Faraday Discussions

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Metal-air batteries including Li-air, Na-air, Al-air, and Zn-air, have received significant scientific and technological interest for at least the last three decades. The interest stems primarily from the fact that the electrochemically active material (O2 ) in the cathode can in principle be harvested from the surroundings. In practice, however, parasitic reactions with reactive components other than oxygen in dry air passivate the anode, limit cycling stability of air-sensitive ( e.g. , Li, Na, Al) and electrolyte-sensitive ( e...

The demand for practical implementation of rechargeable lithium-oxygen batteries (LOBs) has grown owing to their extremely high theoretical energy density. However, the factors determining the performance of cell-level high energy density LOBs remain unclear. In this study, LOBs with a stacked-cell configuration were fabricated and their performance evaluated under different experimental conditions to clarify the unique degradation phenomenon under lean-electrolyte and high areal capacity conditions. First, the effect of the electrolyte amount against areal capacity ratio ( E / C ) on the battery performance was evaluated, revealing a complicated voltage profile for an LOB cell operated under high areal capacity conditions...

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The reaction mechanism underpinning the operation of K-O2 batteries, particularly the O2 reactions at the positive electrode, is still not completely understood. In this work, by combining in situ Raman spectroelectrochemistry and density functional theory calculations, we report on a fundamental study of K-O2 electrochemistry at a model interface of Au electrode/DMSO electrolyte. The key products and intermediates (O2 - , KO2 and K2 O2 ) are identified and their dependency on the electrode potential is revealed...

The full electrification of transportation will require batteries with both 3-5× higher energy densities and a lower cost than what is available in the market today. Energy densities of >1000 W h kg-1 will enable electrification of air transport and are among the very few technologies capable of achieving this energy density. Limetal -O2 or Limetal -air are theoretically able to achieve this energy density and are also capable of reducing the cost of batteries by replacing expensive supply chain constrained cathode materials with "free" air...

The effect of Group 1 alkali-metal cations (Na+ , K+ , and Cs+ ) on the oxygen reduction and evolution reactions (ORR and OER) using dimethyl sulfoxide (DMSO)-based electrolytes was investigated. Cyclic voltammetry (CV) utilising different Pt-electrode surfaces (polycrystalline Pt, Pt(111) and Pt(100)) was undertaken to investigate the influence of surface structure upon the ORR and OER. For K+ and Cs+ , negligible variation in the CV response (in contrast to Na+ ) was observed using Pt(111), Pt(100) and Pt(poly) electrodes, consistent with a weak surface-metal/superoxide complex interaction...

Lithium-oxygen batteries are promising but have many challenges. Unlike lithium-ion batteries, they are usually discharge-charge cycled with capacity cutoff instead of potential cutoff, which brings controversy. Additionally, which superoxide intermediate, the dissolved or the adsorbed superoxide, is more reactive and leads to cell premature death and unsatisfactory discharge capacity? These questions puzzle researchers and impede the development of lithium-oxygen batteries. Herein, on one hand, we tried to decouple the influence of discharging potential and discharging current density on the discharge products and side reactions...

The cathode of a lithium-oxygen battery (LOB) should be well designed to deliver high catalytic activity and long stability, and to provide sufficient space for accommodating the discharge product. Herein, a facile coprecipitation approach is employed to synthesize LaNi0.5 Co0.5 O3 (LNCO) perovskite oxide with a low annealing temperature. The assembled LOB exhibits superior electrochemical performance with a low charge overpotential of 0.03-0.05 V in the current density range of 0.1-0.5 mA cm-2 . The battery ran stably for 119 cycles at a high coulombic efficiency...

Singlet oxygen (1 O2 ) formation is now recognised as a key aspect of non-aqueous oxygen redox chemistry. For identifying 1 O2 , chemical trapping via 9,10-dimethylanthracene (DMA) to form the endoperoxide (DMA-O2 ) has become the main method due to its sensitivity, selectivity, and ease of use. While DMA has been shown to be selective for 1 O2 , rather than forming DMA-O2 with a wide variety of potentially reactive O-containing species, false positives might hypothetically be obtained in the presence of previously overlooked species...

A summary of the Faraday Discussion presented in this issue and a perspective on that discussion is presented. The work highlights the specific science contributions made and the key conclusions associated with those findings so that readers can identify papers that they would like to explore in more detail.

Lithium-metal solid-state batteries (LMSSBs) have garnered immense interest due to their potential to enhance safety and energy density compared to traditional Li-ion batteries. The anode-free approach to manufacturing Li-metal anodes could provide the additional benefit of reducing cost. However, a lack of understanding of the mechano-electrochemical behavior related to the cycling of in situ formed Li anodes remains a significant challenge. To bridge this knowledge gap, this work aims to understand the cycling behavior of in situ formed Li anodes on garnet Li7 La3 Zr2 O12 (LLZO) solid-electrolyte as a function of the depth of discharge (DOD)...

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Is this the dawn of iontronics? Iontronics underpins the notion of devices and ionic machines, whereby ion and water also act as information carriers. Thinking about iontronics gives a vision and a road map, with applications in the water-energy nexus.

A general theory of coupled ion-electron transfer (CIET) is presented, which unifies Marcus kinetics of electron transfer (ET) with Butler-Volmer kinetics of ion transfer (IT). In the limit of large reorganization energy, the theory predicts normal Marcus kinetics of "electron-coupled ion transfer" (ECIT). In the limit of large ion transfer energies, the theory predicts Butler-Volmer kinetics of "ion-coupled electron transfer" (ICET), where the charge transfer coefficient and exchange current are connected to microscopic properties of the electrode/electrolyte interface...

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