or grid-storage, they will require new materials with dramatically improved performance. Efforts must also focus on using Earth-abundant and nontoxic compounds so that whatever developments are made will not create new environmental problems. In this Account, we describe a general strategy for the design and development of new insertion electrode materials for Li(Na)-ion batteries that meet these requirements. We begin by reviewing the current state of the art of insertion electrodes and highlighting the intrinsic material properties of electrodes that must be re-engineered for extension to larger-scale applications. We then present a detailed discussion of the relevant criteria for the conceptual design and appropriate selection of new electrode chemical compositions. We describe how the open-circuit voltage of Li-ion batteries can be manipulated and optimized through structural and compositional tuning by exploiting differences in the electronegativity among possible electrode materials. We then discuss which modern synthetic techniques are most sustainable, allowing the creation of new materials via environmentally responsible reactions that minimize the use of energy and toxic solvents. Finally, we present a case study showing how we successfully employed these approaches to develop a large number of new, useful electrode materials within the recently discovered family of transition metal fluorosulfates. This family has attracted interest as a possible source of improved Li-ion batteries in larger scale applications and benefits from a relatively "green" synthesis.