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The lithium‐sulfur battery is a compelling energy storage system because its high theoretical energy density exceeds Li‐ion batteries at much lower cost, but applications are thwarted by capacity decay caused by the polysulfide shuttle. Here, proof of concept and the critical metrics of a strategy to entrap polysulfides within the sulfur cathode by their reaction to form a surface‐bound active redox mediator are demonstrated. It is shown through a combination of surface spectroscopy and cyclic voltammetry studies that only materials with redox potentials in a targeted window react with polysulfides to form active surface‐bound polythionate species. These species are directly correlated to superior Li‐S cell performance by electrochemical studies of high surface area oxide cathodes with redox potentials below, above, and within this window. Optimized Li‐S cells yield a very low fade rate of 0.048% per cycle. The insight gained into the fundamental surface mechanism and its correlation to the stability of the electrochemical cell provides a bridge between mechanistic understanding and battery performance essential for the design of high performance Li‐S cells.

A sulfur electrode exhibiting strong polysulfide chemisorption using a porous N, S dual-doped carbon is reported. The synergistic functionalization from the N and S heteroatoms dramatically modifies the electron density distribution and leads to much stronger polysulfide binding. X-ray photoelectron spectroscopy studies combined with ab initio calculations reveal strong Li(+) -N and Sn (2-) -S interactions. The sulfur electrodes exhibit an ultralow capacity fading of 0.052% per cycle over 1100 cycles.

Fuel-cooled thermal management, including endothermic cracking and reforming of hydrocarbon fuels, is an enabling technology for advanced aero engines and offers potential for cycle improvements and pollutant emissions control in gas turbine engine applications. The successful implementation of this technology is, however, predicated on the use of conventional multicomponent hydrocarbon fuels and an understanding of the combustion characteristics of the reformed fuel mixture. The objective of this research is to develop and demonstrate the technologies necessary for utilizing conventional multicomponent hydrocarbon fuels for fuel-cooled thermal management, including the development of the endothermic potential of JP-7 and JP-8+100, a demonstration of the combustion of supercritical/endothermic fuel mixtures, and conceptual design of a fuel-air heat exchanger. The ability to achieve high heat sinks with existing jet fuels (e.g., JP-7 and JP-8+100) was demonstrated with a bench-scale test rig operating under flow conditions and passage geometries simulative of practical heat exchangers for aircraft and missile applications. Key measurements included fuel heat sink, reaction products, and extent of conversion. Full-scale sector rig tests were conducted to characterize the combustion and emissions of supercritical jet fuel, and demonstrate the safety and operability of the fuel system, including a fuel-air heat exchanger.

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