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91.
We report the synthesis of monomers for atom-transfer radical polymerization (ATRP) and a reversible addition-fragmentation chain transfer (RAFT) agent bearing trifluoroborate iminiums (TIMs), which are quantitatively converted into potassium acyltrifluoroborates (KATs) after polymerization. The resulting KAT-containing polymers are suitable for rapid amide-forming ligations for both post-polymerization modification and polymer conjugation. The polymer conjugation occurs rapidly, even under dilute (micromolar) aqueous conditions at ambient temperatures, thereby enabling the synthesis of a variety of linear and star-shaped block copolymers. In addition, we applied post-polymerization modification to the covalent linking of a photocaged cyclic antibiotic (gramicidin S) to the side chains of the KAT-containing copolymer. Cellular assays revealed that the polymer–antibiotic conjugate is biocompatible and provides efficient light-controlled release of the antibiotic on demand.  相似文献   
92.

Background  

The aim of this study was to examine the relationship between chronic neuropathic pain after incomplete peripheral nerve lesion, chronic nociceptive pain due to osteoarthritis, and the excitability of the motor cortex assessed by transcranial magnetic stimulation (TMS). Hence in 26 patients with neuropathic pain resulting from an isolated incomplete lesion of the median or ulnar nerve (neuralgia), 20 patients with painful osteoarthritis of the hand, and 14 healthy control subjects, the excitability of the motor cortex was tested using paired-pulse TMS to assess intracortical inhibition and facilitation. These excitability parameters were compared between groups, and the relationship between excitability parameters and clinical parameters was examined.  相似文献   
93.
Dispatching rules are simple scheduling heuristics that are widely applied in industrial practice. Their popularity can be attributed to their ability to flexibly react to shop floor disruptions that are prevalent in many real-world manufacturing environments. However, it is a challenging and time-consuming task to design local, decentralised dispatching rules that result in a good global performance of a complex shop.An evolutionary algorithm is developed to generate job shop problem instances for which an examined dispatching rule fails to achieve a good solution due to a single suboptimal decision. These instances can be easily analysed to reveal limitations of that rule which helps with the design of better rules. The method is applied to a job shop problem from the literature, resulting in new best dispatching rules for the mean flow time measure.  相似文献   
94.
Forecasting enterprise-wide revenue is critical to many companies and presents several challenges and opportunities for significant business impact. This case study is based on model developments to address these challenges for forecasting in a large-scale retail company. Focused on multivariate revenue forecasting across collections of supermarkets and product categories, hierarchical dynamic models are natural: these are able to couple revenue streams in an integrated forecasting model, while allowing conditional decoupling to enable relevant and sensitive analysis together with scalable computation. Structured models exploit multi-scale modeling to cascade information on price and promotion activities as predictors relevant across categories and groups of stores. With a context-relevant focus on forecasting revenue 12 weeks ahead, the study highlights product categories that benefit from multi-scale information, defines insights into when, how, and why multivariate models improve forecast accuracy, and shows how cross-category dependencies can relate to promotion decisions in one category impacting others. Bayesian modeling developments underlying the case study are accessible in custom code for interested readers.  相似文献   
95.
The equations of motion for a conformal field theory in the presence of defect lines can be derived from an action that includes contributions from bibranes. For T-dual toroidal compactifications, they imply a direct relation between Poincaré line bundles and the action of T-duality on boundary conditions. We also exhibit a class of diagonal defects that induce a shift of the B-field. We finally study T-dualities for S1S1-fibrations in the example of the Wess–Zumino–Witten model on SU(2)SU(2) and lens spaces. Using standard techniques from D-branes, we derive from algebraic data in rational conformal field theories geometric structures familiar from Fourier–Mukai transformations.  相似文献   
96.
Constrained peptides are promising next-generation therapeutics. Peptide stapling is a particularly attractive technique to generate constrained macrocycles with improved biological activity and metabolic stability. We introduce a biocompatible two-component stapling approach based on the reagent 2,6-dicyanopyridine and a pseudo-cysteine amino acid. Stapling can proceed either directly on-resin during solid-phase synthesis or following isolation of the linear peptide. The stapling reaction is orthogonal to natural amino acid side chains and completes in aqueous solution at physiological pH, enabling its direct use in biochemical assays. We performed a small screening campaign of short peptides targeting the Zika virus protease NS2B-NS3, allowing the direct comparison of linear with in situ stapled peptides. A stapled screening hit showed over 28-fold stronger inhibition than its linear analogue, demonstrating the successful identification of constrained peptide inhibitors.

A synthetically straightforward and biocompatible peptide-stapling strategy that can be used directly in biochemical assays to identify constrained enzyme inhibitors.  相似文献   
97.
98.
The preparation and X‐ray analysis of the title compound, [Sn2Br4(CH3)4(C5H9NO)], are described. The compound contains two Sn atoms in the asymmetric unit, that complexed by N‐methyl­pyrrolidin‐2‐one being hexacoordinated (a), the other exhibiting pentacoordination (b). The most important features are three different Sn—Br bond lengths at both Sn atoms with the following values: (a) 2.5060 (9), 2.7152 (10) and 3.7118 (10) Å; (b) 2.5084 (10), 2.5279 (9) and 3.5841 (10) Å.  相似文献   
99.
In this article we report a femtosecond time-resolved transient absorption study of a neutral organic mixed-valence (MV) compound with the aim to gain insight into its charge-transfer dynamics upon optical excitation. The back-electron transfer was investigated in five different solvents, toluene, dibutyl ether, methyl-tert-butyl ether (MTBE), benzonitrile and n-hexane. In the pump step, the molecule was excited at 760 nm and 850 nm into the intervalence charge-transfer band. The resulting transients can be described by two time constant. We assign one time constant to the rearrangement of solvent molecules in the charge-transfer state and the second time constant to back-electron transfer to the electronic ground state. Back-electron transfer rates range from 1.5 × 1012 s−1 in benzonitrile through 8.3 × 1011 s−1 in MTBE, around 1.6 × 1011 s−1 in dibutylether and toluene and to 3.8 × 109 s−1 in n-hexane.  相似文献   
100.
By means of metal-atom ligand-vapor cocondensation (CC) hexa(eta1-arsenine)molybdenum (11) and hexa(eta1-arsenine)tungsten (12) have been prepared; in the molybdenum case, the sandwich complex bis(eta6-arsenine)molybdenum (10) has been isolated as the primary product. The structure of 12 follows from a single-crystal X-ray diffraction study. Based on the results of CC synthesis, chromium binds to arsenine in the eta6-mode exclusively, molybdenum features both options eta1 and eta6, and for tungsten only eta1 coordination is observed.  相似文献   
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