Design Principles and Applications of Next‐Generation High‐Energy‐Density Batteries Based on Liquid Metals

Abstract

battery market. Thanks to the investigation of host materials that allow stable Li-ion intercalation, rechargeable Li-ion batteries (LIBs) are commercialized with stable cyclability and remarkable energy-density, which have been awarded with the 2019 Nobel Prize in Chemistry. [2,3] Whereas in the initial stage of electrode materials exploration, Li metal was the primary anode selection which offers the lowest reduction potential in the periodic table (3.045 V) and extremely high theoretical capacity (3840 mAh g -1 ) that is ten times higher than its commercialized graphite anode (≈370 mAh g -1 ). [4] One of the major reasons hindering Li metal application is the dendrite issue existing in metals during the electrochemical process, which is describing the protuberance growing from the metal surface at electrode-electrolyte interface resulting in the ramified morphology. [5][6][7] The elongated dendrite tips could penetrate the separator membrane, causing the internal shorts, thermal runaway, and the successive safety issues. [8,9] Besides the dendrite issue, other interfacial issues also impede the commercialization of Li metal anodes, such as the dead lithium which leads to the decay of anode capacity, as well as the unstable solid-electrolyte interface (SEI) causing the continuous decomposition of electrolyte or inefficient charge transport. [10,11] With the troublesome interfacial issues unsolved, the Li resource is already over consumed, for which the demand is estimated to soon surpass the supply in near future unless being efficiently managed and recycled. [12,13] Elements that are more abundant than Li have been proposed as battery materials in these years, among which the Na and K alkali metals are popular selections for their comparably low standard reduction potential (Na −2.714 V, K −2.925 V), promising high battery energy and fast charge transport kinetics allowing the high battery power. [4,[14][15][16][17][18] Whereas these metals also cannot avoid the severe dendrite issue as existing in the Li metal anodes.The investigation of high temperature liquid metal batteries (HTLMBs) initiated since 1900s, which later became actively studied in the 1960s by the national labs and industries and then revived at MIT in 2000s. [19,20] A typical design of the HTLMB normally involves a self-segregated tri-layer structure with two types of molten metals or alloys as electrodes and a molten salt as the electrolyte. Although these designs could achieve remarkably high battery capacity, to maintain sufficiently high temperature for stable operation, such a design requires extra energy input, and could lead to the limited energy density and further issues such as relatively low battery voltage and high Increasing need for the renewable energy supply accelerated the thriving studies of Li-ion batteries, whereas if the high-energy-density Li as well as alkali metals should be adopted as battery electrodes is still under fierce debate for safety concerns. Recently, a group of low-melting temperature metals and alloys tha...

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