Data from: Electrostatic compatibilization of amorphous and semi-crystalline immiscible polymer blends

Beech, Haley 1 ; Karnaukh, Kseniia1 ; Miyamoto, Madeleine1; Chen, KeRay1; Edmund, Jerrick1; Read de Alaniz, Javier 1 ; Hawker, Craig1 ; Segalman, Rachel1

Published Jul 18, 2025 on Dryad. https://doi.org/10.5061/dryad.0k6djhbd0

Data files

Jul 18, 2025 version files 21.19 MB

dryad_electrostatic_blends.zip
21.16 MB
README.md
25.03 KB

Abstract

The rapid accumulation of plastic waste underscores the urgent need for effective recycling strategies, yet conventional approaches are hindered by the immiscibility of chemically dissimilar polymers, which phase-separate upon blending and yield poor material properties. This study demonstrates a versatile strategy for electrostatic compatibilization, utilizing acid–base proton transfer between minimally functionalized polymers. Waste-derived polystyrene (PS) was successfully modified with < 4 mol% acid groups, while amorphous polybutadiene (PBD) was functionalized with < 6 mol% diethylamino base groups and subsequently hydrogenated to yield semi-crystalline polyethylene (PE) with the same functionalization level as the PBD. In both cases, blending with functionalized PS produced optically transparent, mechanically robust films. Notably, increasing charge density from 1.0 to 3.5 mol% significantly reduced domain sizes, indicating enhanced compatibilization, while increasing PS molecular weight from 28 to 470 kDa led to a notable three-order-of-magnitude increase in toughness. In PE/PS blends, the preservation of crystallinity during melt reprocessing was achieved by maintaining low functionalization levels, demonstrating compatibility without sacrificing critical material properties. These findings establish electrostatic compatibilization as a powerful, scalable platform for creating high-performance materials from chemically diverse and mixed plastic waste streams.

Data from a peer-reviewed article:

Title: Electrostatic Compatibilization of Amorphous and Semi-Crystalline Immiscible Polymer Blends
Journal: ACS Macro Letters
Authors: Haley K. Beech#, Kseniia M. Karnaukh#, Madeleine E. Miyamoto, KeRay Chen, Jerrick Edmund, Javier Read de Alaniz, Craig J. Hawker, and Rachel A. Segalman
#co-first author

Corresponding authors: Javier Read de Alaniz (javier@ucsb.edu), Craig J. Hawker (hawker@mrl.ucsb.edu), Rachel A. Segalman (segalman@ucsb.edu)

This dataset contains the necessary experimental data to reproduce all main text and supporting figures.

Data files are organized to match the manuscript’s figure and supporting information.
All data can be opened as a .csv file using Excel. Figures that are illustrations are not included in the folders.
This includes Fig. 1, Figure 2, Figure 6a, Schemes S1-S6

Folder and File List:

A) Figure 3a
B) Figure 3b.csv
C) Figure 4a
D) Figure 4d
E) Figure 5a.csv
F) Figure 5b.png
G) Figure 5c.png
H) Figure 5d.png
I) Figure 5e.png
J) Figure 6b.csv
K) Figure 6c

L) Figure S1.csv
M) Figure S2.csv
N) Figure S3.csv
O) Figure S4.csv
P) Figure S5.csv
Q) Figure S6.csv
R) Figure S7.csv
S) Figure S8.csv
T) Figure S9.csv
U) Figure S10.csv

V) Figure S11.csv
W) Figure S12.csv
X) Figure S13.csv
Y) Figure S14.csv
Z) Figure S15.csv
AA) Figure S16.csv
AB) Figure S17.csv
AC) Figure S18.csv
AD) Figure S19.csv
AE) Figure S20a.csv
AF) Figure S20b.csv

AG) Figure S21a.csv
AH) Figure S21b.csv
AI) Figure S21c.csv
AJ) Figure S22a.csv
AK) Figure S22b.csv
AL) Figure S23a.csv
AM) Figure S23b.csv
AN) Figure S24.csv
AO) Figure S25left.csv
AP) Figure S25right.csv

AQ) Figure S26.csv
AR) Figure S27left.csv
AS) Figure S27right.csv
AT) Figure S28left.csv
AU) Figure S28right.csv
AV) Figure S29.csv
AW) Figure S30a.csv
AX) Figure S30b.csv
AY) Figure S30c.csv
AZ) Figure S31.csv

BA) Figure S33a
BB) Figure S33b
BC) Figure S34a
BD) Figure S34b
BE) Figure S35a
BF) Figure S35b
BG) Figure S36a
BH) Figure S36b
BI) Figure S37left.csv
BJ) Figure S37right.csv

BK) Figure S38left.csv
BL) Figure S38right.csv
BM) Figure S39left.csv
BN) Figure S39right.csv
BO) Figure S40left.csv
BP) Figure S41left.csv
BQ) Figure S41right.csv
BR) Figure S42left.csv
BS) Figure S42right.csv

BT) Figure S44a
BU) Figure S44b
BV) Figure S44c
BW) Figure S44d
BX) Figure S45

Abstract.txt

README.txt

Figure 3: SAXS Profile and Domain Spacing

A) Fig3a: Folder: SAXS PS/PBD blends with varied levels of charge; each file is named for the mol% charge of the blend

Column A: Scattering Vector, q (A^(-1))
Column B: Scattering Intensity, I(q) (arbitrary units)

B) Fig3b: Domain size as a function of the average mol% charge of blend

Column A: Average Charge of Blend (mol%)
Column B: Domain Size (nm)

Figure 4: Tensile Tests and Tensile Properties. Data for Figures 4b, c, e, and f are available in Table S11

C) Fig4a: Folder: Stress strain curves for PBD/PS blends of varied PS molecular weight

Column A: Strain (%)
Column B: Stress (MPa)

D) Fig4d: Folder: Stress strain curves for PBD/PS blends of varied average charge

Column A: Strain (%)
Column B: Stress (MPa)

Figure 5A: Percent crystallinity trends of 27 kDa PE / 28 kDa PS blends prepared using different processing techniques as a function of the average charge of blend components.

E) Figure 5a.csv

Row 1: X and Y axes, corresponding to Average Charge of Blend Components and Percent Crystallinity (%) with STDEV.S
Row 2: Processing technique
- dataset 1: Theoretical - Average Charge of Blend Components (X) and Percent Crystallinity with STDEV.S (Y) -> Columns A + B + C
- dataset 2: Hot-Pressed - Average Charge of Blend Components (X) and Percent Crystallinity with STDEV.S (Y) -> Columns A + D + E
- dataset 3: Drop-Cast & Hot-Press - Average Charge of Blend Components (X) and Percent Crystallinity with STDEV.S (Y) -> Columns A + F + G

Figure 5B-E: Photos of PE/PS blends

F) Figure 5b.png: unfunctionalized blend, hot pressed
G) Figure 5c.tif: optical microscopy of unfunctionalized blend
H) Figure 5d.png: functionalized blend, hot pressed
I) Figure 5e.png: drop-cast followed by hot press
————————————————-

Figure 6: Tensile Tests and Tensile Properties. Data for Figure 6b available in Table S17; data for Figure 6d are available in Table S18.

J) Figure 6b.csv: The percent crystallinity of the blend throughout reprocessing cycles.

Column 1: Sample/Processing
Column 2: Percent Crystallinity
Column 2: STDEV.S

K) Fig6c: Folder: Stress strain curves for PE/PS blends of varied reprocessing histories

Column A: Strain (%)
Column B: Stress (MPa)

FIGURE S1: 1H NMR spectrum of polystyrene synthesized via RAFT before chain end removal.

L) FigS1.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S2: 1H NMR spectrum of polystyrene synthesized via RAFT after chain end removal.

M) FigS2.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S3: 1H NMR spectrum of 28 kDa polystyrene sulfonate with 1.5 mol% sulfonate groups.

N) FigS3.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S4: 1H NMR spectrum of 28 kDa polystyrene sulfonate with 2.6 mol% sulfonate groups.

O) FigS4.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S5: 1H NMR spectrum of 28 kDa polystyrene sulfonate with 3.5 mol% sulfonate groups.

P) FigS5.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S6: 1H NMR spectrum of 140 kDa recycled polystyrene sulfonate with 2.9 mol% sulfonate groups.

Q) FigS6.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S7: 1H NMR spectrum of 470 kDa polystyrene sulfonate with 1.1 mol% sulfonate groups.

R) FigS7.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S8: 1H NMR spectrum of 470 kDa polystyrene sulfonate with 3.6 mol% sulfonate groups.

S) FigS8.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S9: Representative 1H NMR spectrum of polystyrene sulfonate titrated with ethyl imidazole. The sample shown is 28 kDa PSS with 3.5 mol% sulfonate groups.

T) FigS9.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S10: Representative 1H NMR spectrum of methylated polystyrene sulfonate for GPC. The sample shown is 470 kDa PSS with 1.1 mol% sulfonate groups.

U) FigS10.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S11: 1H NMR spectrum of 26 kDa polybutadiene (LBR-305, Kuraray).

V) FigS11.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S12: Quantitative 13C NMR spectrum of 26 kDa polybutadiene (LBR-305, Kuraray).

W) FigS12.csv

Column 1: 13C (ppm)
Column 2: signal/arbitrary intensity

FIGURE S13: 1H NMR spectrum of polybutadiene with ≈ 0.7 mol% diethylamino functionality.

X) FigS13.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S14: 1H NMR spectrum of polybutadiene with ≈ 2.6 mol% diethylamino functionality.

Y) FigS14.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S15: 1H NMR spectrum of polybutadiene with ≈ 5.3 mol% diethylamino functionality.

Z) FigS15.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S16: 1H NMR spectrum of 26 kDa polybutadiene hydrogenated to 27 kDa PE.

AA) FigS16.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S17: 1H NMR spectrum of polybutadiene with ≈ 0.7 mol% diethylamino functionality, hydrogenated to PE.

AB) FigS17.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S18: 1H NMR spectrum of polybutadiene with ≈ 2.6 mol% diethylamino functionality, hydrogenated to PE.

AC) FigS18.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S19: 1H NMR spectrum of polybutadiene with ≈ 5.3 mol% diethylamino functionality, hydrogenated to PE.

AD) FigS19.csv

Column 1: 1H (ppm)
Column 2: signal/arbitrary intensity

FIGURE S20: SEC Traces

AE) FigS20a.csv: SEC trace of 28 kDa RAFT PS polymer before chain end removal

Column A: Elution Time (min)
Column B: RI Signal (a.u.)
Column C: Normalized RI

AF) FigS20b.csv: SEC trace of 28 kDa RAFT PS polymer after chain end removal

Column A: Elution Time (min)
Column B: RI Signal (a.u.)
Column C: Normalized RI

FIGURE S21: SEC Traces

AG) FigS21a.csv: SEC trace of PSS 1.5 mol% methylated

Column A: Elution Time (min)
Column B: RI Signal (a.u.)
Column C: Normalized RI

AH) FigS21b.csv: SEC trace of PSS 2.5 mol% methylated

Column A: Elution Time (min)
Column B: RI Signal (a.u.)
Column C: Normalized RI

AI) FigS21c.csv: SEC trace of PSS 3.5 mol% methylated

Column A: Elution Time (min)
Column B: RI Signal (a.u.)
Column C: Normalized RI

FIGURE S22: SEC Traces

AJ) FigS22a.csv: SEC trace of unfunctionalized 140 kDa PS foam

Column A: Elution Time (min)
Column B: RI Signal (a.u.)
Column C: Normalized RI

AK) FigS22b.csv: SEC trace of 3 mol% functionalized 140 kDa PSS

Column A: Elution Time (min)
Column B: RI Signal (a.u.)
Column C: Normalized RI

FIGURE S23: SEC Traces

AL) FigS23a.csv: SEC trace of unfunctionalized 470 kDa PS

Column A: Elution Time (min)
Column B: RI Signal (a.u.)
Column C: Normalized RI

AM) FigS23b.csv: SEC trace of 1.1 mol% functionalized 470 kDa PSS

Column A: Elution Time (min)
Column B: RI Signal (a.u.)
Column C: Normalized RI

FIGURE S24: Chloroform SEC traces show unfunctionalized polybutadiene (LBR-305, Kuraray) and polybutadiene samples incorporating ≈ 0.7, 2.6, and 5.3 mol% diethylamino groups.

AN) FigS24.csv

Row 1: X and Y axes, corresponding to Retention time (min) and RI Signal (a.u.)/Normalized dRI
Row 2: Polybutadiene functionalization
- dataset 1: Unfunctionalized - Retention Time (X) and RI Signal (Y) -> Columns A + B
- dataset 2: Unfunctionalized - Retention Time (X) and Normalized dRI (Y) -> Columns A + C
- dataset 3: 0.7 mol% - Retention Time (X) and RI Signal (Y) -> Columns A + D
- dataset 4: 0.7 mol% - Retention Time (X) and Normalized dRI (Y) -> Columns A + E
- dataset 5: 2.6 mol% - Retention Time (X) and RI Signal (Y) -> Columns A + F
- dataset 6: 2.6 mol% - Retention Time (X) and Normalized dRI (Y) -> Columns A + G
- dataset 7: 5.3 mol% - Retention Time (X) and RI Signal (Y) -> Columns A + H
- dataset 8: 5.3 mol% - Retention Time (X) and Normalized dRI (Y) -> Columns A + I

FIGURE S25: Thermogravimetric analysis of 26 kDa PBD (left) and 27 kDa PE (right) functionalized with varying mol% of diethylamino groups.

AO) FigS25left.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Weight %
Row 2: Polybutadiene functionalization
- dataset 1: PBD - Temperature (X) and Weight% (Y) -> Columns A + B
- dataset 2: PBD 0.7 mol% - Temperature (X) and Weight% (Y) -> Columns C + D
- dataset 3: PBD 2.6 mol% - Temperature (X) and Weight% (Y) -> Columns E + F
- dataset 4: PBD 5.3 mol% - Temperature (X) and Weight% (Y) -> Columns G + H

AP) FigS25right.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Weight %
Row 2: Polyethylene functionalization
- dataset 1: PE - Temperature (X) and Weight% (Y) -> Columns A + B
- dataset 2: PE 0.7 mol% - Temperature (X) and Weight% (Y) -> Columns A + C
- dataset 3: PE 2.6 mol% - Temperature (X) and Weight% (Y) -> Columns A + D
- dataset 4: PE 5.3 mol% - Temperature (X) and Weight% (Y) -> Columns A + E

FIGURE S26:Thermogravimetric analysis of 28 kDa PS samples functionalized with varying mol% of sulfonic acid groups.

AQ) FigS26.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Weight %
Row 2: Polystyrene functionalization
- dataset 1: PS - Temperature (X) and Weight% (Y) -> Columns A + B
- dataset 2: PS 1.5 mol% - Temperature (X) and Weight% (Y) -> Columns C + D
- dataset 3: PS 2.6 mol% - Temperature (X) and Weight% (Y) -> Columns E + F
- dataset 4: PS 3.5 mol% - Temperature (X) and Weight% (Y) -> Columns G + H

FIGURE S27: DSC of 26 kDa PBD (left) and 28 kDa PS (right) samples with varying degrees of functionalization (mol%). The third heating cycle at a ramp rate of 10 °C/min (exo up).

AR) FigS27left.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Normalized Heat Flow
Row 2: Polybutadiene functionalization
- dataset 1: PBD - Temperature (X) and Normalized Heat Flow (Y) -> Columns A + B
- dataset 2: PBD 0.7 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns C + D
- dataset 3: PBD 2.6 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns E + F
- dataset 4: PBD 5.3 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns G + H

AS) FigS27right.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Normalized Heat Flow
Row 2: Polystyrene functionalization
- dataset 1: PS - Temperature (X) and Normalized Heat Flow (Y) -> Columns A + B
- dataset 2: PS 1.5 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns C + D
- dataset 3: PS 2.6 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns E + F
- dataset 4: PS 3.5 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns G + H

FIGURE S28: DSC of 27 kDa PE samples with varying degrees of functionalization (mol%). The third heating cycle (left) and the second cooling cycle (right) at a ramp rate of 10 °C/min (exo up).

AT) FigS28left.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Normalized Heat Flow
Row 2: Polyethylene functionalization
- dataset 1: PE - Temperature (X) and Normalized Heat Flow (Y) -> Columns A + B
- dataset 2: PE 0.7 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns C + D
- dataset 3: PE 2.6 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns E + F
- dataset 4: PE 5.3 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns G + H

AU) FigS28right.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Normalized Heat Flow
Row 2: Polyethylene functionalization
- dataset 1: PE - Temperature (X) and Normalized Heat Flow (Y) -> Columns A + B
- dataset 2: PE 0.7 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns C + D
- dataset 3: PE 2.6 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns E + F
- dataset 4: PE 5.3 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns G + H

FIGURE S29: DSC traces for a series of 26 kDa PBD / 28 kDa PS blends with varying average charge. The third heating cycle at a ramp rate of 10 °C/min (exo up).

AV) FigS29: Folder: DSC curves for PBD/PS blends with varied mol% charge

Column A: Temperature (°C)
Column B: Normalized Heat Flow

FIGURE S30: SAXS Profiles

AW) FigS30a: SAXS of 28 kDa PS PBD blend

Column A: Scattering Vector, q (A^(-1))
Column B: Scattering Intensity, I(q) (arbitrary units)

AX) FigS30b: SAXS of 140 kDa PS PBD blend

Column A: Scattering Vector, q (A^(-1))
Column B: Scattering Intensity, I(q) (arbitrary units)

AY) FigS30c: SAXS of 470 kDa PS PBD blend

Column A: Scattering Vector, q (A^(-1))
Column B: Scattering Intensity, I(q) (arbitrary units)

FIGURE S31: SAXS Profiles

AZ) FigS31a: SAXS of 1 mol% charge PS PBD blend

Column A: Scattering Vector, q (A^(-1))
Column B: Scattering Intensity, I(q) (arbitrary units)

FigS31b: same data as file FigS30c (SAXS of 3 mol% charge PS PBD blend)

FIGURE S32 data are included in Table S11

FIGURE S33: Tensile Test Replicates

BA) FigS33a: Folder: Replicate stress strain curves for PBD 0.7 / PS 1.5 mol% blend

Column A: Strain (%)
Column B: Stress (MPa)

BB) FigS33b: Folder: Replicate stress strain curves for PBD 2.6 / PS 3.5 mol% blend

Column A: Strain (%)
Column B: Stress (MPa)

FIGURE S34: Tensile Test Replicates

BC) FigS34a: Folder: Replicate stress strain curves for PBD 2.6 / PS 3 mol% 140 kDa blend

Column A: Strain (%)
Column B: Stress (MPa)

BD) FigS34b: Folder: Replicate stress strain curves for commercial HIPS

Column A: Strain (%)
Column B: Stress (MPa)

FIGURE S35: Tensile Test Replicates

BE) FigS35a: Folder: Replicate stress strain curves for PBD 0.7 / PS 1.1 mol% 470 kDa blend

Column A: Strain (%)
Column B: Stress (MPa)

BF) FigS35b: Folder: Replicate stress strain curves for PBD 2.6 / PS 3.7 mol% 470 kDa blend

Column A: Strain (%)
Column B: Stress (MPa)

FIGURE S36: Tensile Test Replicates

BG) FigS36a: Folder: Replicate stress strain curves for Styrofoam packaging

Column A: Strain (%)
Column B: Stress (MPa)

BH) FigS36b: Folder: Replicate stress strain curves for 470 kDa PS

Column A: Strain (%)
Column B: Stress (MPa)

FIGURE S37: DSC analysis of 27 kDa PE / 28 kDa PS blends prepared by hot pressing with varied levels of average charge (mol%). The third heating cycle (left) and the second cooling cycle (right) at a ramp rate of 10 °C/min (exo up).

BI) FigS37left.csv:

Row 1: X and Y axes, corresponding to Temperature (°C) and Normalized Heat Flow
Row 2: Average charge of the PE/PS blend
- dataset 1: Unfunctionalized - Temperature (X) and Normalized Heat Flow (Y) -> Columns A + B
- dataset 2: 1 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns C + D
- dataset 3: 2.6 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns E + F
- dataset 4: 4 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns G + H

BJ) FigS37right.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Normalized Heat Flow
Row 2: Average charge of the PE/PS blend
- dataset 1: Unfunctionalized - Temperature (X) and Normalized Heat Flow (Y) -> Columns A + B
- dataset 2: 1 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns C + D
- dataset 3: 2.6 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns E + F
- dataset 4: 4 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns G + H

FIGURE S38: DSC analysis of 27 kDa PE / 28 kDa PS blends prepared by drop-casting with varied levels of average charge (mol%). The third heating cycle (left) and the second cooling cycle (right) at a ramp rate of 10 °C/min (exo up).

BK) FigS38left.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Normalized Heat Flow
Row 2: Average charge of the PE/PS blend
- dataset 1: Unfunctionalized - Temperature (X) and Normalized Heat Flow (Y) -> Columns A + B
- dataset 2: 1 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns C + D
- dataset 3: 2.6 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns E + F
- dataset 4: 4 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns G + H

BL) FigS38right.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Normalized Heat Flow
Row 2: Average charge of the PE/PS blend
- dataset 1: Unfunctionalized - Temperature (X) and Normalized Heat Flow (Y) -> Columns A + B
- dataset 2: 1 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns C + D
- dataset 3: 2.6 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns E + F
- dataset 4: 4 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns G + H

FIGURE S39: DSC analysis of 27 kDa PE / 28 kDa PS blends prepared by drop-casting & hot pressing with varied levels of average charge (mol%). The third heating cycle (left) and the second cooling cycle (right) at a ramp rate of 10 °C/min (exo up).

BM) FigS39left.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Normalized Heat Flow
Row 2: Average charge of the PE/PS blend
- dataset 1: Unfunctionalized - Temperature (X) and Normalized Heat Flow (Y) -> Columns A + B
- dataset 2: 1 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns C + D
- dataset 3: 2.6 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns E + F
- dataset 4: 4 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns G + H

BN) FigS39right.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Normalized Heat Flow
Row 2: Average charge of the PE/PS blend
- dataset 1: Unfunctionalized - Temperature (X) and Normalized Heat Flow (Y) -> Columns A + B
- dataset 2: 1 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns C + D
- dataset 3: 2.6 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns E + F
- dataset 4: 4 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns G + H

FIGURE S40left: Percent crystallinity trends of 27 kDa PE / 28 kDa PS blends prepared using different processing techniques as a function of the average charge of blend components (left).

BO) FigS40left.csv

Row 1: X and Y axes, corresponding to Average Charge of Blend Components and Percent Crystallinity (%) with STDEV.S
Row 2: Processing technique
- dataset 1: Theoretical - Average Charge of Blend Components (X) and Percent Crystallinity with STDEV.S (Y) -> Columns A + B + C
- dataset 2: Hot-Pressed - Average Charge of Blend Components (X) and Percent Crystallinity with STDEV.S (Y) -> Columns A + D + E
- dataset 3: Drop-Cast - Average Charge of Blend Components (X) and Percent Crystallinity with STDEV.S (Y) -> Columns A + F + G
- dataset 4: Drop-Cast & Hot-Press - Average Charge of Blend Components (X) and Percent Crystallinity with STDEV.S (Y) -> Columns A + H + I

FIGURE S41: Overlaid image of DSC analysis of 27 kDa PE with 0.7 mol% of base groups, 140 kDa PS with 3 mol% sulfonic acid groups, and their corresponding blend with 1.4 mol% average charge, prepared by drop-casting. The third heating cycle (left) and the second cooling cycle (right) at a ramp rate of 10 °C/min (exo up).

BP) FigS41left.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Normalized Heat Flow
Row 2: Type of polymer/blend
- dataset 1: PS 3 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns A + B
- dataset 2: PE 0.7 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns C + D
- dataset 3: PE/PS 1.4 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns E + F

BQ) FigS41right.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Normalized Heat Flow
Row 2: Type of polymer/blend
- dataset 1: PS 3 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns A + B
- dataset 2: PE 0.7 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns C + D
- dataset 3: PE/PS 1.4 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns E + F

FIGURE S42: Overlaid image of DSC analysis of 27 kDa PE / 140 kDa PS blend with average charge of 1.4 mol% prepared by drop-casting and corresponding blends after each reprocessing cycle. The third heating cycle (left) and the second cooling cycle (right) at a ramp rate of 10 °C/min (exo up).

BR) FigS42left.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Normalized Heat Flow
Row 2: Type of blend
- dataset 1: PE/PS 1.4 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns A + B
- dataset 2: REP1 - Temperature (X) and Normalized Heat Flow (Y) -> Columns C + D
- dataset 3: REP2 - Temperature (X) and Normalized Heat Flow (Y) -> Columns E + F
- dataset 4: REP3 - Temperature (X) and Normalized Heat Flow (Y) -> Columns G + H

BS) FigS42right.csv

Row 1: X and Y axes, corresponding to Temperature (°C) and Normalized Heat Flow
Row 2: Type of blend
- dataset 1: PE/PS 1.4 mol% - Temperature (X) and Normalized Heat Flow (Y) -> Columns A + B
- dataset 2: REP1 - Temperature (X) and Normalized Heat Flow (Y) -> Columns C + D
- dataset 3: REP2 - Temperature (X) and Normalized Heat Flow (Y) -> Columns E + F
- dataset 4: REP3 - Temperature (X) and Normalized Heat Flow (Y) -> Columns G + H

FIGURE S43 data are included in table S18

FIGURE S44: Tensile Test Replicates

BT) FigS44a: Folder: Replicate stress strain curves for PE 0.7 / PS 3 mol% 140 kDa drop cast blend

Column A: Strain (%)
Column B: Stress (MPa)

BU) FigS44b: Folder: Replicate stress strain curves for PE 0.7 / PS 3 mol% 140 kDa drop cast blend and hot pressed

Column A: Strain (%)
Column B: Stress (MPa)

BV) FigS44c: Folder: Replicate stress strain curves for PE 0.7 / PS 3 mol% 140 kDa drop cast blend and hot pressed x2

Column A: Strain (%)
Column B: Stress (MPa)

BW) FigS44d: Folder: Replicate stress strain curves for PE 0.7 / PS 3 mol% 140 kDa drop cast blend and hot pressed x3

Column A: Strain (%)
Column B: Stress (MPa)

FIGURE S45: Tensile Test Replicates

BX) FigS45: Folder: Replicate stress strain curves for PE (hydrogenated PBD)

Column A: Strain (%)
Column B: Stress (MPa)