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31.
Arlanda Huffer Ben Jeffery Benjamin J. Waller Andreas A. Danopoulos 《Comptes Rendus Chimie》2013,16(6):557-565
A method for the synthesis and isolation of 1,1′-methylene-bis-(3-aryl-imidazol-2-ylidene) ligands, aryl = 2,6-diisopropyl-phenyl (DiPP), LDiPP, mesityl (mes), Lmes, is reported, which provides synthetically useful quantities of high purity. Derivatisation of LDiPP with chalcogenides gave the adducts LDiPPE2, E = S, Se, Te. Reaction of LDiPP with [Pd(tmeda)Me2], [Pt(μ-SMe2)Me2]2, [Ir(1,5-COD)(μ-Cl)]2/KPF6 and [NiBr2(dme)] gave [Pd(LDiPP)Me2] (1), [Pt(LDiPP)Me2] (2), [Ir(LDiPP)(1,5-COD)](PF6) (3) and [Ni(LDiPP)Br2] (4), respectively. The latter was reduced in the presence of CO to [Ni(LDiPP)(CO)2] (5). The structures of Lmes, LDiPPTe2, and 1–5 are also reported. 相似文献
32.
Preparation of Stereoregular Isotactic Poly(mandelic acid) through Organocatalytic Ring‐Opening Polymerization of a Cyclic O‐Carboxyanhydride
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Dr. Antoine Buchard Dr. David R. Carbery Prof. Matthew G. Davidson Dr. Petya K. Ivanova Dr. Ben J. Jeffery Dr. Gabriele I. Kociok‐Köhn Dr. John P. Lowe 《Angewandte Chemie (International ed. in English)》2014,53(50):13858-13861
Poly(mandelic acid) (PMA) is an aryl analogue of poly(lactic acid) (PLA) and a biodegradable analogue of polystyrene. The preparation of stereoregular PMA was realized using a pyridine/mandelic acid adduct (Py?MA) as an organocatalyst for the ring‐opening polymerization (ROP) of the cyclic O‐carboxyanhydride (manOCA). Polymers with a narrow polydispersity index and excellent molecular‐weight control were prepared at ambient temperature. These highly isotactic chiral polymers exhibit an enhancement of the glass‐transition temperature (Tg) of 15 °C compared to the racemic polymer, suggesting potential future application as high‐performance commodity and biomedical materials. 相似文献
33.
Dr. Jeffery M. Tharp Dr. Omer Ad Dr. Kazuaki Amikura Fred R. Ward Emma M. Garcia Prof. Dr. Jamie H. D. Cate Prof. Dr. Alanna Schepartz Prof. Dr. Dieter Söll 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(8):3146-3150
By transplanting identity elements into E. coli tRNAfMet, we have engineered an orthogonal initiator tRNA (itRNATy2) that is a substrate for Methanocaldococcus jannaschii TyrRS. We demonstrate that itRNATy2 can initiate translation in vivo with aromatic non-canonical amino acids (ncAAs) bearing diverse sidechains. Although the initial system suffered from low yields, deleting redundant copies of tRNAfMet from the genome afforded an E. coli strain in which the efficiency of non-canonical initiation equals elongation. With this improved system we produced a protein containing two distinct ncAAs at the first and second positions, an initial step towards producing completely unnatural polypeptides in vivo. This work provides a valuable tool to synthetic biology and demonstrates remarkable versatility of the E. coli translational machinery for initiation with ncAAs in vivo. 相似文献
34.
Fan Yang Wenhui Hu Chongqing Yang Margaret Patrick Andrew L. Cooksy Jian Zhang Jeffery A. Aguiar Chengcheng Fang Yinghua Zhou Ying Shirley Meng Jier Huang Jing Gu 《Angewandte Chemie (International ed. in English)》2020,59(11):4572-4580
A gas‐phase approach to form Zn coordination sites on metal–organic frameworks (MOFs) by vapor‐phase infiltration (VPI) was developed. Compared to Zn sites synthesized by the solution‐phase method, VPI samples revealed approximately 2.8 % internal strain. Faradaic efficiency towards conversion of CO2 to CO was enhanced by up to a factor of four, and the initial potential was positively shifted by 200–300 mV. Using element‐specific X‐ray absorption spectroscopy, the local coordination environment of the Zn center was determined to have square‐pyramidal geometry with four Zn?N bonds in the equatorial plane and one Zn‐OH2 bond in the axial plane. The fine‐tuned internal strain was further supported by monitoring changes in XRD and UV/Visible absorption spectra across a range of infiltration cycles. The ability to use internal strain to increase catalytic activity of MOFs suggests that applying this strategy will enhance intrinsic catalytic capabilities of a variety of porous materials. 相似文献
35.
Jeffery M. Tharp Omer Ad Kazuaki Amikura Fred R. Ward Emma M. Garcia Jamie H. D. Cate Alanna Schepartz Dieter Sll 《Angewandte Chemie (International ed. in English)》2020,59(8):3122-3126
By transplanting identity elements into E. coli tRNAfMet, we have engineered an orthogonal initiator tRNA (itRNATy2) that is a substrate for Methanocaldococcus jannaschii TyrRS. We demonstrate that itRNATy2 can initiate translation in vivo with aromatic non‐canonical amino acids (ncAAs) bearing diverse sidechains. Although the initial system suffered from low yields, deleting redundant copies of tRNAfMet from the genome afforded an E. coli strain in which the efficiency of non‐canonical initiation equals elongation. With this improved system we produced a protein containing two distinct ncAAs at the first and second positions, an initial step towards producing completely unnatural polypeptides in vivo. This work provides a valuable tool to synthetic biology and demonstrates remarkable versatility of the E. coli translational machinery for initiation with ncAAs in vivo. 相似文献
36.
37.
Dr. Louwanda Lakiss Dr. Aurélie Vicente Prof. Jean-Pierre Gilson Dr. Valentin Valtchev Dr. Svetlana Mintova Dr. Alexandre Vimont Dr. Robert Bedard Dr. Suheil Abdo Dr. Jeffery Bricker 《Chemphyschem》2020,21(16):1873-1881
We outline two methodologies to selectively characterize the Brønsted acidity of the external surface of FAU-type zeolites by IR and NMR spectroscopy of adsorbed basic probe molecules. The challenge and goal are to develop reliable and quantitative IR and NMR methodologies to investigate the accessibility of acidic sites in the large pore FAU-type zeolite Y and its mesoporous derivatives often referred to as ultra-stable Y (USY). The accessibility of their Brønsted acid sites to probe molecules (n-alkylamines, n-alkylpyridines, n-alkylphosphine- and phenylphosphine-oxides) of different molecular sizes is quantitatively monitored either by IR or 31P NMR spectroscopy. It is now possible, for the first time to quantitatively discriminate between the Brønsted acidity located in the microporosity and on the external surface of large pore zeolites. For instance, the number of external acid sites on a Y (LZY-64) zeolite represents 2 % of its total acid sites while that of a USY (CBV760) represents 4 % while the latter has a much lower framework Si/Al ratio. 相似文献
38.
Jenna M. Allan Md Abdul Mumin Jeffery A. Wood William Z. Xu Wei Wu Paul A. Charpentier 《Journal of Polymer Science.Polymer Physics》2014,52(14):927-935
Poly(ethylene‐co‐vinyl acetate) (EVA) plastic films are widely used for solar coverings including photovoltaic modules and commercial greenhouse films, but are poor at controlling heat flow. In this work, silica aerogel (SA) nanogels were examined for preparing transparent heat retention EVA films that block far infrared spectra radiation to maintain heat, without compromising the optical performance of the films. SA nanogels were melt‐mixed using a mini twin‐screw extruder with EVA pellets to form SA/EVA composite, which were pressed into thin films with controlled thickness. The composite films were characterized in terms of optical properties using a variety of analytical methods including FTIR, UV–Vis spectroscopy, electron, confocal, and atomic force microscopy. Both thermicity and thermal conductivity of commercial and experimental SA/EVA films were measured. The results demonstrated that the SA/EVA films gave improved infrared retention compared to commercial thermal plastic films without compromising visible light transmission, showing the potential for this approach in next generation heat retention films. © 2014 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2014 , 52, 927–935 相似文献
39.
Dr. Todd R. Zeitler Timothy Van Heest Prof. David S. Sholl Dr. Mark D. Allendorf Dr. Jeffery A. Greathouse 《Chemphyschem》2013,14(16):3740-3750
A set of 98 nanoporous framework material (NFM) structures was investigated by classical Grand canonical Monte Carlo simulations for low-pressure O2 adsorption properties (Henry’s constant and isosteric heat of adsorption). The set of materials includes those that have shown high O2 uptake experimentally as well as a subset of more than 2000 structures previously screened for noble-gas uptake. While use of the general force field UFF is fruitful for noble-gas adsorption studies, its use is shown to be limited for the case of O2 adsorption—one distinct limitation is a lack of sufficient O2–metal interactions to be able to describe O2 interaction with open metal sites. Nonetheless, those structures without open metal sites that have very small pores (<2.5 Å) show increased O2/N2 selectivity. Additionally, O2/N2 mixture simulations show that in some cases, H2O or N2 can hinder O2 uptake for NFMs with small pores due to competitive adsorption. 相似文献
40.