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991.
Efficient computation of operator‐type response sensitivities for uncertainty quantification and predictive modeling: illustrative application to a spent nuclear fuel dissolver model 下载免费PDF全文
This work honors the 75th birthday of Professor Ionel Michael Navon by presenting original results highlighting the computational efficiency of the adjoint sensitivity analysis methodology for function‐valued operator responses by means of an illustrative paradigm dissolver model. The dissolver model analyzed in this work has been selected because of its applicability to material separations and its potential role in diversion activities associated with proliferation and international safeguards. This dissolver model comprises eight active compartments in which the 16 time‐dependent nonlinear differential equations modeling the physical and chemical processes comprise 619 scalar and time‐dependent model parameters, related to the model's equation of state and inflow conditions. The most important response for the dissolver model is the time‐dependent nitric acid in the compartment furthest away from the inlet, where measurements are available at 307 time instances over the transient's duration of 10.5 h. The sensitivities to all model parameters of the acid concentrations at each of these instances in time are computed efficiently by applying the adjoint sensitivity analysis methodology for operator‐valued responses. The uncertainties in the model parameters are propagated using the above‐mentioned sensitivities to compute the uncertainties in the computed responses. A predictive modeling formalism is subsequently used to combine the computational results with the experimental information measured in the compartment furthest from the inlet and then predict optimal values and uncertainties throughout the dissolver. This predictive modeling methodology uses the maximum entropy principle to construct an optimal approximation of the unknown a priori distribution for the a priori known mean values and uncertainties characterizing the model parameters and the computed and experimentally measured model responses. This approximate a priori distribution is subsequently combined using Bayes' theorem with the “likelihood” provided by the multi‐physics computational models. Finally, the posterior distribution is evaluated using the saddle‐point method to obtain analytical expressions for the optimally predicted values for the parameters and responses of both multi‐physics models, along with corresponding reduced uncertainties. This work shows that even though the experimental data pertains solely to the compartment furthest from the inlet (where the data were measured), the predictive modeling procedure used herein actually improves the predictions and reduces the predicted uncertainties for the entire dissolver, including the compartment furthest from the measurements, because this predictive modeling methodology combines and transmits information simultaneously over the entire phase‐space, comprising all time steps and spatial locations. Copyright © 2016 John Wiley & Sons, Ltd. 相似文献
992.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2018,130(39):12848-12851
Covalent surface immobilization of proteins for binding assays is typically performed non‐specifically via lysine residues. However, receptors that either have lysines near their binding pockets, or whose presence at the sensor surface is electrostatically disfavoured, can be hard to probe. To overcome these limitations and to improve the homogeneity of surface functionalization, we adapted and optimized three different enzymatic coupling strategies (4′‐phosphopantetheinyl transferase, sortase A, and asparaginyl endopeptidase) for biolayer interferometry surface modification. All of these enzymes can be used to site‐specifically and covalently ligate proteins of interest via short recognition sequences. The enzymes function under mild conditions and thus immobilization does not affect the receptors’ functionality. We successfully employed this enzymatic surface functionalization approach to study the binding kinetics of two different receptor–ligand pairs. 相似文献
993.
《Journal of polymer science. Part A, Polymer chemistry》2018,56(9):1012-1019
Herein, we report the synthesis, characterization, and field‐effect properties of two cross‐conjugated dithienylmethanone (DMO)‐based alternating polymers, namely, PDMO‐S and PDMO‐Se . Both polymers possess high thermal stability, good solubility, and broad absorption spectra. Their electrochemical properties were investigated using cyclic voltammetry, indicating that PDMO‐Se has higher HOMO/LUMO energy levels of −5.49/−3.49 eV than −5.57/−3.58 eV of PDMO‐S . The two polymers exhibited promising charge transport properties with the highest hole mobility of 0.12 cm2 V−1 s−1 for PDMO‐S and 0.025 cm2 V−1 s−1 for PDMO‐Se . AFM and 2D‐GIXRD analyses demonstrated that the PDMO‐S formed lamellar, edge‐on packing thin film with close π‐π stacking. These findings suggest that cross‐conjugated polymers might be potential semiconducting materials for low‐cost and flexible organic electronics. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2018 , 56, 1012–1019 相似文献
994.
Near‐infrared emissive (NIR) porphyrin‐implanted carbon nanodots (PCNDs or MPCNDs) are prepared by selectively carbonization of free base or metal complexes [M = Zn(II) or Mn(III)] of tetra‐(meso‐aminophenyl)porphyrin in the presence of citric acid. The as‐prepared nanodots exhibit spontaneously NIR emission, small size, good aqueous dispersibility, and favorable biocompatibility characteristic of both porphyrins and pristine carbon nanodots. The subcellular localization experiment of nanodots indicates a lysosome‐targeting feature. And the in vitro photodynamic therapy (PDT) results on HeLa cells indicate the nanodots alone have no adverse effect on tumor cells, but display remarkable photodynamic efficacy upon irradiation. Moreover, MnPCNDs containing paramagnetic Mn(III) ions, which possesses good biocompatibility, NIR luminescence, and magnetic resonance imaging and efficient singlet oxygen production, are further studied in magnetic resonance imaging‐guided photodynamic therapy in vivo. 相似文献
995.
Ryszard Krzyminiewski Bernadeta Dobosz Grzegorz Schroeder Joanna Kurczewska 《Physics letters. A》2018,382(44):3192-3196
The paper shows the application of a new method – Magnetic Nanoparticles Focusing 3D, MNF-3D – for focusing of magnetic nanoparticles at any point in a three-dimensional space between the rotating magnet system. The results of focusing process of nanoparticles in water, human blood, human serum and polyurethane sponge are presented. Additionally, blood flow was also considered. The effectiveness of nanoparticle focusing was monitored optically and quantitatively by electron spin resonance method. The method enabled focusing of magnetic nanoparticles within a few minutes in different environments. A good efficiency of focusing process was observed for all the samples. 相似文献
996.
磁共振图像的重建、后处理及可视化是磁共振成像(MRI)系统的重要组成部分.本文开发了一个新的用于磁共振图像重建、后处理及可视化的开源框架YAP(Yet Another Pipeline),利用此框架可以方便地构建图像处理流水线.与现有的一些其他开源框架相比,本文开发的框架具有如下特点:(1)采用基于接口的设计,可使用基于接口的插件对流水线的功能进行扩展;(2)允许用户使用编写脚本的方式构建图像处理流水线,编辑与修改流水线都很方便;(3)支持带有分支结构的流水线,便于流水线的构建与调试.目前,该框架已经在商用系统中获得了应用. 相似文献
997.
Application of Anodic Stripping Differential Alternative Pulses Voltammetry for Simultaneous Species Quantification 下载免费PDF全文
《Electroanalysis》2018,30(9):1902-1905
The second order voltammetric technique Differential Alternative Pulses Voltammetry (DAPV) was applied in anodic stripping mode for simultaneous quantification of traces of species having close E1/2. The potential‐time waveform and the signal processing allowing the DAPV application in stripping mode are presented. The pulses widths and amplitudes were optimized to obtain maximal sensitivity and resolution at traces of In3+ and Cd2+ (having E1/2 difference of 45 mV) simultaneous quantification in presence of excess of Pb2+. Precise results for both species concentrations were obtained up to In3+ to Cd2+ concentration ratio as high as 1 to 10 without any sample pre‐treatment in purified industrial waste waters using 0.1 mol L−1 HCl as supporting electrolyte. 相似文献
998.
《Journal of polymer science. Part A, Polymer chemistry》2018,56(14):1584-1592
Starting from commonly available sugar derivatives, a single step protocol to access a small family of isohexide‐dioxalates ( 2a–c ) has been established. The synthetic competence of 2a–c has been demonstrated by subjecting them to condensation polymerization. Quite surprisingly, the proton NMR of poly(isomannide‐co‐hexane)oxalate revealed a 1:2 ratio between isomannide‐dioxalate ( 2a ) and 1,6‐hexanediol ( 3a ) in the polymer backbone. This intriguing reactivity was found to be an outcome of a cross metathesis reaction between 2a and 3a . The cross metathesis products 3a ”[2‐(2‐methoxyacetoxy)ethyl 2‐(2‐hydroxyethoxy)‐2‐(λ3‐oxydanylidene)acetate] and 2a ‘(3R,6R)‐6‐hydroxyhexahydrofuro[3,2‐b]‐furan‐3‐yl methyl oxalate were isolated in a control experiment. Based on direct and indirect evidence, and control experiments, an alternative polymerization mechanism is proposed. Polymerization conditions were optimized to obtain polyoxalates P1(2a‐3a)‐P9(2c‐3c) with molecular weights in the range of 14,000–68,000 g/mol, and narrow polydispersities. The identity of the polyoxalates was unambiguously established using 1‐2D NMR spectroscopy, MALDI‐ToF‐MS, and GPC measurements. The practical implication of these polymers is demonstrated by preparing transparent, mechanically robust films. The environmental footprint of the selected polyoxalates was investigated by subjecting them to solution and solid‐state degradation. The polyoxalates were found to be amenable to degradation. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2018 , 56, 1584–1592 相似文献
999.
The newly found ternary compound NdNiMg5 has been studied within DFT based methodologies. Results of cohesive energy, charge transfers, elastic constants and electron localized function mapping as well as electronic structure and bonding properties have been compared with those of isostructural binary NdNi. The calculation results have shown that Mg substructures interlayering NdNi – like slabs exhibit different magnitudes of charge transfers all within range of metallic behavior and the different Mg substructures selectively bind with Nd and Ni substructures. As a consequence an enhanced cohesion with respect to binary intermetallic NdNi is identified. The whole set of elastic constants and their combinations in orthorhombic symmetry confirm the mechanical stability of NdNiMg5 with larger compressibility and less ductility (more brittleness) with respect substructures to NdNi. While in an intermetallic compound such as NdNi the bonding is ensured mainly by Nd–Ni interaction, in NdNiMg5 Nd–Ni, Nd–Mg, Ni–Mg as well as Mg–Mg participate to the bonding and the extra electrons brought by Mg are found within bonding states thus illustrating furthermore the enhanced cohesion of the ternary versus the binary systems. 相似文献
1000.
The work of the author in measure and integration is based on new inner and outer envelope formations, which replace the traditional Carathéodory outer measure and certain simple suprema and infima. The new formations lead to essential improvements in both the extent and the adequacy of the basic results. However, they did not find an entrance into the recent textbook literature. The present paper seeks to demonstrate their power with the examples of the basic inner and outer extension and representation theorems for set functions and functionals. 相似文献