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Intermolecular Hydrogen Bonding between Poly[(R)-3-hydroxybutyrate] (PHB) and Pseudoboehmite and Its Effect on Crystallization of PHB
ACS Applied Polymer Materials ( IF 4.4 ) Pub Date : 2020-08-31 , DOI: 10.1021/acsapm.0c00758 Changhao Liu 1 , Meng Jia 2 , Jing Qu 3 , Isao Noda 1, 4 , D. Bruce Chase 1 , Reva Street 1 , John F. Rabolt 1
ACS Applied Polymer Materials ( IF 4.4 ) Pub Date : 2020-08-31 , DOI: 10.1021/acsapm.0c00758 Changhao Liu 1 , Meng Jia 2 , Jing Qu 3 , Isao Noda 1, 4 , D. Bruce Chase 1 , Reva Street 1 , John F. Rabolt 1
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In the present study, we focused on the intermolecular H-bonding interactions of poly[(R)-3-hydroxybutyrate] (PHB) with an inorganic material, pseudoboehmite (PB), and their effect on PHB crystallization. Noncrystallizable atactic PHB and crystallizable isotactic PHB (a-PHB and i-PHB) ultrathin films were spin-coated on a PB substrate, as well as an aluminum oxide (AO) and a gold substrate for comparison. Infrared reflection–absorption spectroscopy (IRRAS) data show an absorption peak in the carbonyl region located at 1724 cm–1 for a 2.8 nm a-PHB film deposited on PB. A peak at this frequency, often observed for thick bulk crystalline i-PHB films, was not observed for a 1.4 nm a-PHB film deposited on a gold or AO substrate, indicating that the 1724 cm–1 peak observed for a-PHB on PB is not due to a geometric confinement effect or crystallization but due to the existence of intermolecular H-bonding (H-bondinter) between −C═O of a-PHB and −OH from PB. Supercooled, amorphous i-PHB was also found to exhibit the same H-bondinter with PB. It was found that a PB surface significantly modified the crystal orientation and morphologies of the films. Grazing incident wide-angle X-ray diffraction (GIWAXD) data show that the crystallites in i-PHB on PB are randomly oriented, whereas those on AO are predominantly edge-on oriented. Polarized optical microscopy (POM) images show spherulites for i-PHB on AO, whereas no spherulites were observed for i-PHB on PB. This study demonstrates a novel method of using PB to modulate the crystallization behavior of PHB thin films.
中文翻译：
聚[（R）-3-羟基丁酸酯]（PHB）与假勃姆石之间的分子间氢键及其对PHB结晶的影响
在本研究中，我们重点研究了聚[（R）-3-羟基丁酸酯]（PHB）与无机材料假勃姆石（PB）的分子间H键相互作用及其对PHB结晶的影响。将不可结晶的无规PHB和可结晶的等规PHB（a-PHB和i-PHB）超薄膜旋涂在PB基板上，以及氧化铝（AO）和金基板上进行比较。红外反射吸收光谱（IRRAS）数据显示，沉积在PB上的2.8 nm a-PHB膜的羰基区域的吸收峰位于1724 cm –1处。在厚的块状i-PHB晶体中经常观察到该频率下的峰值，而在金或AO衬底上沉积的1.4 nm a-PHB膜则未观察到此峰，表明1724 cm –1关于PB A-PHB观察到的峰是不是由于几何约束效果或结晶，但是由于分子间氢键（H键的存在帧间一个-PHB的-C = O和-OH从PB之间）。过冷，非晶i PHB也被发现表现出相同的H-键间与PB。发现PB表面显着改变了膜的晶体取向和形态。掠入射的广角X射线衍射（GIWAXD）数据表明，PB上i-PHB中的微晶是随机取向的，而AO上的微晶则主要是边沿取向的。偏光显微镜（POM）图像显示AO上i-PHB的球晶，而PB上未观察到i-PHB的球晶。这项研究表明使用PB来调节PHB薄膜的结晶行为的一种新方法。
更新日期：2020-08-31
中文翻译：
聚[（R）-3-羟基丁酸酯]（PHB）与假勃姆石之间的分子间氢键及其对PHB结晶的影响
在本研究中，我们重点研究了聚[（R）-3-羟基丁酸酯]（PHB）与无机材料假勃姆石（PB）的分子间H键相互作用及其对PHB结晶的影响。将不可结晶的无规PHB和可结晶的等规PHB（a-PHB和i-PHB）超薄膜旋涂在PB基板上，以及氧化铝（AO）和金基板上进行比较。红外反射吸收光谱（IRRAS）数据显示，沉积在PB上的2.8 nm a-PHB膜的羰基区域的吸收峰位于1724 cm –1处。在厚的块状i-PHB晶体中经常观察到该频率下的峰值，而在金或AO衬底上沉积的1.4 nm a-PHB膜则未观察到此峰，表明1724 cm –1关于PB A-PHB观察到的峰是不是由于几何约束效果或结晶，但是由于分子间氢键（H键的存在帧间一个-PHB的-C = O和-OH从PB之间）。过冷，非晶i PHB也被发现表现出相同的H-键间与PB。发现PB表面显着改变了膜的晶体取向和形态。掠入射的广角X射线衍射（GIWAXD）数据表明，PB上i-PHB中的微晶是随机取向的，而AO上的微晶则主要是边沿取向的。偏光显微镜（POM）图像显示AO上i-PHB的球晶，而PB上未观察到i-PHB的球晶。这项研究表明使用PB来调节PHB薄膜的结晶行为的一种新方法。
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