Data from: Alkylidene functionalization produces highly recyclable and scalable polyhydroxyalkanoates
Data files
Apr 23, 2026 version files 22.85 MB
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Excel_S1.xlsx
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Excel_S2.xlsx
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Excel_S3.xlsx
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fig._S10.xlsx
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fig._S11.xlsx
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fig._S12.xlsx
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fig._S13.xlsx
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fig._S15.xlsx
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fig._S17.xlsx
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fig._S18.xlsx
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fig._S19.xlsx
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fig._S5.xlsx
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fig._S9.xlsx
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NMR_data.7z
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README.md
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Tabel_S12.xlsx
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Abstract
Recyclable polymers that can be produced at scale and readily tuned within the same polymer framework for specific properties is critical to achieving a circular materials economy. To this end, synthetic poly(3-hydroxyalkanoate)s (PHAs) have emerged as high-performance, chemically-recyclable variants of biological PHAs, but their difficult monomer syntheses and sub-optimal recycling efficiencies pose challenges for large-scale deployment. Here, we investigate a β-isopropylidene PHA, i-PHA, for which the lactone monomer can be synthesized by existing industrial methods from biomass-derived isobutyric acid. The alkylidene substituent prevents decarboxylative degradation typically observed during PHA depolymerization, enabling near-quantitative chemical recycling to monomer. Controlled hydrogenation of the β-isopropylidene side group produces PHAs with diverse performance metrics competitive with a range of commodity polymers, spanning strong fibers to ductile thermoplastics to superglue epoxy resins.
Dataset DOI: 10.5061/dryad.r7sqv9ssg
Description of the data and file structure
This data set contains the tabulated data for all plots displayed graphically in the article: Alkylidene functionalization produces highly recyclable and scalable polyhydroxyalkanoates and the associated supplementary information file. This includes raw data files for DSC, TGA, GPC, rheology, tensile analyses, UV-Vis, computational models, NMR files, etc. Files are labeled according to their reference labels in the associated article.
Files and variables
File: NMR_data.7z
Description: zip file containing 1H and 13C NMR spectra for all compounds and polymers reported in the article. After extracting the compressed files, the spectra contained within the Revision-NMR-fid folder may be viewed using Mestre Nova or similar software for viewing NMR spectra; e.g., TopSpin or NMRium.
File: Excel_S1.xlsx
Description: tabulated data for graphs displayed in Fig. 2 of the main article. Spreadsheet pages are labeled according to their labels in Fig. 2 of the main article. Pages found in the spreadsheet are described as follows: 2B - Differential Scanning Calorimetry (DSC) curves of 1st cooling and 2nd heating scans of P3H(Me)2iPP. Temperature is given in Celsius and heat flow is given in W/g. 2C - Thermal Gravimetric Analysis (TGA) and derivative TGA curves of P3H(Me)2iPP. Temperature is given in Celsius and weight loss is given as a percentage. 2D - Cyclic frequency sweeps of P3H(Me)2iPP under N2 (repeated every 20 min, total 100 min), 0.1 to 628 rad/s, 5 % strain, 220 °C), showing good melt processability. 2E - The viscosity value at 10 rad/s over time for P3H(Me)2iPP at different processing conditions (x % Irganox, air or N2 ). Viscosity was normalized with respect to the 0-min viscosity data collected when running in N2. 2G - DSC curves of first heating cycle of P3H(Me)2iPP fibers pre- and post annealing. Scan rate of 2°C/min in an N2 environment (exo-up). 8 m/min fibers as- spun. 2H - Tensile testing results for P3H(Me)2iPP monofilament fibers pre- and post annealing, tested at a strain rate of 250 m/min.
File: Excel_S3.xlsx
Description: tabulated data for graphs displayed in Fig. 4 of the main article. This figure shows a process model for the production of P3H(Me)2iPP and an associated technoeconomic analysis spreadsheet pages are labeled according to their labels in Fig. 4 of the main article. Pages found in the spreadsheet are described as follows: 4B - Breakdown of the capital expenses by process area. TIC, total installed equipment cost; OSBL, outside battery limits (which is taken to be 25 % of the inside battery limits costs); MM, million USD. 4C - Breakdown of the minimum selling price (MSP) of P3H(Me)2iPP. 4D - Sensitivity analysis demonstrating the impact of process and TEA parameters on the MSP. Parameter values for the sensitivity are shown beside the variable name in parenthesis in the following order: optimistic case (blue), base case, pessimistic case (orange). All costs are given in 2024 USD.
File: Excel_S2.xlsx
Description: tabulated data for graphs displayed in Fig. 3 of the main article. This figure shows tensile and adhesion data for P3H(Me)2iPP at varying saturation levels as well as a computational analysis of the chemical recycling of P3H(Me)2iPP. Spreadsheet pages are labeled according to their labels in Fig. 3 of the main article. Pages found in the spreadsheet are described as follows: 3A -Representative stress-strain curves of P3H(Me)2iPP, 42 % hydrogenated P3H(Me)2iPP, 84 % hydrogenated P3H(Me)2iPP and virgin PET. Strain is measure as % displacement while stress is measure in MPa. 3B - Representative stress- strain curves of P3H(Me)2iPrP and it-PP. Strain is measure as % displacement while stress is measure in MPa. 3C -Adhesion performance of unsaturated and saturated PHAs compared with PU, EVA and it-PP hot- melt adhesives. Adhesion strength is measured in MPa.
File: fig._S5.xlsx
Description: UV-Visible Transmittance overlays of P3H(Me)2iPP, Ziplok bag (LDPE), and it-P3HB. Wavelength is given in nm while transmittance is given as % transmittance. Retention time is given in minutes while light scattering data is given in a.u.
File: fig._S9.xlsx
Description: Size exclusion chromatogram (SEC) trace (chloroform) of P3H(Me)2iPP produced by a [(Me)2iPPL]/[tBu-P4] ratio of 1600:1. Retention time is given in minutes while light scattering data is given in a.u.
File: fig._S10.xlsx
Description: Size exclusion chromatogram (SEC) trace (chloroform) of P3H(Me)2iPP/iPrP (58/42) prepared from hydrogenation of P3H(Me)2iPP. Retention time is given in minutes while light scattering data is given in a.u.
File: fig._S11.xlsx
Description: Size exclusion chromatogram (SEC) trace (chloroform) of P3H(Me)2iPrP prepared from hydrogenation of P3H(Me)2iPP. Retention time is given in minutes while light scattering data is given in a.u.
File: fig._S13.xlsx
Description: Tensile stress-strain for P3H(Me)2iPP/iPrP (58/42, Mn = 306 kDa, Ð = 1.27) prepared from hydrogenation of P3H(Me)2iPP (Mn = 322 kDa, Ð = 1.24), strain rate = 5 mm/min, ambient condition. Strain is measure as % displacement while stress is measure in MPa.
File: fig._S12.xlsx
Description: Tensile stress-strain for P3H(Me)2iPP (Mn = 492 kDa, Ð = 1.11) produced by a [(Me)2iPPL]:[tBu-P4] ratio of 1600:1, after melting at 220 ºC under nitrogen, strain rate = 5 mm/min, ambient condition. Strain is measure as % displacement while stress is measure in MPa.
File: fig._S16.xlsx
Description: Differential Scanning Calorimetry (DSC) curves of 1st cooling and 2nd heating scans of virgin PET chips. Scan rate: 10 ºC/min. Temperature is given in Celsius and heat flow is given in W/g.
File: fig._S14.xlsx
Description: Tensile stress-strain for P3H(Me)2iPP/iPrP (16/84, Mn = 325 kDa, Ð = 1.47) prepared from hydrogenation of P3H(Me)2iPP (Mn = 322 kDa, Ð = 1.24), strain rate = 5 mm/min, ambient condition. Strain is measure as % displacement while stress is measure in MPa.
File: fig._S17.xlsx
Description: Differential Scanning Calorimetry (DSC) curves of second heating scans of P3H(Me)2iPP (Mn = 492 kDa) and virgin PET chips. Scan rate: 10 °C/min, Temperature is given in Celsius and heat flow is given in W/g.
File: fig._S15.xlsx
Description: Tensile stress-strain for P3H(Me)2iPrP (Mn = 304 kDa, Ð = 1.41) prepared from hydrogenation of P3H(Me)2iPP (Mn = 322 kDa, Ð = 1.24), strain rate = 5 mm/min, ambient condition. Strain is measure as % displacement while stress is measure in MPa.
File: fig._S19.xlsx
Description: Differential Scanning Calorimetry (DSC) curves of first heating scans of P3H(Me)2iPrP (Mn = 304 kDa) and second heating scans of it-PP. Scan rate: 10 °C/min. Temperature is given in Celsius and heat flow is given in W/g.
File: fig._S20.xlsx
Description: Differential Scanning Calorimetry (DSC) curves of 1st heating (black), 1st cooling, and 2nd heating scans of P3H(Me)2iPP/iPrP (58/42, Mn = 306 kDa, Ð = 1.27) prepared from hydrogenation of P3H(Me)2iPP. Scan rate: 10 ºC/min. Temperature is given in Celsius and heat flow is given in W/g.
File: fig._S18.xlsx
Description: Differential Scanning Calorimetry (DSC) curves of 1st cooling and 2nd heating scans of it-PP. Scan rate: 10 ºC/min. Temperature is given in Celsius and heat flow is given in W/g.
File: fig._S23.xlsx
Description: Thermal Gravimetric Analysis (TGA) and derivative TGA curves of P3H(Me)2iPrP (Mn = 304 kDa, Ð = 1.41) prepared from hydrogenation of P3H(Me)2iPP (Mn = 322 kDa, Ð = 1.24). Temperature is given in Celsius and weight loss is given as a percentage.
File: fig._S22.xlsx
Description: Thermal Gravimetric Analysis (TGA) and derivative TGA curves of P3H(Me)2iPP/iPrP (58/42, Mn = 306 kDa, Ð = 1.27) prepared from hydrogenation of P3H(Me)2iPP (Mn = 322 kDa, Ð = 1.24). Temperature is given in Celsius and weight loss is given as a percentage.
File: fig._S25.xlsx
Description: Oscillatory frequency sweep of P3H(Me)2iPrP at 120 ºC. Storage and loss moduli are measured in Pa, complex viscosity is measured in Pa*s, and angular frequency is measure in rad/s.
File: fig._S26.xlsx
Description: Oscillatory frequency sweeps at 70 °C of P3H(Me)2iPrP. Storage and loss moduli are measured in Pa and angular frequency is measure in rad/s.
File: fig._S27.xlsx
Description: Oscillatory frequency sweeps at 90 °C of PU. Storage and loss moduli are measured in Pa and angular frequency is measure in rad/s.
File: fig._S29.xlsx
Description: Frequency sweeps of P3H(Me)2iPrP from 60 – 150 °C. Storage and loss moduli are measured in Pa and angular frequency is measure in rad/s.
File: fig._S30.xlsx
Description: Frequency sweeps of EVA from 30 – 70 °C. Storage and loss moduli are measured in Pa and angular frequency is measure in rad/s.
File: fig._S31.xlsx
Description: Frequency sweeps of PU from 90 – 130 °C. Storage and loss moduli are measured in Pa and angular frequency is measure in rad/s.
File: fig._S21.xlsx
Description: Differential Scanning Calorimetry (DSC) curves of 1st heating, 1st cooling (black), and 2nd heating scans of P3H(Me)2iPrP (Mn = 304 kDa, Ð = 1.41) prepared from hydrogenation of P3H(Me)2iPP. Scan rate: 10 ºC/min. Temperature is given in Celsius and heat flow is given in W/g.
File: fig._S34.xlsx
Description: Size exclusion chromatogram (SEC) trace (chloroform) of P3H(Me)2iPP reproduced from the recovered monomer (Me)2iPPL with a [(Me)2iPPL]:[tBu-P4] ratio of 1600:1, Mn = 434 kDa, Đ = 1.10. Retention time is given in minutes while light scattering data is given in a.u.
File: fig._S28.xlsx
Description: Oscillatory frequency sweeps at 110 °C of it-PP. Storage and loss moduli are measured in Pa and angular frequency is measure in rad/s.
File: fig._S36.xlsx
Description: Size exclusion chromatogram (SEC) trace (chloroform) of P3H(Me)2iPrP reproduced from the recovered monomer (Me)2iPrPL with a [(Me)2iPrPL]:[tBu-P4] ratio of 800:1, Mn = 141 kDa, Đ = 1.01. Retention time is given in minutes while light scattering data is given in a.u.
File: fig._S32.xlsx
Description: Frequency sweeps of itPP from 90 – 150 & 170 °C. Storage and loss moduli are measured in Pa and angular frequency is measure in rad/s.
File: fig._S24.xlsx
Description: Adhesion behavior of P3H(Me)2iPrP (Mn = 304 kDa, Ð = 1.41) on steel, aluminum and wood. Adhesion strength is measured in MPa.
File: Tabel_S4.xlsx
Description: Energies of the optimized structures during dimer-(R)-3HB decomposition.
File: Tabel_S5.xlsx
Description: Energies of the optimized structures during trimer-3H(Me)2iPP decomposition
File: Tabel_S12.xlsx
Description: DFT analysis of the depolymerization of P3H(Me)2iPP. Energies of the optimized structures – depolymerization pathways of trimer-3H(Me)2iPP
File: Tabel_S13.xlsx
Description: DFT analysis of the depolymerization of P3H(Me)2iPrP. Energies of the optimized structures – depolymerization for trimer-3H(Me)2iPrP to CO2
File: Tabel_S14.xlsx
Description: DFT analysis of the decarboxylation of P3H(Me)2iPrP. Energies of the optimized structures – depolymerization for trimer-3H(Me)2iPP to CO2
Code/software
Microsoft Excel
MestReNova, Bruker TopSpin, NMRium, or other NMR software