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Reversible Chlorite/Chlorine Dioxide Anion Redox Couple for Low-Cost Energy Storage Merrill K. Chiang,1* Liang Su,1* Kailash Raman,1 Yet-Ming Chiang,1,2 and William H. Woodford1 1Form Energy Inc., Somerville, MA, USA 2Massachusetts Institute of Technology, Cambridge, MA, USA *Equal contributions Email correspondence to: wwoodford@formenergy.com ABSTRACT: The ClO2-/ClO2 electrochemical reaction is shown to be highly reversible in acidic, near- neutral, and alkaline electrolytes while using low-cost carbon electrodes. Its equilibrium potential (0.954 V vs SHE) is pH-independent and enables high aqueous cell voltages of 1.38-2.15 V when used as a positive electrode with negative electrodes such as Zn, Fe, or S. This anion redox couple may enable low-cost aqueous rechargeable batteries free of resource-constrained metals, here demonstrated in prototype Zn-NaClO2 full cells. The rapid reaction kinetics and stability of the ClO2 phase at low temperatures also suggests that chlorite-based batteries may be favorable for applications in cold environments. Cost-effective and scalable electrical energy storage is critically needed for decarbonization of the electricity system, the electrification of transportation, and decarbonization of industrial production.[1- 4] To first order, the cost of power generation ($/kW), and the duration (h) over which electric power is delivered determine the required installed cost of storage ($/kWh). For example, delivering electricity at cost parity with today’s natural gas power plants, about $2,000/kW, requires storage technology with installed cost of $20/kWh if multi-day storage (100h) is required, while a cost of $200/kWh is acceptable if the required storage duration is only 10h. Choosing amongst electrochemical storage technologies, these two use cases may be met, for example, by low-cost metal-air batteries such as iron-air [4,5] and Li-ion storage [1], respectively. Considering scalability, it is estimated that decarbonization of the global electricity system by midcentury will require as much as 100 TWh of storage to be deployed.[1,6] This creates challenges in terms of both the availability and the scaling of mining and extraction of critical metals such as Li, Co, Ni, V, or Sb, depending on the elemental requirements of the technology. For battery chemistries that do meet cost and scalability criteria, additional criteria such as energy efficiency (typically represented by coulombic and voltaic efficiency), durability (cycle and calendar life), operating temperature, and safety come into play. However, one size does not fit all; the ranked importance of criteria is unique to each application. There exists a continuing need for new redox couples for rechargeable batteries that can meet current and future needs. Here, we show that the aqueous chlorine dioxide/chlorite (ClO2/ClO2-) redox couple, not previously considered for energy storage, has high electrochemical reversibility on catalyst-free low-cost carbon electrodes. The high planetary abundance of chlorine, highest amongst halogens and greater than that of nitrogen,[7] makes it attractive as the basis for low-cost large-scale storage, and the chlorite ion in particular is widely available at low cost source from sodium chlorite (NaClO2). Furthermore, since oxidation to chlorine dioxide occurs at a standard electrode potential of 0.954V vs SHE, the ClO2/ClO2- couple is attractive as a positive electrode paired with a wide range of possible negative electrodes, amongst which low-cost candidates include Zn or Fe metal, or S in the form of dissolved polysulfide species. Table1 summarizes the theoretical equilibrium cell voltages of rechargeable batteries using 1PDF Image | Reversible Chlorite Chlorine Dioxide Anion Redox Storage
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