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1.
2.
Polymers such as poly(ethylene glycol) (PEG) have proven use in a variety of applications including organic synthesis. We now disclose our investigations into the recently disputed report that PEG tartrate esters can reverse the enantioselectivity of the Sharpless asymmetric epoxidation reaction. The results presented herein have clarified that the enantioselectivity of this reaction can be reproducibly reversed solely as a function of the molecular weight of the appended PEG. By preparing a range of tartrate ligands with varying PEG chains lengths, the reversal was found to occur within a molecular weight change of only 800. As the PEG chain did not affect the inherent chirality of the ligand, the enantioreversal was proposed to occur as a result of two Ti-ligand complexes which differ in their molecularity of ligand, one monomeric in ligand and the other dimeric. Support for this hypothesis was given through equilibrium measurements which revealed that the predominant species in Ti/PEG tartrate ester mixtures is a distinct 2:1 Ti-ligand complex, as opposed to the 2:2 Ti-ligand complex of traditional Sharpless asymmetric epoxidations. In total, these data represent an unrecognized property of PEG-supported catalysts that could open up new venues in the control of asymmetric reactions by means of achiral appended polymers. 相似文献
3.
Retrobiosynthetic analysis of the allergenic sesquiterpene lactone, anthecotuloide, suggested that this natural product could be formed either by head to head condensation of geranyl diphosphate with dimethylallyl diphosphate, or from farnesyl diphosphate (FPP), the accepted regular sesquiterpene precursor via the rearrangement of a germacranolide precursor. Isotopic labelling of anthecotuloide has now been achieved by feeding [1-(13)C]-glucose, [U-13C6]-glucose and [6,6-(2)H2]-glucose to aseptically grown plantlets of Anthemis cotula(family Asteraceae). Analysis of labelling patterns and absolute 13C abundances using quantitative 13C NMR spectroscopy showed that the isoprene building blocks of this sesquiterpene are formed exclusively via the MEP terpene biosynthetic pathway. This was supported by results from an experiment using [U-13C6]-glucose. A deuterium labelling experiment using [6,6-(2)H2]-glucose supported the original proposal and showed that anthecotuloide is formed from a non FPP precursor. Isotope ratio mass spectrometry suggested that there were two pathways for sesquiterpene biosynthesis in A. cotula. 相似文献
4.
Dickerson CA Fisher MJ Sykora RE Albrecht-Schmitt TE Cody JA 《Inorganic chemistry》2002,41(4):640-642
The compound K(3)PSe(4).2Se(6) was synthesized at 110 degrees C via solventothermal techniques from binary starting materials and Se in acetonitrile. The compound crystallizes in the space group Fd macro 3 of the cubic system with eight formula units in a cell with a dimension of a = 16.415(2) A at T = 193 K. The structure contains an unusual intermixing of ionic and uncharged species. The selenophosphate tetrahedral trianions PSe(4)(3-) are surrounded by potassium cations; other potassium cations in the structure are coordinated to 12 selenium atoms from four Se(6) rings in a tetrahedral arrangement. There are no short contacts between adjacent selenium rings. Heating the same reaction mixture to 160 degrees C results in the formation of only needles of trigonal selenium. 相似文献
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Matheus Dorneles de Mello Gaurav Kumar Tarnuma Tabassum Sheetal K. Jain Tso‐Hsuan Chen Stavros Caratzoulas Xinyu Li Dionisios G. Vlachos Songi‐I Han Susannah L. Scott Paul Dauenhauer Michael Tsapatsis 《Angewandte Chemie (International ed. in English)》2020,59(32):13260-13266
Phosphorus‐modified all‐silica zeolites exhibit activity and selectivity in certain Brønsted acid catalyzed reactions for biomass conversion. In an effort to achieve similar performance with catalysts having well‐defined sites, we report the incorporation of Brønsted acidity to metal–organic frameworks with the UiO‐66 topology, achieved by attaching phosphonic acid to the 1,4‐benzenedicarboxylate ligand and using it to form UiO‐66‐PO3H2 by post‐synthesis modification. Characterization reveals that UiO‐66‐PO3H2 retains stability similar to UiO‐66, and exhibits weak Brønsted acidity, as demonstrated by titrations, alcohol dehydration, and dehydra‐decyclization of 2‐methyltetrahydrofuran (2‐MTHF). For the later reaction, the reported catalyst exhibits site‐time yields and selectivity approaching that of phosphoric acid on all‐silica zeolites. Using solid‐state NMR and deprotonation energy calculations, the chemical environments of P and the corresponding acidities are determined. 相似文献
7.
Skidmore MA Patey SJ Thanh NT Fernig DG Turnbull JE Yates EA 《Chemical communications (Cambridge, England)》2004,(23):2700-2701
Glycosaminoglycan oligosaccharides have been attached to thiol-derivatised gold surfaces, via the formation of mercury-sugar adducts at the non-reducing end, representing a new method of generating versatile glycoconjugates incorporating this class of biologically and medically important carbohydrate. 相似文献
8.
Dickerson MB Naik RR Stone MO Cai Y Sandhage KH 《Chemical communications (Cambridge, England)》2004,(15):1776-1777
Peptides that promote the rapid, room-temperature precipitation of amorphous germania nanoparticle networks from solution have been identified via use of a combinatorial peptide display library. 相似文献
9.
Brandon J. O'Neill David H. K. Jackson Dr. Anthony J. Crisci Carrie A. Farberow Fengyuan Shi Dr. Ana C. Alba‐Rubio Dr. Junling Lu Dr. Paul J. Dietrich Dr. Xiangkui Gu Dr. Christopher L. Marshall Prof. Peter C. Stair Dr. Jeffrey W. Elam Dr. Jeffrey T. Miller Prof. Fabio H. Ribeiro Prof. Paul M. Voyles Prof. Jeffrey Greeley Prof. Manos Mavrikakis Prof. Susannah L. Scott Prof. Thomas F. Kuech Prof. James A. Dumesic 《Angewandte Chemie (International ed. in English)》2013,52(51):13824-13824
10.
We have coupled CIEF with an LIF detector that is based on a post‐column sheath flow cuvette. We employed Chromeo P503 as a fluorogenic reagent to label proteins before analysis. This reagent reacts with the ε‐amine of lysine residues, preserving the cationic nature of the residue; labeled proteins generate extremely sharp peaks in CIEF. A set of four standard proteins generated a linear relationship between migration time and pI. A protein homogenate prepared from a Barrett's esophagus cell line resolved over 100 components in a 40 min separation. Detection limits for Chromeo P503‐labeled β‐lactoglobulin were 5 amol injected into the capillary. Fluorescent impurities present in the ampholytes generated a large background signal that degraded the detection limit by four orders of magnitude compared with other forms of capillary electrophoresis with this detector. 相似文献