Gilbertbengtsson8620

This review provides an overview of the chemistry developed with all classes of specially activated carbon π-systems by discussing their general and specific reactivities, presenting and commenting on their gold-catalyzed transformations as well as their applications.Direct harvesting of electricity from photosynthesis is highly desired as an eco-friendly and sustainable energy harvesting technology. Photosynthetic apparatuses isolated from plants, such as thylakoid membranes (TMs), are deposited on an electrode by which photosynthetic electrons (PEs) are collected from water splitting. To enhance PE collection efficiency, it is critical to increase the electrochemical interfaces between TMs and the electrode. Considering the size of TMs to be around a few hundred nanometer, we hypothesize that an array of micropillar-shaped (MP) electrode can maximize the TM/electrode interface area. Thus, we developed MP electrodes with different heights and investigated the electrospraying of TM-alginate mixtures to fill the gaps between MPs uniformly and conformally. #link# The uniformity of the TM-alginate film and the interaction between the TM and the MP electrode were evaluated to understand how the MP heights and film quality influenced the magnitude of the PE currents. PE currents increased up to 2.4 times for an MP electrode with an A/R of 1.8 compared to a flat electrode, indicating increased direct contact interface between TMs and the electrode. Furthermore, to demonstrate the scalability of this approach, an array of replicated SU-8 MP electrodes was prepared and PE currents of up to 3.2 μA were monitored without a mediator under 68 mW/cm2. Finally, the PE current harvesting was sustained for 14 days without decay, demonstrating the long-term stability of the TM-alginate biophotoanodes.Recombination can be used in the laboratory to overcome component limitations in synthetic biology by creating enzymes that exhibit distinct activities and stabilities from native proteins. To investigate how recombination affects the properties of an oxidoreductase that transfers electrons in cells, we created ferredoxin (Fd) chimeras by recombining distantly related cyanobacterial and cyanomyophage Fds (53% identity) that present similar midpoint potentials but distinct thermostabilities. Fd chimeras having a wide range of amino acid substitutions retained the ability to coordinate an iron-sulfur cluster, although their thermostabilities varied with the fraction of residues inherited from each parent. The midpoint potentials of chimeric Fds also varied. However, all of the synthetic Fds exhibited midpoint potentials outside of the parental protein range. link2 Each of the chimeric Fds could also support electron transfer between Fd-NADP reductase and sulfite reductase in Escherichia coli, although the chimeric Fds varied in the expression required for similar levels of cellular electron transfer. These results show how Fds can be diversified through recombination and reveal differences in the inheritance of thermostability and electrochemical properties. Furthermore, they illustrate how electron transfer efficiencies of chimeric Fds can be rapidly evaluated using a synthetic metabolic pathway.Bismuth-based (nano)materials have been attracting increasing interest due to appealing properties such as high refractive indexes, intrinsic opacity, and structural distortions due to the stereochemistry of 6s2 lone pair electrons of Bi3+. However, the control over specific phases and strategies able to stabilize uniform bismuth-based (nano)materials is still a challenge. In this study, we employed the ability of bismuth to lower the melting point of silica to introduce a new synthetic approach able to confine the growth of bismuth-oxide-based materials into nanostructures. Combining in situ temperature-dependent synchrotron radiation X-ray powder diffraction (XRPD) with high-resolution transmission electron microscopy (HR-TEM) analyses, we demonstrate the evolution of a confined Bi2O3-SiO2 nanosystem from Bi2SiO5 to Bi4Si3O12 through a melting process. The silica shell acts as both a nanoreactor and a silicon source for the stabilization of bismuth silicate glass-ceramic nanocrystals keeping the original spherical shape. link3 The exciton peak of Bi2SiO5 is measured for the first time allowing the estimation of its real energy gap. Moreover, based on a detailed spectroscopic investigation, we discuss the potential and the limitations of Nd3+-activated bismuth silicate systems as ratiometric thermometers. The synthetic strategy introduced here could be further explored to stabilize other bismuth-oxide-based materials, opening the way toward the growth of well-defined glass-ceramic nanoparticles.The various bioactivity types and potencies of peptidic natural products (PNPs) are of high interest for the development of new drugs. In particular, the intrinsic antibiotic properties of PNPs appear essential to combat antimicrobial resistance that is currently threatening the world. The first steps in dereplication and characterization of PNPs often involve tandem mass spectrometry (MS/MS). However, such structurally complex peptides challenge the interpretation of MS/MS results. Only a few software solutions are dedicated to PNP analysis but with a mutually exclusive focus on dereplication or annotation. Hence, key functionalities such as automatic peak annotation or statistically validated scoring systems to support the characterization/identification processes are missing. Here, we present NRPro, a new MS/MS analysis platform that overcomes some limitations of the existing software and provides a comprehensive toolset for both automatic annotation and dereplication of PNPs.Lithium-ion batteries (LIBs) with high-nickel (Ni) content LiNi x Mn y Co z O2 (x + y + z = 1) (NMC with Ni ≥ 0.6) cathodes operated at high charge voltages have been considered as one of the most promising candidates for addressing the challenge of increasing energy density demand. Conventional LiPF6-organocarbonate electrolytes exhibit incompatibility with such cell chemistries under certain testing conditions because of the instability of electrode/electrolyte interphases. In response to this challenge, ether-based electrolytes with finely tuned structure and composition of solvation sheaths were developed and evaluated in graphite (Gr)∥NMC811 cell chemistry in 2.5-4.4 V, despite ethers being conventionally considered to be unfavorable electrolyte solvents for LIBs because of their anodic instability above 4.0 V and cointercalation into Gr electrodes. The functional ether-based electrolytes in this work enable both excellent cycle life and high rate capability of Gr∥NMC811 cells. Mechanistic studies reveal that the unique structure and composition of the solvation sheath of the functional ether electrolytes are the main reasons behind their excellent anodic stability and effective protection of the Gr electrode and, consequently, the extraordinary cell performances when operated at high charge cutoff voltages. This work also provides a feasible approach in developing highly stable functional electrolytes for high-energy density LIBs.Potassium-ion capacitors (KICs) have received a surge of interest because of their higher reserves and lower costs of potassium than lithium. However, the cycle performance and capacity of potassium devices have been reported to be unsatisfactory. Herein, a unique crystalline MnCo2O4.5 and amorphous MnCo2S4 core/shell nanoscale flower structure grown on graphene (MCO@MCS@rGO) was synthesized by a two-step hydrothermal process and demonstrated in KICs. The MCO@MCS@rGO exhibits improved electrical conductivity and excellent structural integrity during the charging and discharging process. The reasons could be attributed to the cavity structure of MCO, the mechanical buffer and high electrolyte diffusion rate of MCS, and the auxiliary effect of graphene. The electrical conductivity of MCO@MCS shows a specific capacity of 272.3 mA h g-1 after 400 cycles at 1 A g-1 and a capacity of 125.6 mA h g-1 at 2 A g-1. Besides, Varespladib price @MCS@rGO and high-surface-area activated carbon in KICs exhibit a relative energy density of 85.3 W h kg-1 and a power density of 9000 W kg-1 and outstanding cycling stability with a capacity retention of 76.6% after 5000 cycles. Moreover, the reaction mechanism of MCO@MCS@rGO in the K-ion cell was investigated systematically using X-ray diffraction and transmission electron microscopy, providing guidance on the further development of pseudocapacitive materials.Plasmonics has emerged as a promising methodology to promote chemical reactions and has become a field of intense research effort. Ag nanoparticles (NPs) as plasmonic catalysts have been extensively studied because of their remarkable optical properties. This review analyzes the emergence and development of localized surface plasmon resonance (LSPR) in organic chemistry, mainly focusing on the discovery of novel reactions with new mechanisms on Ag NPs. Initially, the basics of LSPR and LSPR-promoted photocatalytic mechanisms are illustrated. Then, the recent advances in plasmonic nanosilver-mediated photocatalysis in organic transformations are highlighted with an emphasis on the related reaction mechanisms. Finally, a proper perspective on the remaining challenges and future directions in the field of LSPR-promoted organic transformations is proposed.It is still a big challenge to simultaneously enhance the ionic conductivity, dendrite suppression capability, and interfacial compatibility of sulfide solid electrolytes. In this work, a novel Li7P2.88Nb0.12S10.7O0.3 solid electrolyte is prepared via Nb and O cosubstitution of glass-ceramic Li7P3S11. This sulfide-based electrolyte possesses a high ionic conductivity (3.59 mS cm-1) at 298 K, improved critical current density (1.16 mA cm-2), and excellent interfacial compatibility between the sulfide electrolyte and Li2S active material. The improved electrochemical stability of the sulfide solid electrolyte against metallic lithium is attributed to the formation of Nb and Li2O at the interface, which can induce uniform Li deposition and prevent further side reaction. The all-solid-state Li/Li2S batteries based on this electrolyte exhibit remarkably enhanced cycling stability and rate performance.Metal halide perovskites are promising contenders for next-generation photovoltaic applications due to their remarkable photovoltaic efficiency and their compatibility with solution-processed fabrication. Among the various strategies to control the crystallinity and the morphology of the perovskite active layer and its interfaces with the transport layers, fabrication of perovskite solar cells from precursor solutions with a slight excess of PbI2 has become very common. Despite this, the role of such excess PbI2 is still rather controversial, lacking consensus on its effect on the bulk and interface properties of the perovskite layer. In this work, we investigate the effect of removing the excess PbI2 from the surface of a triple-cation mixed-halide Cs0.05(FA0.83MA0.17)0.95Pb(I0.83Br0.17)3 perovskite layer by four different organic salts on their photovoltaic performance and stability. We show that treatments with iodide salts such as methylammonium iodide (MAI) and formamidinium iodide (FAI) can lead to the strongest beneficial effects on solar cell efficiency, charge recombination suppression, and stability while non-iodide salts such as methylammonium bromide (MABr) and methylammonium chloride (MACl) can also provide improvement in terms of charge recombination suppression and stability to a moderate extent in comparison to the untreated sample.