dataesr/scientific-paragraphs-categorization huggingface dataset:
Conclusions In the present work, a methodology for the development of accurate and robust ROM generation using a combination of PCA and Kriging was presented. The methodology was demonstrated for a 1D laminar flame with an increasing number of input parameters (equivalence ratio, composition of the fuel, inlet temperature), and for a 2D flame with two input parameters (inlet velocity and inlet fuel composition). In all three cases and for the 2D flame as well, both training and test data were available. The training data was employed to generate the ROM. The test data was used to assess the ROM's predictive capabilities. The results showed that the combination of PCA with Kriging is a valid solution for the development of physics-based SMs. Mainly, we want to stress the following points: • The developed surrogate models can be used for parameter exploration with low prediction errors: < 10%.
Acknowledgement We thank  Mr. Herve Arlaud  and  Dr. Gildas Lalizel  for providing the thermocouples for this study. We thank  Mr. Alain Claverie  and  Mr. Antoine Delicourt  for their assistance in the PIV experiments. We acknowledge the financial support of  ANRT  ( PN :  ANR-PLASMAFLAME-2011BS0902501 ).
The electrodes were directly tattooed on skin. With a commercial liquid bandage added on top, this tattoo stayed functional for several days. Humidity was measured by electrical impedance between two tattooed electrodes. Values were consistent with medically used silver/silver-chloride (Ag/AgCl) gel electrodes, but tattoos obviously offered superior comfort (Figure  22 ). Yao et al. (2017)  [70]  described a wearable, fully conformable, skin hydration sensor based on overall impedance. They used two interdigitated silver electrodes (more precisely, the Ag ink was made of silver nanowires, AgNWs) embedded into a PDMS matrix. The hydration sensor was calibrated against a commercial skin hydration system and was included into a flexible wristband, together with a miniaturized network analyzer chip, a small battery, and a Bluetooth chip for data transmission.
They used two interdigitated silver electrodes (more precisely, the Ag ink was made of silver nanowires, AgNWs) embedded into a PDMS matrix. The hydration sensor was calibrated against a commercial skin hydration system and was included into a flexible wristband, together with a miniaturized network analyzer chip, a small battery, and a Bluetooth chip for data transmission. A chest patch was also developed on the same basis (Figure  23 ). Even if designed for continuous monitoring directly on skin, the authors did not perform long-term experiments to discuss the stability of their sensor under operation. Yao et al. (2017)  [70]  described a wearable, fully conformable, skin hydration sensor based on overall impedance. They used two interdigitated silver electrodes (more precisely, the Ag ink was made of silver nanowires, AgNWs) embedded into a PDMS matrix.
Iontophoresis was not used to get interstitial fluid, but to deliver pilocarpine which induced sweat production; in turn, ethanol was detected using a conventional alcohol-oxidase/Prussian blue electrode. On-body experiments showed an increase of ethanol levels after alcohol intake. The integrated electronic board was able to control the iontophoresis/amperometry operation and transmit data wirelessly via Bluetooth. However, the paper did not provide any indication on the possibility of using this tattoo continuously and above all, there is still a potential for improvement to achieve a real integrated tool. Indeed, here, the flexible wireless instrumentation electronics is not included in the tattoo. Lansdorp et al. (Milo Sensors, Inc. ) reported very recently a wearable transdermal alcohol sensor  [93]  in the form of a wristband, which allows measurements up to 24 h in a row.
The detection principle is similar to the one of the previous examples (alcohol oxidase + Prussian blue); it delivers a linear response between 0 and 50 mM. The authors showed continuous data recorded with their device on a subject for two consecutive days, with accurate results (Figure  31 ). The sensor is composed of a disposable capsule made of an electrochemical device with three electrodes covered with a hydrophilic membrane in contact with the skin. In this remarkable example of integration, transdermal alcohol is recovered passively without the need for stimulation. Lawson et al. [94]  developed a SnO 2 sensor for monitoring ethanol on the skin. Transdermal alcohol emissions by perspiration were investigated during clinical trials on six subjects to demonstrate the relevance of this method.
The integrated electronic board was able to control the iontophoresis/amperometry operation and transmit data wirelessly via Bluetooth. However, the paper did not provide any indication on the possibility of using this tattoo continuously and above all, there is still a potential for improvement to achieve a real integrated tool. Indeed, here, the flexible wireless instrumentation electronics is not included in the tattoo. Kim et al. [92]  reported in 2016 a tattoo-like sensor for alcohol monitoring in sweat, which was evaluated directly on skin under real conditions. It integrated an iontophoretic part, an amperometric sensing part and flexible wireless electronics (Figure  30 ). Iontophoresis was not used to get interstitial fluid, but to deliver pilocarpine which induced sweat production; in turn, ethanol was detected using a conventional alcohol-oxidase/Prussian blue electrode.
Apart from alcohol, it is also possible to detect consumption of drugs using skin sensors. Reports concerning these applications are scarce, however. Voss et al. [95]  described in 2014 a portable (even if not wearable) electronic nose to detect directly on skin some changes in body odor caused by cannabis consumption. The authors enrolled 20 cannabis-smoking subjects for this study and compared their results to 20 tobacco-smoking ones. Because signals were difficult to interpret on a simple basis, two data processing techniques were used: principle component analysis (PCA) and pattern recognition with subsequent support vector machines (SVM). The SVM analysis obtained an accuracy of 92. 5% between cannabis-consuming volunteers and tobacco-smoking subjects. Technically, the electronic nose consisted of relatively non-specific gas sensors, one suitable for combustible gases, one for hydrocarbons, and the third one for NO 2.
The authors enrolled 20 cannabis-smoking subjects for this study and compared their results to 20 tobacco-smoking ones. Because signals were difficult to interpret on a simple basis, two data processing techniques were used: principle component analysis (PCA) and pattern recognition with subsequent support vector machines (SVM). The SVM analysis obtained an accuracy of 92. 5% between cannabis-consuming volunteers and tobacco-smoking subjects. Technically, the electronic nose consisted of relatively non-specific gas sensors, one suitable for combustible gases, one for hydrocarbons, and the third one for NO2. More recently, Mishra et al. [96]  developed a wearable potentiometric tattoo biosensor for monitoring various toxins such as organophosphates. Diisopropyl fluorophosphate (DFP) was used as a model.
The SC is known indeed to play a critical role in the barrier function of the skin (e. g. , protecting tissue from infections, dehydration, or even chemicals). Data obtained from this sensor were compared to 'tissue dielectric constant' (TDC) measurements obtained from the commercially available MoistureMeterD (MMD, Delfin Technologies). The tattoo sensor was able to reliably identify changes related to skin hydration/dehydration and was proposed as a technical aid for the management of skin diseases, such as atopic dermatitis or psoriasis. More recently, the same team  [99]  described a thin, flexible sensing platform based on silver electrodes screen-printed on a thin elastomeric substrate for skin monitoring. Using an acrylate porous adhesive layer improved the mechanical properties of the patch without degradation of the electrical performances.
Acknowledgments:  Université de Paris ,  CNRS  and  ANR (Agence Nationale de la Recherche)  and  CGI (Commissariat à l'Investissement d'Avenir ) are gratefully acknowledged for their financial support of this work through  Labex SEAM (Science and Engineering for Advanced Materials and devices)   ANR 11 LABX 086 ,  ANR 11 IDEX 05 02.
A distance of 500 µm between the electrode surface and the optical window was typically used. Fluorescence videos were then recorded, with a 100 ms exposure time per image, simultaneously with the cyclic voltammograms acquisitions at specified scan rates. Camera control and image processing were performed with the LightField 6. 0 software (Princeton Instruments). Variation of fluorescence intensity over time was measured from a sequence of images of the same region of interest (ROI). For the 1 mm disk electrode, a large square ROI was chosen in the middle of the circular area of the electrode, where incident light appears uniformly distributed. For platinum ultramicroelectrode (UME) with 25 µm in diameter, a 100x100 pixels ROI (~70x70 µm in real scale) encompassing the electroactive area was used to collect fluorescence photons emitted by all resorufin molecules distributed in the whole expanding diffusion layer.
Resorufin reduction, occurring at the level of the second CV wave, is also modeled as the direct transfer of two electrons characterized by the set of apparent parameters , ,  2 , reaction (III). 1] [32] [33]  Yet, in the absence of extensive data regarding the actual reduction mechanism of RF this simplification is required. Finally, the thermodynamically favorable homogeneous comproportionation reaction between DH and RZ,  28  yielding RF and RZ red , is represented by reaction (IV), and characterized by the second order rate constant k 2. We now intend to make use of the proposed mechanism to simulate the experimental CV and CVF of resazurin we recorded, using the DigiElch software. This simulation requires that all of the parameters appearing in the above kinetic scheme are quantitatively known, or that further simplifying assumptions are made.
ASSOCIATED CONTENT Supporting Information The Supporting Information is available free of charge on the ACS Publications website at DOI: 10. 1021/acs. analchem. xxxxxxx. CV characterization of resorufin reduction. CV of resazurin at a millimetric electrode: effect of the cleavage rate constant k 1 on the simulated current signal, correlation between the derivative of the fluorescence intensity and the CV current. Extra data acquired with the current-to-fluorescence converter setup. Discussion about the proportionality of the fluorescence signal and the amount of resorufin in the UME diffusion layer.
Acknowledgements The authors acknowledge the  French Ministère de l'Enseignement Supérieur et de la Recherche (MESR)  and  École Doctorale Matériaux  for supporting this project. They also thank  R. Vera  from the  Centre de Diffractometrie H. Longchambon  ( UCBL ) for the XRD experiments, and  P. Alcouffe  ( UMR5223 ) for the surface preparation of AFM samples.
Theoretical details Spin-polarized density functional theory calculations, within periodic boundary conditions, were performed using the plane wave approach, as implemented in the Vienna ab initio simulation package (VASP) code. 27, 28 The generalized gradient approximation functional of the exchange-correlation energy was calculated within the Perdew, Burke, and Ernzerhof formulation of the generalized-gradient approximation (GGA-PBE). 29, 30 To correct for the well-known band-gap problem of GGA type of functionals, the Hubbard U parameter was added by using the Dudarev's approach (PBE+U)  31  with an optimal value for the Coulomb interaction corrections of Ti electrons U eff ¼ 3. 3 eV. The calculations included projector augmentedwave (PAW) pseudopotentials,  32, 33  where oxygen 2s and 2p, titanium 3p, 4s, and 3d, copper 3p and 3d and platinum 6s and 5d electrons were explicitly treated.
Acknowledgements This work was granted access to the HPC resources of [CCRT/ CINES/IDRIS] under the allocation 2017 [x2017087369] made by  GENCI  ( Grand Equipement National de Calcul Intensif). Financial support of  CEST Kompetenzzentrum für elektrochemische Oberächentechnologie GmbH, Austria  in the frame of the  COMET program  is gratefully acknowledged.
VIBRATIONAL SPECTROSCOPY Infrared spectroscopy data were acquired by attenuated total reflectance spectra on a Vertex 70-RAM II Bruker spectrometer (Bruker Analytical, Madison, WI) operating with a Golden Gate TM diamond ATR accessory (Specac Ltd. , Slough, UK). FTIR/ATR spectra [3500-600 cm -1 ] were collected with a nominal resolution of 1 cm - 1 by co-adding 64 scans for each spectrum. Only for the sample containing Cl -as anion, an additional spectrum was acquired in transmission mode by means of an Agilent Cary 660 with a resolution of 1 cm -1 in the frequency range between 4000 and 400 cm -1 , by dissolving the ionic salt in KBr in the proportion 1:100 in mass. The measurement was the mean of 100 scans. Prior of this measurement the sample was kept at 80°C for 48 hours in order to increase its crystallinity and remove hydration water.
COMPUTATIONAL The isolated cation (m-xylene) was investigated computationally by means of the Spartan software  [23] [24]. Concerning the anions their spectra are well known both from an experimental and computational point of view  [25] [26]. After the optimization, we obtained many degenerate geometries, that were removed from the following procedures. The vibration frequencies and the infrared intensity and Raman activity of the optimized structures having an energy not higher than 5 kJ/mol from the lowest energy conformer were calculated by means of the Spartan software. Only 7 of them had all positive vibrational frequencies and can therefore, be considered as stable points of the potential energy surface. In order to compare the experimental infrared and Raman spectra with the calculated one, we constructed expected IR and Raman spectra summing Gaussian curves centered at each calculated vibration frequency, with an intensity proportional to the calculated one and a fixed line width of 10 cm -1.
ACKNOWLEDGEMENTS The authors gratefully acknowledge the financial support by The  Ministry of Higher Education and Scientific Research (MESRS) of Algeria  in  PRFU  project code:  B00L01UN200120180002 ; also,  Mostefa Boumediene  would like to thank  Doctor Guendouzi Abdelkrim ,  Head  of the  Department of Chemistry, Faculty of Sciences, University of Saïda, Algeria  for their fruitful support, Moreover;  Mostefa Boumediene  would like to congratulate his supervisor  Mr : HADDAD , who deserve the second place in the promotion of the rank of Professor related to 41st session of CUN results.
The analysis of the images obtained in these experiments involved six steps: determining the slope of the linear increase / decrease of the corrected mean intensity that was observed immediately after setting the potential of the electrode to OCP (i. e. after t = 257 s). This slope reflects the initial rate of the enzyme catalyzed reaction and is our analyte concentration-proportional analytical signal. Steps 1 and 2 were realized using ImageJ  29  while the other steps were carried out using various scientific graphing and data analysis software packages.
Acknowledgements Financial support from the  Romanian Executive Agency for Higher Education, Research, Development and Innovation Funding (projects GRAPHTIVITY ,  PN-III-P4-ID-PCE-2016-0619 , and  PN-III-P4-ID-PCE-2016-0762 ), the  Belgian Fund for Scientific Research  (project  GRAPHTIVITY ), the  German Research Foundation  (project  GRAPHTIVITY ), the  French National Research Agency  (project  GRAPHTIVITY ), and  Fonds européen de développement régional (FEDER)  and the  Walloon region  under the  Operational Program "Wallonia-2020. EU"  (project  CLEARPOWER ) is gratefully acknowledged.
4%) in helium which was pre-mixed with oxygen to attain a 1:10 (or 10:1) cyclohexane to oxygen ratio and was fed into the reactor at a flow of 30 sccm  29. Details of the GISAXS/GIXANES/TPRx approach are given for example in ref. 45. The reaction products were analyzed using a differentially pumped massspectrometer (Pfeiffer Vacuum Prisma QMS 200) continuously sampling from the reaction cell. Typical raw reactivity data are shown in Supplementary Figure  10. The rates of formation of products were calculated using the number of deposited Co atoms and calibrating the mass spectrometer using diluted calibrated gas mixtures (AirGas). The GIXANES data were analyzed with IFEFFIT interactive software package (with ATHENA and ARTEMIS graphical interfaces)  46. The GISAXS data were collected on a Platinum detector developed by the Advanced Photon Source (1024 × 1024 pixels) with X-rays of 7.
Acknowledgements The authors thank  Drs. Jeffrey W. Elam  and  Joseph A. Libera  for providing the ALDcoated substrates. The work at  Argonne  was supported by the  US Department of Energy, BES Materials Sciences  under Contract  DEAC02-06CH11357  with  UChicago Argonne, LLC , operator of  Argonne National Laboratory. The work at the  Advance Photon Source  (beamline 12-ID-C) was supported by the  US Department of Energy, Scientific User Facilities  under Contract  DEAC02-06CH11357  with  UChicago Argonne, LLC , operator of  Argonne National Laboratory. A. H. thanks for the support provided by the  Air Force Office of Scientific Research. We thank  Helmholtz-Zentrum Berlin  for allocation of synchrotron radiation beamtime.
Evolution of textural properties from FeFER to FeFER800 The evaluation of the effects of the ageing procedure on the textural properties of the catalysts was carried out using the standard N2 physisorption at liquid nitrogen temperature. For plots relative to both FeFER and FeFER800, the isotherm was typical for the type I one (also called Langmuir isotherm) for which the adsorbed volume readily reaches a plateau (P/P o < 0. 2). The isotherm data were processed according to several theories (Langmuir, BET and t-plot) in order to estimate the microporous volumes. The total porous volume was directly obtained from the isotherm at P/P° = 0. 99 (which corresponds to the filling of pores with size below 100 nm) and then the sum of mesoporous and macroporous volumes was determined by difference.
Preliminary processing of the gas phase data provided estimated values for = 43 kJ. mol -1 and for NO adsorption heat ∆Hads NO = -30 kJ. mol -1 (see section 3. 3. 3). Estimate for 2 A2 PO2 LFe 2 was obtained from the slope of the following plot: plot 3 8 ' F""" "F"G • A = -V" • -˜™ š› ™• … \ Estimate for B was obtained from the slope of the following plot: plot 4 oe•žŸ Ÿ•ž ¡ ¢z£¤ ¥ Ÿ Ÿ•ž ¡ = ¦ ‡ V - §¨© ªoe «¡ \ OE Estimate for LFe 2 was obtained from the slope of the following plot: plot 5 8 ' F""" "F"G • A = -F""" "F"G ' • Table  5  reports the whole estimated values together with their optimized values obtained after minimization of SD for the reaction rate calculated using both eq. 8 and eq. 9. a RDS E A similar methodology was applied for the eight remaining possible RDS (i. j). The number of parameters required to model the whole experimental data was always fixed to the minimum value (see first column of Table  6 ) and their initial estimated values were always in a reasonable range as indicated by the initial estimated standard deviation lying between 1.
Grid masking and tracking As measurements are focused around the swept zone, the oscillating grid is visible on the recorded images (gure ?? a)), which is an asset for grid tracking but problematic for the velocity eld calculation. The grid has therefore to be rst removed from images for velocity calculation and then isolated for the grid tracking step. Grid masking is achieved using DaVis software from LaVision. At rst, an horizontal median lter is applied on every recorded image (gure ?? b)). These images are then binarized using an arbitrary threshold based on the image gray level values such that the pixel corresponding to the grid are set to zero and the rest of the image to one (gure ?? c)). Each mask image is then applied to the corresponding image when calculating the velocity eld.
One eect that can not be easily corrected with this procedure is the shaded area visible on the left part of gure ?? a) under the grid. Here the PIV laser sheet was directed so that it always met the grid from the top, and the shaded region was always under the grid. In doing so, the region above the grid is always well lighted, and measurements can always be considered reliable there. The shaded particle region is represented by a gray zone on each PIV-deduced elds at specic grid positions in the following gures, to recall that this region is prone to errors. Grid tracking is performed by a Matlab custom script. It also starts by an horizontal median ltering step to smooth particles o the image. Gray level intensity is then horizontally averaged on the whole image width, and the peaks of width averaged intensity gradients are used to detect grid boundaries (gure ??).
The main idea is to derive local shear rate elds from instantaneous, phase averaged or 1105 time averaged velocity elds. Local shear rate values are then used to estimate an apparent viscosity through the constitutive equation of the polymer, here a CY law for the rheological behaviour derived in section ?? (equation ??, gure ??). 1110 This method is limited because the velocity data is only 2D and lacks the third velocity component. Shear rate values can thus only roughly approach the real local shear rate, and no precise quantitative study can be performed. However the method allows to qualitatively 1115 estimate the viscosity variations in a plane of measurement. In practice, the apparent instantaneous shear rate is computed as γapp = ∂U x ∂z 2 + ∂U z ∂x 2 (18) an the instantaneous apparent viscosity as µ app = f CY ( γapp ) (19) with f CY the Carreau-Yasuda function dened in equation (??), and using tting parameters obtained in section ??.
Acknowledgements. The authors thank  P. Moonen  and  F. Guerton  from of  UMS CNRS-UPPA-Total 3360  DMEX for the DRP data, and  P. Laurençot  for fruitful discussions. The financial contribution of the  Carnot Institute ISIFoR and Conseil Départemental Pyrénées-Atlantiques  ( CD64 ) is greatly acknowledged.
The maximum theoretical degree of substitution (DS max ) was calculated as the ratio of RIL and anhydroglucose (AGU) molar masses taking into account the weight of RIL and CAP used to prepare CAP-RIL films according to the following equation (Equation (  2 )): DS max = M RIL m RIL M AGU m CAP (2) where, MAGU is the average molar mass of the AGU unit in CAP (325. 67 g mol -1 ), MRIL is the molar mass of the ionic liquid, and mCAP and mRIL is the weight (g) of CAP and RIL respectively, in a given CAP-RIL film. MAGU was calculated using the data provided by the producer (Eastman, USA), concerning the acetyl, propionyl, and free OH groups content in CAP equal to 1. 3 wt %, 48. 0 wt %, and 1. 7 wt %, respectively. Generally, the primary carbon atom at C6 position (Figure  5A ) is the most reactive CAP substituent.
In the case of polymers analyses, the conversion as well as the composition of the polymers and the microstructural contents were calculated by mean of 1 H-and 13 C-NMR spectroscopy analysis using Topspin or MestreNova softwares. Size exclusion chromatography (SEC) analysis of the samples were performed in THF as an eluent at 40 • C (1 mL/min) with a SIS HPLC pump (Waters S. A. S, Saint-Quentin-en-Yvelines, France), a Waters 410 refractometer, and Waters Styragel columns (HR2, HR3, HR4, and HR5E) calibrated with polystyrene standards. FTIR analyses were performed on an ATR spectrometer (Shimadzu France, Marne-la-Vallée, France).
Acknowledgments: We gratefully acknowledge the  University of Lille  for the financial support of  Obaid H. Hashmi , and  CNRS  for donation. Aurélie Malfait  and  Jonathan Potier  are acknowledged for SEC analyses. We would also like to thank  Céline Delabre  for performing the elemental analysis as well as  Patrick Daubias  and  Eric Buisine  for the availability for NMR experiments.