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21.
Bence Paul Kai Kysenius James B. Hilton Michael W. M. Jones Robert W. Hutchinson Daniel D. Buchanan Christophe Rosty Fred Fryer Ashley I. Bush Janet M. Hergt Jon D. Woodhead David P. Bishop Philip A. Doble Michelle M. Hill Peter J. Crouch Dominic J. Hare 《Chemical science》2021,12(30):10321
Tumours are abnormal growths of cells that reproduce by redirecting essential nutrients and resources from surrounding tissue. Changes to cell metabolism that trigger the growth of tumours are reflected in subtle differences between the chemical composition of healthy and malignant cells. We used LA-ICP-MS imaging to investigate whether these chemical differences can be used to spatially identify tumours and support detection of primary colorectal tumours in anatomical pathology. First, we generated quantitative LA-ICP-MS images of three colorectal surgical resections with case-matched normal intestinal wall tissue and used this data in a Monte Carlo optimisation experiment to develop an algorithm that can classify pixels as tumour positive or negative. Blinded testing and interrogation of LA-ICP-MS images with micrographs of haematoxylin and eosin stained and Ki67 immunolabelled sections revealed Monte Carlo optimisation accurately identified primary tumour cells, as well as returning false positive pixels in areas of high cell proliferation. We analysed an additional 11 surgical resections of primary colorectal tumours and re-developed our image processing method to include a random forest regression machine learning model to correctly identify heterogenous tumours and exclude false positive pixels in images of non-malignant tissue. Our final model used over 1.6 billion calculations to correctly discern healthy cells from various types and stages of invasive colorectal tumours. The imaging mass spectrometry and data analysis methods described, developed in partnership with clinical cancer researchers, have the potential to further support cancer detection as part of a comprehensive digital pathology approach to cancer care through validation of a new chemical biomarker of tumour cells.Digital pathology and laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS) imaging reveals a unique elemental signature of colorectal cancer. 相似文献
22.
The subdifferential of a function is a generalization for nonsmooth functions of the concept of gradient. It is frequently used in variational analysis, particularly in the context of nonsmooth optimization. The present work proposes algorithms to reconstruct a polyhedral subdifferential of a function from the computation of finitely many directional derivatives. We provide upper bounds on the required number of directional derivatives when the space is ?1 and ?2, as well as in ? n where subdifferential is known to possess at most three vertices. 相似文献
23.
We prove that if ma = mK*da*mK{\mu _{a}\,{=}\,m_{K}*\delta _{a}*m_{K}} is the K-bi-invariant measure supported on the double coset KaK í SU(n){KaK\subseteq SU(n)} , for K = SO(n), then mak{\mu _{a}^{k}} is absolutely continuous with respect to the Haar measure on SU(n) for all a not in the normalizer of K if and only if k ≥ n. The measure, μ
a
, supported on the minimal dimension double coset has the property that man-1{\mu _{a}^{n-1}} is singular to the Haar measure. 相似文献
24.
Nomeir AA Pramanik BN Heimark L Bennett F Veals J Bartner P Hilbert M Saksena A McNamara P Girijavallabhan V Ganguly AK Lovey R Pike R Wang H Liu YT Kumari P Korfmacher W Lin CC Cacciapuoti A Loebenberg D Hare R Miller G Pickett C 《Journal of mass spectrometry : JMS》2008,43(4):509-517
Posaconazole (SCH 56592) is a novel triazole antifungal drug that is marketed in Europe and the United States under the trade name 'Noxafil' for prophylaxis against invasive fungal infections. SCH 56592 was discovered as a possible active metabolite of SCH 51048, an earlier lead. Initial studies have shown that serum concentrations determined by a microbiological assay were higher than those determined by HPLC from animals dosed with SCH 51048. Subsequently, several animals species were dosed with (3)H-SCH 51048 and the serum was analyzed for total radioactivity, SCH 51048 concentration and antifungal activity. The antifungal activity was higher than that expected based on SCH 51048 serum concentrations, confirming the presence of active metabolite(s). Metabolite profiling of serum samples at selected time intervals pinpointed the peak that was suspected to be the active metabolite. Consequently, (3)H-SCH 51048 was administered to a large group of mice, the serum was harvested and the metabolite was isolated by extraction and semipreparative HPLC. LC-MS/MS analysis suggested that the active metabolite is a secondary alcohol with the hydroxyl group in the aliphatic side chain of SCH 51048. All corresponding monohydroxylated diastereomeric mixtures were synthesized and characterized. The HPLC retention time and LC-MS/MS spectra of the diastereomeric secondary alcohols of SCH 51048 were similar to those of the isolated active metabolite. Finally, all corresponding individual monohydroxylated diasteriomers were synthesized and evaluated for in vitro and in vivo antifungal potencies, as well as pharmacokinetics. SCH 56592 emerged as the candidate with the best overall profile. 相似文献
25.
MF Miller IA Franchi AS Sexton CT Pillinger 《Rapid communications in mass spectrometry : RCM》1999,13(13):1211-1217
The use of infrared laser-assisted fluorination to release oxygen from milligram quantities of silicates or other oxide mineral grains is a well-established technique. However, relatively few studies have reported the optimisation of this procedure for oxygen-17 isotope measurements. We describe here details of an analytical system using infrared (10 μm) laser-assisted fluorination, in conjunction with a dual inlet mass spectrometer of high resolving power ( approximately 250) to provide (17)O and (18)O oxygen isotope measurements from 0.5-2 mg of silicates or other oxide mineral grains. Respective precisions (1) of typically 0.08 and 0.04 per thousand are obtained for the complete analytical procedure. Departures from the mass-dependent oxygen isotope fractionation line are quantified by Delta(17)O; our precision (1) of such measurements on individual samples is shown to be +/-0.024 per thousand. In turn, this permits the offset between parallel, mass-dependent fractionation lines to be characterised to substantially greater precision than has been possible hitherto. Application of this system to investigate the (17)O versus (18)O relationship for numerous terrestrial whole-rock and mineral samples, of diverse geological origins and age, indicates that the complete data set may be described by a single, mass-dependent fractionation line of slope 0.5244+/- 0.00038 (standard error). Copyright 1999 John Wiley & Sons, Ltd. 相似文献
26.
CM Silva MF Duarte ML Mira MH Florêncio K Versluis AJ Heck 《Rapid communications in mass spectrometry : RCM》1999,13(12):1098-1103
Fast atom bombardment, combined with high-energy collision-induced tandem mass spectrometry, has been used to investigate gas-phase metal-ion interactions with captopril, enalaprilat and lisinopril, all angiotensin-converting enzyme inhibitors.Suggestions for the location of metal-binding sites are presented. For captopril, metal binding occurs most likely at both the sulphur and the nitrogen atom. For enalaprilat and lisinopril, binding preferably occurs at the amine nitrogen. Copyright 1999 John Wiley & Sons, Ltd. 相似文献
27.
We prove that the G-invariant orbital measures supported on adjoint orbits in the Lie algebra of a classical, compact, connected, simple Lie
group satisfy a smoothness dichotomy: Either μ
k
is singular to Lebesgue measure or μ
k
∈ L
2. The minimum k for which μ
k
∈ L
2 is specified and is also the minimum k such that the k-fold sum of the orbit has positive measure.
S. K. Gupta appreciates the hospitality of the Department of Pure Mathematics at the University of Waterloo where some of
this research was done. K. E. Hare was supported in part by NSERC. 相似文献
28.
This review provides analysts with critical insights of current approaches for quantification by laser ablation-inductively coupled plasma-mass spectrometry in the field of elemental imaging. This encompasses both calibration strategies that have been used with success in imaging biological samples, as well as those with potential to improve analytical accuracy and precision if applied to imaging. Methods reviewed include the use of CRMs, laboratory prepared matrix matched standards, internal standardisation, online standard addition and a variety of novel approaches that makes elemental imaging accessible to a wider base of analysts. The importance of quantification and factors affecting its use in imaging will also be considered. 相似文献
29.
30.
Sydney Leach Michel Vervloet Alain Despr s Emilienne Br heret Jonathan P. Hare T. John Dennis Harold W. Kroto Roger Taylor David R. M. Walton 《Chemical physics》1992,160(3):451-466
Absorption spectra of C60 have been measured in the ranges (a) 190–700 nm in n-hexane solutions at 300 K, (b) 390–700 nm in n-hexane and in 3-methylpentane solutions at 77 K. 40 vibronic bands were observed. They exhibit a large range of bandwidths and intensities, whose significance is discussed. Assignment of electronic transitions has been carried out using the results of theoretical calculations. Vibronic structures have been analyzed within the framework of theories of electronic transitions of polyatomic molecules applied to the Ih symmetry group. Nine allowed 1T1u−1Ag transitions have been assigned in the 190–410 nm region. Observed and calculated allowed transition energies and oscillator strengths are compared. Detailed vibronic analyses of the 1 1T1u−1 1Ag and 2 1T1u−1 1Ag transitions illustrate the role of Jahn-Teller couplings. Orbitally forbidden singlet-singlet transitions are observed between 410 and 620 nm. Their vibronic structures were analyzed in terms of concurrent Herzberg-Teller and Jahn-Teller vibronic interactions. The 77 K spectra provided useful information on hot bands and on other aspects of the analyses. Vibronic bands belonging to triplet←singlet transitions were detected between 620 and 700 nm. 相似文献