Abstract

Inter- and intramolecular interactions in multicomponent polymer systems influence their physical and chemical properties significantly and thus have implications on their synthesis and processing. In the present study, chemical images were obtained by plotting the peak position of a spectral band from the data sets generated using in situ attenuated total reflection Fourier transform infrared (ATR FT-IR) spectroscopic imaging. This approach was successfully used to visualize changes in intra- and intermolecular interactions in poly(3-hydroxybutyrate)/poly(L-lactic acid) (PHB/PLLA) blends during the isothermal melt crystallization. The peak position of ν(C=O) band, which reflects the nature of the intermolecular interaction, shows that the intermolecular interactions between PHB and PLLA in the miscible state (1733 cm−1) changes to the inter- and intramolecular interaction (CH3⋯O=C, 1720 cm−1) within PHB crystal during the isothermal melt crystallization. Compared with spectroscopic images obtained by plotting the distribution of absorbance of spectral bands, which reveals the spatial distribution of blend components, the approach of plotting the peak position of a spectral band reflects the spatial distribution of different intra- and intermolecular interactions. With the process of isothermal melt-crystallization, the disappearance of the intermolecular interaction between PHB and PLLA and the appearance of the inter- and intramolecular interactions within the PHB crystal were both visualized through the images based on the observation of the band position. This work shows the potential of using in-situ ATR FT-IR spectroscopic imaging to visualize different types of inter- or intramolecular interactions between polymer molecules or between polymer and other additives in various types of multicomponent polymer systems.

© 2021 The Author(s)

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  21. E. Blümm, A.J. Owen. “Miscibility, Crystallization and Melting of Poly(3-hydroxybutyrate)/Poly(L-Lactide) Blends”. Polymer. 1995. 36(21): 4077–4081.
  22. N. Koyama, Y. Doi. “Miscibility of Binary Blends of Poly(R)-3-hydroxybutyric Acid, and Poly(S)-Lactic Acid]”. Polymer. 1997. 38(7): 1589–1593.
  23. C. Vogel, E. Wessel, H.W. Siesler. “FT-IR Imaging Spectroscopy of Phase Separation in Blends of Poly(3-hydroxybutyrate) with Poly(L-lactic Acid) and Poly(ɛ-caprolactone)”. Biomacromolecules. 2008. 9(2): 523–527.
  24. H. Lu, S.G. Kazarian, H. Sato. “Simultaneous Visualization of Phase Separation and Crystallization in PHB/PLLA Blends with In Situ ATR-FTIR Spectroscopic Imaging”. Macromolecules. 2020. 53(20): 9074–9085.
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  26. H. Shinzawa, K. Awa, Y. Ozaki, et al. “Near-Infrared Imaging Analysis of Cellulose Tablet by a Band Position Shift”. Appl. Spectrosc. 2009. 63(8): 974–977.
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  29. A.V. Ewing, S.G. Kazarian. “Infrared Spectroscopy and Spectroscopic Imaging in Forensic Science”. Analyst. 2017. 142(2): 257–272.
  30. H. Lu, H. Shinzawa, S.G. Kazarian. “Intermolecular Interactions in the Polymer Blends Under High-Pressure CO2 Studied Using Two-Dimensional Correlation Analysis and Two-Dimensional Disrelation Mapping”. Appl. Spectrosc. 2021. 75(3): 250–258.
  31. H. Lu, S.G. Kazarian. “How Does High-Pressure CO2 Affect the Morphology of PCL/PLA Blends? Visualization of Phase Separation Using In Situ ATR-FTIR Spectroscopic Imaging”. Spectrochim. Acta, Part. A. 2020. 243: 118760.
  32. C.L. Song, S.G. Kazarian. “Effect of Controlled Humidity and Tissue Hydration on Colon Cancer Diagnostic via FTIR Spectroscopic Imaging”. Anal. Chem. 2020. 92(14): 9691–9698.
  33. K.L.A. Chan, A. Altharawi, F. Fale, et al. “Transmission Fourier Transform Infrared Spectroscopic Imaging, Mapping, and Synchrotron Scanning Microscopy with Zinc Sulfide Hemispheres on Living Mammalian Cells at Sub-Cellular Resolution”. Appl. Spectrosc. 2020. 74(5): 544–552.
  34. P. Lasch, I. Noda. “Two-Dimensional Correlation Spectroscopy (2D-COS) for Analysis of Spatially Resolved Vibrational Spectra”. Appl. Spectrosc. 2019. 73(4): 359–379.
  35. Y. Hikima, J. Morikawa, S.G. Kazarian. “Analysis of Molecular Orientation in Polymeric Spherulite Using Polarized Micro Attenuated Total Reflection Fourier Transform Infrared (ATR-FTIR) Spectroscopic Imaging”. Anal. Chim. Acta. 2019. 1065: 79–89.
  36. T. Furukawa, H. Sato, R. Murakami, et al. “Structure, Dispersibility, and Crystallinity of Poly(Hydroxybutyrate)/Poly(L-Lactic Acid) Blends Studied by FT-IR Microspectroscopy and Differential Scanning Calorimetry”. Macromolecules. 2005. 38(15): 6445–6454.

2021 (1)

H. Lu, H. Shinzawa, S.G. Kazarian. “Intermolecular Interactions in the Polymer Blends Under High-Pressure CO2 Studied Using Two-Dimensional Correlation Analysis and Two-Dimensional Disrelation Mapping”. Appl. Spectrosc. 2021. 75(3): 250–258.

2020 (4)

H. Lu, S.G. Kazarian. “How Does High-Pressure CO2 Affect the Morphology of PCL/PLA Blends? Visualization of Phase Separation Using In Situ ATR-FTIR Spectroscopic Imaging”. Spectrochim. Acta, Part. A. 2020. 243: 118760.

C.L. Song, S.G. Kazarian. “Effect of Controlled Humidity and Tissue Hydration on Colon Cancer Diagnostic via FTIR Spectroscopic Imaging”. Anal. Chem. 2020. 92(14): 9691–9698.

K.L.A. Chan, A. Altharawi, F. Fale, et al. “Transmission Fourier Transform Infrared Spectroscopic Imaging, Mapping, and Synchrotron Scanning Microscopy with Zinc Sulfide Hemispheres on Living Mammalian Cells at Sub-Cellular Resolution”. Appl. Spectrosc. 2020. 74(5): 544–552.

H. Lu, S.G. Kazarian, H. Sato. “Simultaneous Visualization of Phase Separation and Crystallization in PHB/PLLA Blends with In Situ ATR-FTIR Spectroscopic Imaging”. Macromolecules. 2020. 53(20): 9074–9085.

2019 (2)

P. Lasch, I. Noda. “Two-Dimensional Correlation Spectroscopy (2D-COS) for Analysis of Spatially Resolved Vibrational Spectra”. Appl. Spectrosc. 2019. 73(4): 359–379.

Y. Hikima, J. Morikawa, S.G. Kazarian. “Analysis of Molecular Orientation in Polymeric Spherulite Using Polarized Micro Attenuated Total Reflection Fourier Transform Infrared (ATR-FTIR) Spectroscopic Imaging”. Anal. Chim. Acta. 2019. 1065: 79–89.

2017 (1)

A.V. Ewing, S.G. Kazarian. “Infrared Spectroscopy and Spectroscopic Imaging in Forensic Science”. Analyst. 2017. 142(2): 257–272.

2016 (1)

H. Tsuji. “Poly(Lactic Acid) Stereocomplexes: A Decade of Progress”. Adv. Drug Deliv. Rev. 2016. 107(15): 97–135.

2014 (1)

C. Peña, T. Castillo, A. García, et al. “Biotechnological Strategies to Improve Production of Microbial Poly-(3-hydroxybutyrate): A Review of Recent Research Work”. Microb. Biotechnol. 2014. 7(4): 278–293.

2012 (1)

M.A. Abdelwahab, A. Flynn, B.-S. Chiou, et al. “Thermal, Mechanical and Morphological Characterization of Plasticized PLA–PHB Blends”. Polym. Degrad. Stab. 2012. 97(9): 1822–1828.

2011 (3)

L. Guo, H. Sato, T. Hashimoto, et al. “Thermally Induced Exchanges of Hydrogen Bonding Interactions and Their Effects on Phase Structures of Poly(3-hydroxybutyrate) and Poly(4-Vinylphenol) Blends”. Macromolecules. 2011. 44(7): 2229–2239.

N. Suttiwijitpukdee, H. Sato, J. Zhang, et al. “Effects of Intermolecular Hydrogen Bondings on Isothermal Crystallization Behavior of Polymer Blends of Cellulose Acetate Butyrate and Poly(3-hydroxybutyrate)”. Macromolecules. 2011. 44(9): 3467–3477.

H. Shinzawa, K. Awa, Y. Ozaki. “Compression-Induced Morphological and Molecular Structural Changes in Cellulose Tablets Probed by Near-Infrared Imaging”. J. Near Infrared Spectrosc. 2011. 19(1): 15–22.

2010 (1)

L. Guo, H. Sato, T. Hashimoto, et al. “FTIR Study on Hydrogen-Bonding Interactions in Biodegradable Polymer Blends of Poly(3-hydroxybutyrate) and Poly(4-Vinylphenol)”. Macromolecules. 2010. 43(8): 3897–3902.

2009 (1)

H. Shinzawa, K. Awa, Y. Ozaki, et al. “Near-Infrared Imaging Analysis of Cellulose Tablet by a Band Position Shift”. Appl. Spectrosc. 2009. 63(8): 974–977.

2008 (2)

C. Vogel, E. Wessel, H.W. Siesler. “FT-IR Imaging Spectroscopy of Phase Separation in Blends of Poly(3-hydroxybutyrate) with Poly(L-lactic Acid) and Poly(ɛ-caprolactone)”. Biomacromolecules. 2008. 9(2): 523–527.

H. Sato, Y. Ando, J. Dybal, et al. “Crystal Structures, Thermal Behaviors, and C–H···O=C Hydrogen Bondings of Poly(3-hydroxyvalerate) and Poly(3-hydroxybutyrate) Studied by Infrared Spectroscopy and X-ray Diffraction”. Macromolecules. 2008. 41(12): 4305–4312.

2007 (1)

K.L.A. Chan, S.G. Kazarian, D. Vassou, et al. “In Situ High-Throughput Study of Drug Polymorphism Under Controlled Temperature and Humidity Using FT-IR Spectroscopic Imaging”. Vib. Spectrosc. 2007. 43(1): 221–226.

2006 (2)

J. Zhang, H. Sato, T. Furukawa, et al. “Crystallization Behaviors of Poly(3-hydroxybutyrate) and Poly(L-Lactic Acid) in Their Immiscible and Miscible Blends”. J. Phys. Chem. B. 2006. 110(48): 24463–24471.

H. Sato, K. Mori, R. Murakami, et al. “Crystal and Lamella Structure and C–H···O=C Hydrogen Bonding of Poly(3-hydroxyalkanoate) Studied by X-ray Diffraction and Infrared Spectroscopy”. Macromolecules. 2006. 39(4): 1525–1531.

2005 (2)

M. Vert. “Aliphatic Polyesters: Great Degradable Polymers That Cannot Do Everything”. Biomacromolecules. 2005. 6(2): 538–546.

T. Furukawa, H. Sato, R. Murakami, et al. “Structure, Dispersibility, and Crystallinity of Poly(Hydroxybutyrate)/Poly(L-Lactic Acid) Blends Studied by FT-IR Microspectroscopy and Differential Scanning Calorimetry”. Macromolecules. 2005. 38(15): 6445–6454.

2004 (3)

H. Sato, M. Nakamura, A. Padermshoke, et al. “Thermal Behavior and Molecular Interaction of Poly(3-hydroxybutyrate-Co-3-Hydroxyhexanoate) Studied by Wide-Angle X-ray Diffraction”. Macromolecules. 2004. 37(10): 3763–3769.

H. Sato, R. Murakami, A. Padermshoke, et al. “Infrared Spectroscopy Studies of CH···O Hydrogen Bondings and Thermal Behavior of Biodegradable Poly(hydroxyalkanoate)”. Macromolecules. 2004. 37(19): 7203–7213.

I. Noda, M.M. Satkowski, A.E. Dowrey, et al. “Polymer Alloys of Nodax Copolymers and Poly(Lactic Acid)”. Macromol. Biosci. 2004. 4(3): 269–275.

2002 (1)

H. Urayama, T. Kanamori, Y. Kimura. “Properties and Biodegradability of Polymer Blends of Poly(L–lactide)S with Different Optical Purity of the Lactate Units”. Macromol. Mater. Eng. 2002. 287(2): 116–121.

2000 (1)

I. Ohkoshi, H. Abe, Y. Doi. “Miscibility and Solid-State Structures for Blends of Poly(S)-Lactide with Atactic Poly(R,S)-3-hydroxybutyrate]”. Polymer. 2000. 41(15): 5985–5992.

1997 (1)

N. Koyama, Y. Doi. “Miscibility of Binary Blends of Poly(R)-3-hydroxybutyric Acid, and Poly(S)-Lactic Acid]”. Polymer. 1997. 38(7): 1589–1593.

1995 (1)

E. Blümm, A.J. Owen. “Miscibility, Crystallization and Melting of Poly(3-hydroxybutyrate)/Poly(L-Lactide) Blends”. Polymer. 1995. 36(21): 4077–4081.

1990 (1)

A.J. Anderson, E.A. Dawes. “Occurrence, Metabolism, Metabolic Role, and Industrial Uses of Bacterial Polyhydroxyalkanoates”. Microbiol. Rev. 1990. 54(4): 450–472.

Abdelwahab, M.A.

M.A. Abdelwahab, A. Flynn, B.-S. Chiou, et al. “Thermal, Mechanical and Morphological Characterization of Plasticized PLA–PHB Blends”. Polym. Degrad. Stab. 2012. 97(9): 1822–1828.

Abe, H.

I. Ohkoshi, H. Abe, Y. Doi. “Miscibility and Solid-State Structures for Blends of Poly(S)-Lactide with Atactic Poly(R,S)-3-hydroxybutyrate]”. Polymer. 2000. 41(15): 5985–5992.

Altharawi, A.

K.L.A. Chan, A. Altharawi, F. Fale, et al. “Transmission Fourier Transform Infrared Spectroscopic Imaging, Mapping, and Synchrotron Scanning Microscopy with Zinc Sulfide Hemispheres on Living Mammalian Cells at Sub-Cellular Resolution”. Appl. Spectrosc. 2020. 74(5): 544–552.

Anderson, A.J.

A.J. Anderson, E.A. Dawes. “Occurrence, Metabolism, Metabolic Role, and Industrial Uses of Bacterial Polyhydroxyalkanoates”. Microbiol. Rev. 1990. 54(4): 450–472.

Ando, Y.

H. Sato, Y. Ando, J. Dybal, et al. “Crystal Structures, Thermal Behaviors, and C–H···O=C Hydrogen Bondings of Poly(3-hydroxyvalerate) and Poly(3-hydroxybutyrate) Studied by Infrared Spectroscopy and X-ray Diffraction”. Macromolecules. 2008. 41(12): 4305–4312.

Auras, R.

R. Auras, L.-T. Lim, S.E.M. Selke, et al. Poly(Lactic Acid): Synthesis, Structures, Properties, Processing, and Applications., Hoboken, NJ: Wiley, 2010.

Awa, K.

H. Shinzawa, K. Awa, Y. Ozaki. “Compression-Induced Morphological and Molecular Structural Changes in Cellulose Tablets Probed by Near-Infrared Imaging”. J. Near Infrared Spectrosc. 2011. 19(1): 15–22.

H. Shinzawa, K. Awa, Y. Ozaki, et al. “Near-Infrared Imaging Analysis of Cellulose Tablet by a Band Position Shift”. Appl. Spectrosc. 2009. 63(8): 974–977.

Bastioli, C.

C. Bastioli. Handbook of Biodegradable Polymers., UK: Rapra Technology Limited, 2005.

Blümm, E.

E. Blümm, A.J. Owen. “Miscibility, Crystallization and Melting of Poly(3-hydroxybutyrate)/Poly(L-Lactide) Blends”. Polymer. 1995. 36(21): 4077–4081.

Castillo, T.

C. Peña, T. Castillo, A. García, et al. “Biotechnological Strategies to Improve Production of Microbial Poly-(3-hydroxybutyrate): A Review of Recent Research Work”. Microb. Biotechnol. 2014. 7(4): 278–293.

Chan, K.L.A.

K.L.A. Chan, A. Altharawi, F. Fale, et al. “Transmission Fourier Transform Infrared Spectroscopic Imaging, Mapping, and Synchrotron Scanning Microscopy with Zinc Sulfide Hemispheres on Living Mammalian Cells at Sub-Cellular Resolution”. Appl. Spectrosc. 2020. 74(5): 544–552.

K.L.A. Chan, S.G. Kazarian, D. Vassou, et al. “In Situ High-Throughput Study of Drug Polymorphism Under Controlled Temperature and Humidity Using FT-IR Spectroscopic Imaging”. Vib. Spectrosc. 2007. 43(1): 221–226.

Chiou, B.-S.

M.A. Abdelwahab, A. Flynn, B.-S. Chiou, et al. “Thermal, Mechanical and Morphological Characterization of Plasticized PLA–PHB Blends”. Polym. Degrad. Stab. 2012. 97(9): 1822–1828.

Dawes, E.A.

A.J. Anderson, E.A. Dawes. “Occurrence, Metabolism, Metabolic Role, and Industrial Uses of Bacterial Polyhydroxyalkanoates”. Microbiol. Rev. 1990. 54(4): 450–472.

Doi, Y.

I. Ohkoshi, H. Abe, Y. Doi. “Miscibility and Solid-State Structures for Blends of Poly(S)-Lactide with Atactic Poly(R,S)-3-hydroxybutyrate]”. Polymer. 2000. 41(15): 5985–5992.

N. Koyama, Y. Doi. “Miscibility of Binary Blends of Poly(R)-3-hydroxybutyric Acid, and Poly(S)-Lactic Acid]”. Polymer. 1997. 38(7): 1589–1593.

Doi, A, Y.

Y. Doi, ASteinbüchel. Biopolymers, Biology, Chemistry, Biotechnology, Applications, Volume 4, Polyesters III: Applications and Commercial Products., Weinheim: Wiley-Blackwell, 2002.

Dowrey, A.E.

I. Noda, M.M. Satkowski, A.E. Dowrey, et al. “Polymer Alloys of Nodax Copolymers and Poly(Lactic Acid)”. Macromol. Biosci. 2004. 4(3): 269–275.

Dybal, J.

H. Sato, Y. Ando, J. Dybal, et al. “Crystal Structures, Thermal Behaviors, and C–H···O=C Hydrogen Bondings of Poly(3-hydroxyvalerate) and Poly(3-hydroxybutyrate) Studied by Infrared Spectroscopy and X-ray Diffraction”. Macromolecules. 2008. 41(12): 4305–4312.

Ewing, A.V.

A.V. Ewing, S.G. Kazarian. “Infrared Spectroscopy and Spectroscopic Imaging in Forensic Science”. Analyst. 2017. 142(2): 257–272.

Fale, F.

K.L.A. Chan, A. Altharawi, F. Fale, et al. “Transmission Fourier Transform Infrared Spectroscopic Imaging, Mapping, and Synchrotron Scanning Microscopy with Zinc Sulfide Hemispheres on Living Mammalian Cells at Sub-Cellular Resolution”. Appl. Spectrosc. 2020. 74(5): 544–552.

Flynn, A.

M.A. Abdelwahab, A. Flynn, B.-S. Chiou, et al. “Thermal, Mechanical and Morphological Characterization of Plasticized PLA–PHB Blends”. Polym. Degrad. Stab. 2012. 97(9): 1822–1828.

Furukawa, T.

J. Zhang, H. Sato, T. Furukawa, et al. “Crystallization Behaviors of Poly(3-hydroxybutyrate) and Poly(L-Lactic Acid) in Their Immiscible and Miscible Blends”. J. Phys. Chem. B. 2006. 110(48): 24463–24471.

T. Furukawa, H. Sato, R. Murakami, et al. “Structure, Dispersibility, and Crystallinity of Poly(Hydroxybutyrate)/Poly(L-Lactic Acid) Blends Studied by FT-IR Microspectroscopy and Differential Scanning Calorimetry”. Macromolecules. 2005. 38(15): 6445–6454.

García, A.

C. Peña, T. Castillo, A. García, et al. “Biotechnological Strategies to Improve Production of Microbial Poly-(3-hydroxybutyrate): A Review of Recent Research Work”. Microb. Biotechnol. 2014. 7(4): 278–293.

Guo, L.

L. Guo, H. Sato, T. Hashimoto, et al. “Thermally Induced Exchanges of Hydrogen Bonding Interactions and Their Effects on Phase Structures of Poly(3-hydroxybutyrate) and Poly(4-Vinylphenol) Blends”. Macromolecules. 2011. 44(7): 2229–2239.

L. Guo, H. Sato, T. Hashimoto, et al. “FTIR Study on Hydrogen-Bonding Interactions in Biodegradable Polymer Blends of Poly(3-hydroxybutyrate) and Poly(4-Vinylphenol)”. Macromolecules. 2010. 43(8): 3897–3902.

Guo, Q.

Q. Guo. “Polymer Morphology: Principles, Characterization, and Processing”., Hoboken, NJ: John Wiley and Sons, 2016.

Hashimoto, T.

L. Guo, H. Sato, T. Hashimoto, et al. “Thermally Induced Exchanges of Hydrogen Bonding Interactions and Their Effects on Phase Structures of Poly(3-hydroxybutyrate) and Poly(4-Vinylphenol) Blends”. Macromolecules. 2011. 44(7): 2229–2239.

L. Guo, H. Sato, T. Hashimoto, et al. “FTIR Study on Hydrogen-Bonding Interactions in Biodegradable Polymer Blends of Poly(3-hydroxybutyrate) and Poly(4-Vinylphenol)”. Macromolecules. 2010. 43(8): 3897–3902.

Hikima, Y.

Y. Hikima, J. Morikawa, S.G. Kazarian. “Analysis of Molecular Orientation in Polymeric Spherulite Using Polarized Micro Attenuated Total Reflection Fourier Transform Infrared (ATR-FTIR) Spectroscopic Imaging”. Anal. Chim. Acta. 2019. 1065: 79–89.

Kanamori, T.

H. Urayama, T. Kanamori, Y. Kimura. “Properties and Biodegradability of Polymer Blends of Poly(L–lactide)S with Different Optical Purity of the Lactate Units”. Macromol. Mater. Eng. 2002. 287(2): 116–121.

Kazarian, S.G.

H. Lu, H. Shinzawa, S.G. Kazarian. “Intermolecular Interactions in the Polymer Blends Under High-Pressure CO2 Studied Using Two-Dimensional Correlation Analysis and Two-Dimensional Disrelation Mapping”. Appl. Spectrosc. 2021. 75(3): 250–258.

H. Lu, S.G. Kazarian, H. Sato. “Simultaneous Visualization of Phase Separation and Crystallization in PHB/PLLA Blends with In Situ ATR-FTIR Spectroscopic Imaging”. Macromolecules. 2020. 53(20): 9074–9085.

C.L. Song, S.G. Kazarian. “Effect of Controlled Humidity and Tissue Hydration on Colon Cancer Diagnostic via FTIR Spectroscopic Imaging”. Anal. Chem. 2020. 92(14): 9691–9698.

H. Lu, S.G. Kazarian. “How Does High-Pressure CO2 Affect the Morphology of PCL/PLA Blends? Visualization of Phase Separation Using In Situ ATR-FTIR Spectroscopic Imaging”. Spectrochim. Acta, Part. A. 2020. 243: 118760.

Y. Hikima, J. Morikawa, S.G. Kazarian. “Analysis of Molecular Orientation in Polymeric Spherulite Using Polarized Micro Attenuated Total Reflection Fourier Transform Infrared (ATR-FTIR) Spectroscopic Imaging”. Anal. Chim. Acta. 2019. 1065: 79–89.

A.V. Ewing, S.G. Kazarian. “Infrared Spectroscopy and Spectroscopic Imaging in Forensic Science”. Analyst. 2017. 142(2): 257–272.

K.L.A. Chan, S.G. Kazarian, D. Vassou, et al. “In Situ High-Throughput Study of Drug Polymorphism Under Controlled Temperature and Humidity Using FT-IR Spectroscopic Imaging”. Vib. Spectrosc. 2007. 43(1): 221–226.

Kimura, Y.

H. Urayama, T. Kanamori, Y. Kimura. “Properties and Biodegradability of Polymer Blends of Poly(L–lactide)S with Different Optical Purity of the Lactate Units”. Macromol. Mater. Eng. 2002. 287(2): 116–121.

Koyama, N.

N. Koyama, Y. Doi. “Miscibility of Binary Blends of Poly(R)-3-hydroxybutyric Acid, and Poly(S)-Lactic Acid]”. Polymer. 1997. 38(7): 1589–1593.

Lasch, P.

P. Lasch, I. Noda. “Two-Dimensional Correlation Spectroscopy (2D-COS) for Analysis of Spatially Resolved Vibrational Spectra”. Appl. Spectrosc. 2019. 73(4): 359–379.

Lim, L.-T.

R. Auras, L.-T. Lim, S.E.M. Selke, et al. Poly(Lactic Acid): Synthesis, Structures, Properties, Processing, and Applications., Hoboken, NJ: Wiley, 2010.

Lu, H.

H. Lu, H. Shinzawa, S.G. Kazarian. “Intermolecular Interactions in the Polymer Blends Under High-Pressure CO2 Studied Using Two-Dimensional Correlation Analysis and Two-Dimensional Disrelation Mapping”. Appl. Spectrosc. 2021. 75(3): 250–258.

H. Lu, S.G. Kazarian. “How Does High-Pressure CO2 Affect the Morphology of PCL/PLA Blends? Visualization of Phase Separation Using In Situ ATR-FTIR Spectroscopic Imaging”. Spectrochim. Acta, Part. A. 2020. 243: 118760.

H. Lu, S.G. Kazarian, H. Sato. “Simultaneous Visualization of Phase Separation and Crystallization in PHB/PLLA Blends with In Situ ATR-FTIR Spectroscopic Imaging”. Macromolecules. 2020. 53(20): 9074–9085.

Mori, K.

H. Sato, K. Mori, R. Murakami, et al. “Crystal and Lamella Structure and C–H···O=C Hydrogen Bonding of Poly(3-hydroxyalkanoate) Studied by X-ray Diffraction and Infrared Spectroscopy”. Macromolecules. 2006. 39(4): 1525–1531.

Morikawa, J.

Y. Hikima, J. Morikawa, S.G. Kazarian. “Analysis of Molecular Orientation in Polymeric Spherulite Using Polarized Micro Attenuated Total Reflection Fourier Transform Infrared (ATR-FTIR) Spectroscopic Imaging”. Anal. Chim. Acta. 2019. 1065: 79–89.

Murakami, R.

H. Sato, K. Mori, R. Murakami, et al. “Crystal and Lamella Structure and C–H···O=C Hydrogen Bonding of Poly(3-hydroxyalkanoate) Studied by X-ray Diffraction and Infrared Spectroscopy”. Macromolecules. 2006. 39(4): 1525–1531.

T. Furukawa, H. Sato, R. Murakami, et al. “Structure, Dispersibility, and Crystallinity of Poly(Hydroxybutyrate)/Poly(L-Lactic Acid) Blends Studied by FT-IR Microspectroscopy and Differential Scanning Calorimetry”. Macromolecules. 2005. 38(15): 6445–6454.

H. Sato, R. Murakami, A. Padermshoke, et al. “Infrared Spectroscopy Studies of CH···O Hydrogen Bondings and Thermal Behavior of Biodegradable Poly(hydroxyalkanoate)”. Macromolecules. 2004. 37(19): 7203–7213.

Nakamura, M.

H. Sato, M. Nakamura, A. Padermshoke, et al. “Thermal Behavior and Molecular Interaction of Poly(3-hydroxybutyrate-Co-3-Hydroxyhexanoate) Studied by Wide-Angle X-ray Diffraction”. Macromolecules. 2004. 37(10): 3763–3769.

Noda, I.

P. Lasch, I. Noda. “Two-Dimensional Correlation Spectroscopy (2D-COS) for Analysis of Spatially Resolved Vibrational Spectra”. Appl. Spectrosc. 2019. 73(4): 359–379.

I. Noda, M.M. Satkowski, A.E. Dowrey, et al. “Polymer Alloys of Nodax Copolymers and Poly(Lactic Acid)”. Macromol. Biosci. 2004. 4(3): 269–275.

Ohkoshi, I.

I. Ohkoshi, H. Abe, Y. Doi. “Miscibility and Solid-State Structures for Blends of Poly(S)-Lactide with Atactic Poly(R,S)-3-hydroxybutyrate]”. Polymer. 2000. 41(15): 5985–5992.

Owen, A.J.

E. Blümm, A.J. Owen. “Miscibility, Crystallization and Melting of Poly(3-hydroxybutyrate)/Poly(L-Lactide) Blends”. Polymer. 1995. 36(21): 4077–4081.

Ozaki, Y.

H. Shinzawa, K. Awa, Y. Ozaki. “Compression-Induced Morphological and Molecular Structural Changes in Cellulose Tablets Probed by Near-Infrared Imaging”. J. Near Infrared Spectrosc. 2011. 19(1): 15–22.

H. Shinzawa, K. Awa, Y. Ozaki, et al. “Near-Infrared Imaging Analysis of Cellulose Tablet by a Band Position Shift”. Appl. Spectrosc. 2009. 63(8): 974–977.

Padermshoke, A.

H. Sato, M. Nakamura, A. Padermshoke, et al. “Thermal Behavior and Molecular Interaction of Poly(3-hydroxybutyrate-Co-3-Hydroxyhexanoate) Studied by Wide-Angle X-ray Diffraction”. Macromolecules. 2004. 37(10): 3763–3769.

H. Sato, R. Murakami, A. Padermshoke, et al. “Infrared Spectroscopy Studies of CH···O Hydrogen Bondings and Thermal Behavior of Biodegradable Poly(hydroxyalkanoate)”. Macromolecules. 2004. 37(19): 7203–7213.

Peña, C.

C. Peña, T. Castillo, A. García, et al. “Biotechnological Strategies to Improve Production of Microbial Poly-(3-hydroxybutyrate): A Review of Recent Research Work”. Microb. Biotechnol. 2014. 7(4): 278–293.

Satkowski, M.M.

I. Noda, M.M. Satkowski, A.E. Dowrey, et al. “Polymer Alloys of Nodax Copolymers and Poly(Lactic Acid)”. Macromol. Biosci. 2004. 4(3): 269–275.

Sato, H.

H. Lu, S.G. Kazarian, H. Sato. “Simultaneous Visualization of Phase Separation and Crystallization in PHB/PLLA Blends with In Situ ATR-FTIR Spectroscopic Imaging”. Macromolecules. 2020. 53(20): 9074–9085.

N. Suttiwijitpukdee, H. Sato, J. Zhang, et al. “Effects of Intermolecular Hydrogen Bondings on Isothermal Crystallization Behavior of Polymer Blends of Cellulose Acetate Butyrate and Poly(3-hydroxybutyrate)”. Macromolecules. 2011. 44(9): 3467–3477.

L. Guo, H. Sato, T. Hashimoto, et al. “Thermally Induced Exchanges of Hydrogen Bonding Interactions and Their Effects on Phase Structures of Poly(3-hydroxybutyrate) and Poly(4-Vinylphenol) Blends”. Macromolecules. 2011. 44(7): 2229–2239.

L. Guo, H. Sato, T. Hashimoto, et al. “FTIR Study on Hydrogen-Bonding Interactions in Biodegradable Polymer Blends of Poly(3-hydroxybutyrate) and Poly(4-Vinylphenol)”. Macromolecules. 2010. 43(8): 3897–3902.

H. Sato, Y. Ando, J. Dybal, et al. “Crystal Structures, Thermal Behaviors, and C–H···O=C Hydrogen Bondings of Poly(3-hydroxyvalerate) and Poly(3-hydroxybutyrate) Studied by Infrared Spectroscopy and X-ray Diffraction”. Macromolecules. 2008. 41(12): 4305–4312.

H. Sato, K. Mori, R. Murakami, et al. “Crystal and Lamella Structure and C–H···O=C Hydrogen Bonding of Poly(3-hydroxyalkanoate) Studied by X-ray Diffraction and Infrared Spectroscopy”. Macromolecules. 2006. 39(4): 1525–1531.

J. Zhang, H. Sato, T. Furukawa, et al. “Crystallization Behaviors of Poly(3-hydroxybutyrate) and Poly(L-Lactic Acid) in Their Immiscible and Miscible Blends”. J. Phys. Chem. B. 2006. 110(48): 24463–24471.

T. Furukawa, H. Sato, R. Murakami, et al. “Structure, Dispersibility, and Crystallinity of Poly(Hydroxybutyrate)/Poly(L-Lactic Acid) Blends Studied by FT-IR Microspectroscopy and Differential Scanning Calorimetry”. Macromolecules. 2005. 38(15): 6445–6454.

H. Sato, R. Murakami, A. Padermshoke, et al. “Infrared Spectroscopy Studies of CH···O Hydrogen Bondings and Thermal Behavior of Biodegradable Poly(hydroxyalkanoate)”. Macromolecules. 2004. 37(19): 7203–7213.

H. Sato, M. Nakamura, A. Padermshoke, et al. “Thermal Behavior and Molecular Interaction of Poly(3-hydroxybutyrate-Co-3-Hydroxyhexanoate) Studied by Wide-Angle X-ray Diffraction”. Macromolecules. 2004. 37(10): 3763–3769.

Selke, S.E.M.

R. Auras, L.-T. Lim, S.E.M. Selke, et al. Poly(Lactic Acid): Synthesis, Structures, Properties, Processing, and Applications., Hoboken, NJ: Wiley, 2010.

Shinzawa, H.

H. Lu, H. Shinzawa, S.G. Kazarian. “Intermolecular Interactions in the Polymer Blends Under High-Pressure CO2 Studied Using Two-Dimensional Correlation Analysis and Two-Dimensional Disrelation Mapping”. Appl. Spectrosc. 2021. 75(3): 250–258.

H. Shinzawa, K. Awa, Y. Ozaki. “Compression-Induced Morphological and Molecular Structural Changes in Cellulose Tablets Probed by Near-Infrared Imaging”. J. Near Infrared Spectrosc. 2011. 19(1): 15–22.

H. Shinzawa, K. Awa, Y. Ozaki, et al. “Near-Infrared Imaging Analysis of Cellulose Tablet by a Band Position Shift”. Appl. Spectrosc. 2009. 63(8): 974–977.

Siesler, H.W.

C. Vogel, E. Wessel, H.W. Siesler. “FT-IR Imaging Spectroscopy of Phase Separation in Blends of Poly(3-hydroxybutyrate) with Poly(L-lactic Acid) and Poly(ɛ-caprolactone)”. Biomacromolecules. 2008. 9(2): 523–527.

Song, C.L.

C.L. Song, S.G. Kazarian. “Effect of Controlled Humidity and Tissue Hydration on Colon Cancer Diagnostic via FTIR Spectroscopic Imaging”. Anal. Chem. 2020. 92(14): 9691–9698.

Suttiwijitpukdee, N.

N. Suttiwijitpukdee, H. Sato, J. Zhang, et al. “Effects of Intermolecular Hydrogen Bondings on Isothermal Crystallization Behavior of Polymer Blends of Cellulose Acetate Butyrate and Poly(3-hydroxybutyrate)”. Macromolecules. 2011. 44(9): 3467–3477.

Tsuji, H.

H. Tsuji. “Poly(Lactic Acid) Stereocomplexes: A Decade of Progress”. Adv. Drug Deliv. Rev. 2016. 107(15): 97–135.

Urayama, H.

H. Urayama, T. Kanamori, Y. Kimura. “Properties and Biodegradability of Polymer Blends of Poly(L–lactide)S with Different Optical Purity of the Lactate Units”. Macromol. Mater. Eng. 2002. 287(2): 116–121.

Vassou, D.

K.L.A. Chan, S.G. Kazarian, D. Vassou, et al. “In Situ High-Throughput Study of Drug Polymorphism Under Controlled Temperature and Humidity Using FT-IR Spectroscopic Imaging”. Vib. Spectrosc. 2007. 43(1): 221–226.

Vert, M.

M. Vert. “Aliphatic Polyesters: Great Degradable Polymers That Cannot Do Everything”. Biomacromolecules. 2005. 6(2): 538–546.

Vogel, C.

C. Vogel, E. Wessel, H.W. Siesler. “FT-IR Imaging Spectroscopy of Phase Separation in Blends of Poly(3-hydroxybutyrate) with Poly(L-lactic Acid) and Poly(ɛ-caprolactone)”. Biomacromolecules. 2008. 9(2): 523–527.

Wessel, E.

C. Vogel, E. Wessel, H.W. Siesler. “FT-IR Imaging Spectroscopy of Phase Separation in Blends of Poly(3-hydroxybutyrate) with Poly(L-lactic Acid) and Poly(ɛ-caprolactone)”. Biomacromolecules. 2008. 9(2): 523–527.

Zhang, J.

N. Suttiwijitpukdee, H. Sato, J. Zhang, et al. “Effects of Intermolecular Hydrogen Bondings on Isothermal Crystallization Behavior of Polymer Blends of Cellulose Acetate Butyrate and Poly(3-hydroxybutyrate)”. Macromolecules. 2011. 44(9): 3467–3477.

J. Zhang, H. Sato, T. Furukawa, et al. “Crystallization Behaviors of Poly(3-hydroxybutyrate) and Poly(L-Lactic Acid) in Their Immiscible and Miscible Blends”. J. Phys. Chem. B. 2006. 110(48): 24463–24471.

Adv. Drug Deliv. Rev (1)

H. Tsuji. “Poly(Lactic Acid) Stereocomplexes: A Decade of Progress”. Adv. Drug Deliv. Rev. 2016. 107(15): 97–135.

Anal. Chem (1)

C.L. Song, S.G. Kazarian. “Effect of Controlled Humidity and Tissue Hydration on Colon Cancer Diagnostic via FTIR Spectroscopic Imaging”. Anal. Chem. 2020. 92(14): 9691–9698.

Anal. Chim. Acta (1)

Y. Hikima, J. Morikawa, S.G. Kazarian. “Analysis of Molecular Orientation in Polymeric Spherulite Using Polarized Micro Attenuated Total Reflection Fourier Transform Infrared (ATR-FTIR) Spectroscopic Imaging”. Anal. Chim. Acta. 2019. 1065: 79–89.

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A.V. Ewing, S.G. Kazarian. “Infrared Spectroscopy and Spectroscopic Imaging in Forensic Science”. Analyst. 2017. 142(2): 257–272.

Appl. Spectrosc (4)

H. Lu, H. Shinzawa, S.G. Kazarian. “Intermolecular Interactions in the Polymer Blends Under High-Pressure CO2 Studied Using Two-Dimensional Correlation Analysis and Two-Dimensional Disrelation Mapping”. Appl. Spectrosc. 2021. 75(3): 250–258.

H. Shinzawa, K. Awa, Y. Ozaki, et al. “Near-Infrared Imaging Analysis of Cellulose Tablet by a Band Position Shift”. Appl. Spectrosc. 2009. 63(8): 974–977.

K.L.A. Chan, A. Altharawi, F. Fale, et al. “Transmission Fourier Transform Infrared Spectroscopic Imaging, Mapping, and Synchrotron Scanning Microscopy with Zinc Sulfide Hemispheres on Living Mammalian Cells at Sub-Cellular Resolution”. Appl. Spectrosc. 2020. 74(5): 544–552.

P. Lasch, I. Noda. “Two-Dimensional Correlation Spectroscopy (2D-COS) for Analysis of Spatially Resolved Vibrational Spectra”. Appl. Spectrosc. 2019. 73(4): 359–379.

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C. Vogel, E. Wessel, H.W. Siesler. “FT-IR Imaging Spectroscopy of Phase Separation in Blends of Poly(3-hydroxybutyrate) with Poly(L-lactic Acid) and Poly(ɛ-caprolactone)”. Biomacromolecules. 2008. 9(2): 523–527.

M. Vert. “Aliphatic Polyesters: Great Degradable Polymers That Cannot Do Everything”. Biomacromolecules. 2005. 6(2): 538–546.

J. Near Infrared Spectrosc (1)

H. Shinzawa, K. Awa, Y. Ozaki. “Compression-Induced Morphological and Molecular Structural Changes in Cellulose Tablets Probed by Near-Infrared Imaging”. J. Near Infrared Spectrosc. 2011. 19(1): 15–22.

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J. Zhang, H. Sato, T. Furukawa, et al. “Crystallization Behaviors of Poly(3-hydroxybutyrate) and Poly(L-Lactic Acid) in Their Immiscible and Miscible Blends”. J. Phys. Chem. B. 2006. 110(48): 24463–24471.

Macromol. Biosci (1)

I. Noda, M.M. Satkowski, A.E. Dowrey, et al. “Polymer Alloys of Nodax Copolymers and Poly(Lactic Acid)”. Macromol. Biosci. 2004. 4(3): 269–275.

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H. Urayama, T. Kanamori, Y. Kimura. “Properties and Biodegradability of Polymer Blends of Poly(L–lactide)S with Different Optical Purity of the Lactate Units”. Macromol. Mater. Eng. 2002. 287(2): 116–121.

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H. Sato, M. Nakamura, A. Padermshoke, et al. “Thermal Behavior and Molecular Interaction of Poly(3-hydroxybutyrate-Co-3-Hydroxyhexanoate) Studied by Wide-Angle X-ray Diffraction”. Macromolecules. 2004. 37(10): 3763–3769.

H. Sato, R. Murakami, A. Padermshoke, et al. “Infrared Spectroscopy Studies of CH···O Hydrogen Bondings and Thermal Behavior of Biodegradable Poly(hydroxyalkanoate)”. Macromolecules. 2004. 37(19): 7203–7213.

H. Sato, K. Mori, R. Murakami, et al. “Crystal and Lamella Structure and C–H···O=C Hydrogen Bonding of Poly(3-hydroxyalkanoate) Studied by X-ray Diffraction and Infrared Spectroscopy”. Macromolecules. 2006. 39(4): 1525–1531.

H. Sato, Y. Ando, J. Dybal, et al. “Crystal Structures, Thermal Behaviors, and C–H···O=C Hydrogen Bondings of Poly(3-hydroxyvalerate) and Poly(3-hydroxybutyrate) Studied by Infrared Spectroscopy and X-ray Diffraction”. Macromolecules. 2008. 41(12): 4305–4312.

L. Guo, H. Sato, T. Hashimoto, et al. “FTIR Study on Hydrogen-Bonding Interactions in Biodegradable Polymer Blends of Poly(3-hydroxybutyrate) and Poly(4-Vinylphenol)”. Macromolecules. 2010. 43(8): 3897–3902.

L. Guo, H. Sato, T. Hashimoto, et al. “Thermally Induced Exchanges of Hydrogen Bonding Interactions and Their Effects on Phase Structures of Poly(3-hydroxybutyrate) and Poly(4-Vinylphenol) Blends”. Macromolecules. 2011. 44(7): 2229–2239.

N. Suttiwijitpukdee, H. Sato, J. Zhang, et al. “Effects of Intermolecular Hydrogen Bondings on Isothermal Crystallization Behavior of Polymer Blends of Cellulose Acetate Butyrate and Poly(3-hydroxybutyrate)”. Macromolecules. 2011. 44(9): 3467–3477.

H. Lu, S.G. Kazarian, H. Sato. “Simultaneous Visualization of Phase Separation and Crystallization in PHB/PLLA Blends with In Situ ATR-FTIR Spectroscopic Imaging”. Macromolecules. 2020. 53(20): 9074–9085.

T. Furukawa, H. Sato, R. Murakami, et al. “Structure, Dispersibility, and Crystallinity of Poly(Hydroxybutyrate)/Poly(L-Lactic Acid) Blends Studied by FT-IR Microspectroscopy and Differential Scanning Calorimetry”. Macromolecules. 2005. 38(15): 6445–6454.

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C. Peña, T. Castillo, A. García, et al. “Biotechnological Strategies to Improve Production of Microbial Poly-(3-hydroxybutyrate): A Review of Recent Research Work”. Microb. Biotechnol. 2014. 7(4): 278–293.

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Vib. Spectrosc (1)

K.L.A. Chan, S.G. Kazarian, D. Vassou, et al. “In Situ High-Throughput Study of Drug Polymorphism Under Controlled Temperature and Humidity Using FT-IR Spectroscopic Imaging”. Vib. Spectrosc. 2007. 43(1): 221–226.

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Supplementary Material (1)

NameDescription
Supplement 1       sj-pdf-1-asp-10.1177_00037028211010216 - Supplemental material for Visualization of Inter- and Intramolecular Interactions in Poly(3-hydroxybutyrate)/Poly(-lactic acid) (PHB/PLLA) Blends During Isothermal Melt Crystallization Using Attenuated Total Reflection Fourier Transform infrared (ATR FT-IR) Spectroscopic Imaging

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