Modification of Transition-Metal Redox by Interstitial Water in Hexacyanometalate Electrodes for Sodium-Ion Batteries.

A sodium-ion battery (SIB) solution is attractive for grid-scale electrical energy storage. Low-cost hexacyanometalate is a promising electrode material for SIBs because of its easy synthesis and open framework. Most hexacyanometalate-based SIBs work with aqueous electrolyte, and interstitial water in the material has been found to strongly affect the electrochemical profile, but the mechanism remains elusive. Here we provide a comparative study of the transition-metal redox in hexacyanometalate electrodes with and without interstitial water based on soft X-ray absorption spectroscopy and theoretical calculations. We found distinct transition-metal redox sequences in hydrated and anhydrated NaxMnFe(CN)6·zH2O. The Fe and Mn redox in hydrated electrodes are separated and are at different potentials, leading to two voltage plateaus. On the contrary, mixed Fe and Mn redox in the same potential range is found in the anhydrated system. This work reveals for the first time how transition-metal redox in batteries is strongly affected by interstitial molecules that are seemingly spectators. The results suggest a fundamental mechanism based on three competing factors that determine the transition-metal redox potentials. Because most hexacyanometalate electrodes contain water, this work directly reveals the mechanism of how interstitial molecules could define the electrochemical profile, especially for electrodes based on transition-metal redox with well-defined spin states

Rethinking Pseudo-LiDAR Representation

The recently proposed pseudo-LiDAR based 3D detectors greatly improve the benchmark of monocular/stereo 3D detection task. However, the underlying mechanism remains obscure to the research community. In this paper, we perform an in-depth investigation and observe that the efficacy of pseudo-LiDAR representation comes from the coordinate transformation, instead of data representation itself. Based on this observation, we design an image based CNN detector named Patch-Net, which is more generalized and can be instantiated as pseudo-LiDAR based 3D detectors. Moreover, the pseudo-LiDAR data in our PatchNet is organized as the image representation, which means existing 2D CNN designs can be easily utilized for extracting deep features from input data and boosting 3D detection performance. We conduct extensive experiments on the challenging KITTI dataset, where the proposed PatchNet outperforms all existing pseudo-LiDAR based counterparts. Code has been made available at: https://github.com/xinzhuma/patchnet.Comment: ECCV2020. Supplemental Material attache

Effect of simulated acid rain on CO₂, CH₄ and N₂O fluxes and rice productivity in a subtropical Chinese paddy field

The need of more food production, an increase in acidic deposition and the large capacity of paddy to emit greenhouse gases all coincide in several areas of China. Studying the effects of acid rain on the emission of greenhouse gases and the productivity of rice paddies are thus important, because these effects are currently unknown. We conducted a field experiment for two rice croppings (early and late paddies independent experiment) to determine the effects of simulated acid rain (control, normal rain, and treatments with rain at pH of 4.5, 3.5 and 2.5) on the fluxes of CO₂, CH₄ and N₂O and on rice productivity in subtropical China. Total CO₂ fluxes at pHs of 4.5, 3.5 and 2.5 were 10.3, 9.7 and 3.2% lower in the early paddy and 28.3, 14.8 and 6.8% lower in the late paddy, respectively, than the control. These differences from the control were significant for pH 3.5 and 4.5. Total CH₄ fluxes at pHs of 4.5, 3.5 and 2.5 were 50.4, 32.9 and 25.2% lower in the early paddy, respectively, than the control. pH had no significant effect on CH₄ flux in the late paddy or for total (early + late) emissions. N₂O flux was significantly higher at pH 2.5 than 3.5 and 4.5 but did not differ significantly from the flux in the control. Global-warming potentials (GWPs) were lower than the control at pH 3.5 and 4.5 but not 2.5, whereas rice yield was not appreciably affected by pH. Acid rain (between 3.5 and 4.5) may thus significantly affect greenhouse gases emissions by altering soil properties such as pH and nutrient pools, whereas highly acidic rain (pH 2.5) could increase GWPs (but not significantly), probably partially due to an increase in the production of plant litter

Dissociate lattice oxygen redox reactions from capacity and voltage drops of battery electrodes.

The oxygen redox (OR) activity is conventionally considered detrimental to the stability and kinetics of batteries. However, OR reactions are often confused by irreversible oxygen oxidation. Here, based on high-efficiency mapping of resonant inelastic x-ray scattering of both the transition metal and oxygen, we distinguish the lattice OR in Na0.6[Li0.2Mn0.8]O2 and compare it with Na2/3[Mg1/3Mn2/3]O2. Both systems display strong lattice OR activities but with distinct electrochemical stability. The comparison shows that the substantial capacity drop in Na0.6[Li0.2Mn0.8]O2 stems from non-lattice oxygen oxidations, and its voltage decay from an increasing Mn redox contribution upon cycling, contrasting those in Na2/3[Mg1/3Mn2/3]O2. We conclude that lattice OR is not the ringleader of the stability issue. Instead, irreversible oxygen oxidation and the changing cationic reactions lead to the capacity and voltage fade. We argue that lattice OR and other oxygen activities should/could be studied and treated separately to achieve viable OR-based electrodes