Structural Evolution of Electrochemically Lithiated MoS2_{2} Nanosheets and the Role of Carbon Additive in Li-Ion Batteries

Understanding the structure and phase changes associated with conversion-type materials is key to optimizing their electrochemical performance in Li-ion batteries. For example, molybdenum disulfide (MoS$_{2}$) offers a capacity up to 3-fold higher (∼1 Ah/g) than the currently used graphite anodes, but they suffer from limited Coulombic efficiency and capacity fading. The lack of insights into the structural dynamics induced by electrochemical conversion of MoS$_{2}$ still hampers its implementation in high energy-density batteries. Here, by combining $\textit{ab initio}$ density-functional theory (DFT) simulation with electrochemical analysis, we found new sulfur-enriched intermediates that progressively insulate MoS$_{2}$ electrodes and cause instability from the first discharge cycle. Because of this, the choice of conductive additives is critical for the battery performance. We investigate the mechanistic role of carbon additive by comparing equal loading of standard Super P carbon powder and carbon nanotubes (CNTs). The latter offer a nearly 2-fold increase in capacity and a 45% reduction in resistance along with Coulombic efficiency of over 90%. These insights into the phase changes during MoS$_{2}$ conversion reactions and stabilization methods provide new solutions for implementing cost-effective metal sulfide electrodes, including Li-S systems in high energy-density batteries.C.G and M.D.V acknowledge the support from ERC starting grant 337739-HIENA. A.J.M. acknowledges the support from the Winton Programme for the Physics of Sustainability. Computational resources were provided by the Cambridge High Performance Computing service. M.H.M acknowledges the support from EPSRC Cambridge NanoDTC, EP/G037221/1

Dominant mutations of the Notch ligand Jagged1 cause peripheral neuropathy

Notch signaling is a highly conserved intercellular pathway with tightly regulated and pleiotropic roles in normal tissue development and homeostasis. Dysregulated Notch signaling has also been implicated in human disease, including multiple forms of cancer, and represents an emerging therapeutic target. Successful development of such therapeutics requires a detailed understanding of potential on-target toxicities. Here, we identify autosomal dominant mutations of the canonical Notch ligand Jagged1 (or JAG1) as a cause of peripheral nerve disease in 2 unrelated families with the hereditary axonal neuropathy Charcot-Marie-Tooth disease type 2 (CMT2). Affected individuals in both families exhibited severe vocal fold paresis, a rare feature of peripheral nerve disease that can be life-threatening. Our studies of mutant protein posttranslational modification and localization indicated that the mutations (p.Ser577Arg, p.Ser650Pro) impair protein glycosylation and reduce JAG1 cell surface expression. Mice harboring heterozygous CMT2-associated mutations exhibited mild peripheral neuropathy, and homozygous expression resulted in embryonic lethality by midgestation. Together, our findings highlight a critical role for JAG1 in maintaining peripheral nerve integrity, particularly in the recurrent laryngeal nerve, and provide a basis for the evaluation of peripheral neuropathy as part of the clinical development of Notch pathway–modulating therapeutics

Evolution of Reduced Graphene Oxide-SnS<inf>2</inf> Hybrid Nanoparticle Electrodes in Li-Ion Batteries

Hybrid nanomaterials where active battery nanoparticles are synthesized directly onto conductive additives such as graphene hold the promise of improving the cyclability and energy density of conversion and alloying type Li-ion battery electrodes. Here we investigate the evolution of hybrid reduced graphene oxide–tin sulfide (rGO-SnS2) electrodes during battery cycling. These hybrid nanoparticles are synthesized by a one-step solvothermal microwave reaction which allows for simultaneous synthesis of the SnS2 nanocrystals and reduction of GO. Despite the hybrid architecture of these electrodes, electrochemical impedance spectroscopy shows that the impedance doubles in about 25 cycles and subsequently gradually increases, which may be caused by an irreversible surface passivation of rGO by sulfur enriched conversion products. This surface passivation is further confirmed by post-mortem Raman spectroscopy of the electrodes, which no longer detects rGO peaks after 100 cycles. Moreover, galvanostatic intermittent titration analysis during the 1st and 100th cycles shows a drop in Li-ion diffusion coefficient of over an order of magnitude. Despite reports of excellent cycling performance of hybrid nanomaterials, our work indicates that in certain electrode systems, it is still critical to further address passivation and charge transport issues between the active phase and the conductive additive in order to retain high energy density and cycling performance.M.H.M acknowledges the support from EPSRC Cambridge NanoDTC, EP/G037221/1. C.G and M.D.V acknowledge the support from ERC starting grant HIENA-337739

Self-Assembly of rGO Coated Nanorods into Aligned Thick Films

© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Self-assembly is a very effective and popular method to create monolayers or thin films of aligned nanorods and ellipsoids. Nevertheless, there has been little attention to forming thick films of aligned nanorods using this approach. Here, the self-assembly mechanism of nanorods coated with reduced graphene oxide in thick films with both a surface and a bulk alignment process is underpinned. The alignment method is robust and results in films with up to 50% higher volumetric density compared to nonaligned films of the same material. To optimize the coating process, an image processing script is implemented that quantifies the quality of the alignment based on a fast Fourier transform of nanorod electron microscope images. Based on this analysis, parameters are identified that influence the alignment to optimize the process for obtaining large area domains. Finally, dip-coating, blade casting and zone coating are tested and compared and lithographically patterned substrates are used to template the self-assembly process

Triple-Cation-Based Perovskite Photocathodes with AZO Protective Layer for Hydrogen Production Applications

Metal halide perovskites are actively pursued as photoelectrodes to drive solar fuel synthesis. However, currently, these photocathodes suffer from limited stability in water, which hampers their practical application. Here, we report a high-performance solution-processable photocathode composed of cesium formamidinium methylammonium triple-cation lead halide perovskite protected by an Al-doped ZnO (AZO) layer combined with a Field's metal encapsulation. Careful selection of charge transport layers resulted in an improvement in photocurrent, fill factor, device stability and reproducibility. The dead pixels count reduced from 25 to 6% for the devices with an AZO layer, and in photocathodes with an AZO layer the photocurrent density increased by almost 20% to 14.3 mA cm-2. In addition, we observed a 5-fold increase in the device lifetime for photocathodes with AZO, which reached up to 18 h before complete failure. Finally, the photocathodes are fabricated using low-cost and scalable methods, which have promise to become compatible with standard solution-based processes