Dilute solution properties and force field model parameters of LLDPE in good solvent from "Structure-dilute property relationships of comb-like macromolecules in a good solvent" and "The importance of branch placement on the dilute solution properties of comb-like macromolecules".

Description

These data and the coarse-grain force-field parameters were used to produce publication (1) "Structure-dilute property relationships of comb-like macromolecules in a good solvent" by Robert J. S. Ivancic (OrcID: https://orcid.org/0000-0001-9969-2534, National Institute of Standards and Technology, Material Measurement Laboratory, Division 642, Group 1), Sara V. Orski (OrcID: https://orcid.org/0000-0002-3455-0866, National Institute of Standards and Technology, Material Measurement Laboratory, Division 642, Group 1), and Debra J. Audus (OrcID: https://orcid.org/0000-0002-5937-7721, National Institute of Standards and Technology, Material Measurement Laboratory, Division 642, Group 1) and (2) "The importance of branch placement on the dilute solution properties of comb-like macromolecules" by Robert J. S. Ivancic, Chase B. Thompson (OrcID: https://orcid.org/0000-0002-8534-486X, Leidos), Devin A. Golla, Bintou Koroma, Jack F. Douglas (OrcID: https://orcid.org/0000-0001-7290-2300, National Institute of Standards and Technology, Material Measurement Laboratory, Division 642, Group 1), Sara V. Orski, and Debra J. Audus. The README.md file describes the dataset.Abstract from publication (1) : The structural characterization of branched polymers still poses experimental challenges despite their technological potential. This lack of clarity is egregious in linear low-density polyethylene (LLDPE), a common industrial plastic. Here, we design a coarse-grain, implicit solvent molecular dynamics model for LLDPE in 1,2,4-trichlorobenzene, a canonical good solvent, thatreplicates all-atom simulations and experiments. We employ this model to test the relationship between the contraction factors, the ratios of branched to linear dilute solution properties. In particular, we relate the contraction factor of the radius of gyration to that of the intrinsic viscosity and the hydrodynamic radius. The contraction exponents are constant as we vary branchlength and spacing in contrast to theoretical expectations. We use this observation to develop a general theory for the dilute solution properties of linear polymers with linear side-chain branches, comb-like macromolecules, in a good solvent and validate the theory by generating master curves for LLDPE.Abstract from publication (2) : Branch density and length substantially impact the properties of comb-like polymers. Scientists often use the dilute solution properties of these materials to quantify their architecture. As branch spacing decreases and branch length increases at a fixed molecular mass, dilute solution properties such as the radius of gyration, intrinsic viscosity, and hydrodynamic radius typically decrease because the length of the backbone decreases. However, this decrease is only partially driven by this change in backbone length, even for relatively short branches. While many models focus on predicting the dilute solution properties of these materials with fixed branch spacing, most comb-like polymers exhibit statistical branch spacing which leads to non-trivial changes in excluded volume effects. Using molecular dynamics simulations, we show how changing the distribution of branches from fixed to statistical and then to diblock affects the dilute solution properties of a coarse-grained linear low-density polyethylene (LLDPE), a canonical comb-like polymer, in 1,2,4-trichlorobenzene, a standard good solvent. This approach explicitly accounts for excluded volume interactions that were not included in prior theories. We extend our previous theoretical work to account for statistical branch spacing and test prior renormalization group estimates of diblocks in good solvent to show that it is consistent with our numerical results. Ourapproach provides a framework for a more quantitative understanding of chain architecture from dilute solution properties, yielding better structure-property relationships.

Resources

Name Format Description Link
8 This file contains data for LLDPE with constant branch spacing from publication (2). This file is a csv with the same properties as measured in `dilute_solution_properties_data.csv`. https://data.nist.gov/od/ds/mds2-2494/publication2_constant_dilute_solution_properties_data.csv
8 This file contains data for LLDPE with diblock spacing from publication (2). Here, one of the blocks is polyethylene and the other is LLDPE with a constant branch spacing of 8 carbons. This file is a csv with the with the same properties as measured in `dilute_solution_properties_data.csv` except the property branch spacing is replaced with branch fraction [f], which is the fraction of the chain backbone that is contant spacing LLDPE. https://data.nist.gov/od/ds/mds2-2494/publication2_diblock_dilute_solution_properties_data.csv
8 This file contains data for LLDPE with random branch spacing from publication (2). Here, branches are placed along the backbone of a polyethylene with a minimum branch spacing of 8 carbons. This file has the same properties as `publication2_dilute_solution_properties_data_diblock.csv`, where a branch fraction of 1 indicates LLDPE with a constant branch spacing of 8 carbons. https://data.nist.gov/od/ds/mds2-2494/publication2_random_dilute_solution_properties_data.csv
0 README describing data in repository https://data.nist.gov/od/ds/mds2-2494/README.md
5 input file containing pair, bond, angle, and dihedral styles, coefficients and masses for coarse-grain force field. This force-field may be used to simulate other polyolefins in good solvent. https://data.nist.gov/od/ds/mds2-2494/input.lammps_force_field
8 This file is a comma-separated-values (csv) file of the mean and bootstrap standard error for each dilute solution property measured (radius of gyration [Rg], intrinsic viscosity [eta], and radius of hydration [Rh]) at each branch spacing [S], branch length [L], and mass [M] of LLDPE studied in the paper. (S,L) = (\infty, 0) corresponds to high-density polyethylene. dilute_solution_properties_data.csv : This file is a comma-separated-values (csv) file of the mean and bootstrap standard error for each dilute solution property measured (radius of gyration [Rg], intrinsic viscosity [eta], and radius of hydration [Rh]) at each branch spacing [S], branch length [L], and mass [M] of LLDPE studied in the paper. (S,L) = (\infty, 0) corresponds to high-density polyethylene. ZENO (https://zeno.nist.gov/) is used to compute dilute solution properties from ensemble of configurations. Monomers with 2 and 4 carbons use a ZENO radius of 2.1 and 2.8 nanometers, respectively. The intrinsic viscosity values are scaled down by a factor of C = 0.68. https://data.nist.gov/od/ds/mds2-2494/dilute_solution_properties_data.csv

Tags

  • good-solvent
  • lldpe
  • coarse-grain
  • radius-of-hydration
  • tcb
  • molecular-dynamics
  • radius-of-gyration
  • linear-low-density-polyethylene
  • intrinsic-viscosity
  • 124-trichlorobenzene

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