Ballnoel7982

Finally, we established a mass spectrometric method for quantifying the incorporated artificial nucleotide and obtained a linear relationship with the amount of O6-carboxymethyl-guanine in the target sequence. In this work, we present a strategy to identify, locate, and quantify a mutagenic DNA adduct, advancing tools for linking DNA alkylation to mutagenesis and for detecting DNA adducts in genes as potential diagnostic biomarkers for cancer prevention.Creating high-density durable bifunctional active sites in an air electrode is essential but still challenging for a long-life rechargeable zinc-air battery with appealing power density. Herein, we discover a general strategy mediated by metastable rock salt oxides for achieving high-density well-defined transition-metal nanocrystals encapsulated in N-doped carbon shells (M@NC) which are anchored on a substrate by a porous carbon network as highly active and durable bifunctional catalytic sites. Small-size (15 ± 5 nm) well-dispersed Co2Fe1@NC in a high density (metal loading up to 54.0 wt %) offers the zinc-air battery a record power density of 423.7 mW cm-2. The dual protection from the complete graphitic carbon shells and the anchoring of the outer carbon network make Co2Fe1@NC chemically and mechanically durable, giving the battery a long cycling life. Systematic in-situ temperature-dependent characterizations as well as DFT modeling rationalize the rock salt oxide-mediated process and its indispensable role in achieving high-density nanosized M@NC. These findings open up opportunities for designing efficient electrocatalysts for high-performance Zn-air batteries and diverse energy devices.A high-consequence chemical emergency is a major public health concern. In the United States, the National Institute of Allergy and Infectious Diseases within the National Institutes of Health pioneers discovery and early development of critical medical countermeasures against chemical threats.Polypeptide micelles are widely used as biocompatible nano-platforms, but often suffer from their poor structural stability. Unimolecular polypeptide micelles can effectively address the structure instability issue, but their synthesis with uniform struc-ture, well controlled and desired sizes remains challenging. Herein, we report the convenient preparation of spherical unimolecular micelles through dendritic polyamine-initiated ultrafast ring-opening polymerization of N-carboxyanhydride (NCA). DTNB chemical structure Synthetic polypeptides with exceptionally high MWs (up to 85 MDa) and low dispersity (Ð less then 1.05) can be readily obtained, which are the biggest synthetic polypeptides ever reported. The degree of polymerization was controlled in a vast range (25 - 3200), giving access to nearly monodisperse unimolecular micelles with predict-able sizes. Many NCA monomers can be polymerized using this ultrafast polymerization method, which enables the incorporation of various structural and functional moieties to the unimolecular micelles. Given the simplicity of the synthesis and superior con-trol over the structure, the unimolecular polypeptide micelles may find applications in nanomedicine, supermolecular chemistry and bio-nanotechnology.Spin-phonon coupling plays a critical role in magnetic relaxation in single-molecule magnets (SMMs) and molecular qubits. Yet, few studies of its nature have been conducted. Phonons here refer to both intermolecular and intramolecular vibrations. In the current work, we show spin-phonon couplings between IR-active phonons in a lanthanide molecular complex and Kramers doublets (from the crystal field). For the SMM Er[N(SiMe3)2]3 (1, Me = methyl), the couplings are observed in the far-IR magnetospectroscopy (FIRMS) of crystals with coupling constants ≈ 2-3 cm-1. In particular, one of the magnetic excitations couples to at least two phonon excitations. The FIRMS reveals at least three magnetic excitations (within the 4I15/2 ground state/manifold; hereafter, manifold) at 0 T at 104, ∼180, and 245 cm-1, corresponding to transitions from the ground state, MJ = ±15/2, to the first three excited states, MJ = ±13/2, ±11/2, and ±9/2, respectively. The transition between the ground and first excited Kramers doublet in 1 is also observed in inelastic neutron scattering (INS) spectroscopy, moving to a higher energy with an increasing magnetic field. INS also gives complete phonon spectra of 1. Periodic DFT computations provide the energies of all phonon excitations, which compare well with the spectra from INS, supporting the assignment of the inter-Kramers doublet (magnetic) transitions in the spectra. The current studies unveil and measure the spin-phonon couplings in a typical lanthanide complex and throw light on the origin of the spin-phonon entanglement.The in situ on-surface conversion process from boroxine-linked covalent organic frameworks (COFs) to boronate ester-linked COFs is triggered and catalyzed at room temperature by an electric field and monitored with scanning tunneling microscopy (STM). The adaptive behavior within the generated dynamic covalent libraries (DCLs) was revealed, providing in-depth understanding of the dynamic network switching process.The complex Ru-MACHO has been previously shown to undergo uncontrolled degradation subsequent to base-induced dehydrochlorination in the absence of a substrate. In this study, we report that stabilization of the dehydrochlorinated Ru-MACHO with phosphines furnishes complexes whose structures depend on the phosphines employed while PMe3 led to the expected octahedral RuII complex, PPh3 provided access to a trigonal-bipyramidal Ru0 complex. Because both complexes proved to be active in base-free (de)hydrogenation reactions, thorough quantum-chemical calculations were employed to understand the reaction mechanism. The calculations show that both complexes lead to the same mechanistic scenario after phosphine dissociation and, therefore, only differ energetically in this step. According to the calculations, the typically proposed metal-ligand cooperation mechanism is not the most viable pathway. Instead, a metal-ligand-assisted pathway is preferred. Finally, experiments show that phosphine addition enhances the catalyst's performance in comparison to the PR3-free "activated" Ru-MACHO.